TWI362934B - Phosphonate analogs of hiv inhibitor compounds - Google Patents

Phosphonate analogs of hiv inhibitor compounds Download PDF

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TWI362934B
TWI362934B TW94125503A TW94125503A TWI362934B TW I362934 B TWI362934 B TW I362934B TW 94125503 A TW94125503 A TW 94125503A TW 94125503 A TW94125503 A TW 94125503A TW I362934 B TWI362934 B TW I362934B
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TW200618804A (en
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Adrian S Ray
Lijun Zhang
Richard L Mackman
Oleg V Petrakovsky
Constantine G Boojamra
Kuei-Ying Lin
David Y Markevitch
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Gilead Sciences Inc
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    • C07F9/02—Phosphorus compounds
    • C07F9/28—Phosphorus compounds with one or more P—C bonds
    • C07F9/38—Phosphonic acids RP(=O)(OH)2; Thiophosphonic acids, i.e. RP(=X)(XH)2 (X = S, Se)
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    • C07H19/02—Compounds containing a hetero ring sharing one ring hetero atom with a saccharide radical; Nucleosides; Mononucleotides; Anhydro-derivatives thereof sharing nitrogen
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    • C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic System
    • C07F9/02—Phosphorus compounds
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    • A61K31/34—Heterocyclic compounds having oxygen as the only ring hetero atom, e.g. fungichromin having five-membered rings with one oxygen as the only ring hetero atom, e.g. isosorbide
    • A61K31/341—Heterocyclic compounds having oxygen as the only ring hetero atom, e.g. fungichromin having five-membered rings with one oxygen as the only ring hetero atom, e.g. isosorbide not condensed with another ring, e.g. ranitidine, furosemide, bufetolol, muscarine
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    • A61K31/495—Heterocyclic compounds having nitrogen as a ring hetero atom, e.g. guanethidine or rifamycins having six-membered rings with two or more nitrogen atoms as the only ring heteroatoms, e.g. piperazine or tetrazines
    • A61K31/505—Pyrimidines; Hydrogenated pyrimidines, e.g. trimethoprim
    • A61K31/513—Pyrimidines; Hydrogenated pyrimidines, e.g. trimethoprim having oxo groups directly attached to the heterocyclic ring, e.g. cytosine
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    • A61K31/683—Diesters of a phosphorus acid with two hydroxy compounds, e.g. phosphatidylinositols
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    • A61K31/70—Carbohydrates; Sugars; Derivatives thereof
    • A61K31/7042—Compounds having saccharide radicals and heterocyclic rings
    • A61K31/7052—Compounds having saccharide radicals and heterocyclic rings having nitrogen as a ring hetero atom, e.g. nucleosides, nucleotides
    • A61K31/706—Compounds having saccharide radicals and heterocyclic rings having nitrogen as a ring hetero atom, e.g. nucleosides, nucleotides containing six-membered rings with nitrogen as a ring hetero atom
    • A61K31/7064—Compounds having saccharide radicals and heterocyclic rings having nitrogen as a ring hetero atom, e.g. nucleosides, nucleotides containing six-membered rings with nitrogen as a ring hetero atom containing condensed or non-condensed pyrimidines
    • A61K31/7076—Compounds having saccharide radicals and heterocyclic rings having nitrogen as a ring hetero atom, e.g. nucleosides, nucleotides containing six-membered rings with nitrogen as a ring hetero atom containing condensed or non-condensed pyrimidines containing purines, e.g. adenosine, adenylic acid
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    • A61K45/00—Medicinal preparations containing active ingredients not provided for in groups A61K31/00 - A61K41/00
    • A61K45/06—Mixtures of active ingredients without chemical characterisation, e.g. antiphlogistics and cardiaca
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    • A61K47/00—Medicinal preparations characterised by the non-active ingredients used, e.g. carriers or inert additives; Targeting or modifying agents chemically bound to the active ingredient
    • A61K47/50—Medicinal preparations characterised by the non-active ingredients used, e.g. carriers or inert additives; Targeting or modifying agents chemically bound to the active ingredient the non-active ingredient being chemically bound to the active ingredient, e.g. polymer-drug conjugates
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    • A61P31/12—Antivirals
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    • A61P31/12—Antivirals
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    • A61P31/00—Antiinfectives, i.e. antibiotics, antiseptics, chemotherapeutics
    • A61P31/12—Antivirals
    • A61P31/14—Antivirals for RNA viruses
    • A61P31/18—Antivirals for RNA viruses for HIV
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61P—SPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
    • A61P31/00—Antiinfectives, i.e. antibiotics, antiseptics, chemotherapeutics
    • A61P31/12—Antivirals
    • A61P31/20—Antivirals for DNA viruses
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    • A61P—SPECIFIC THERAPEUTIC ACTIVITY OF CHEMICAL COMPOUNDS OR MEDICINAL PREPARATIONS
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    • C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic System
    • C07F9/02—Phosphorus compounds
    • C07F9/28—Phosphorus compounds with one or more P—C bonds
    • C07F9/38—Phosphonic acids RP(=O)(OH)2; Thiophosphonic acids, i.e. RP(=X)(XH)2 (X = S, Se)
    • C07F9/40—Esters thereof
    • C—CHEMISTRY; METALLURGY
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    • C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic System
    • C07F9/02—Phosphorus compounds
    • C07F9/28—Phosphorus compounds with one or more P—C bonds
    • C07F9/38—Phosphonic acids RP(=O)(OH)2; Thiophosphonic acids, i.e. RP(=X)(XH)2 (X = S, Se)
    • C07F9/44—Amides thereof
    • C—CHEMISTRY; METALLURGY
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    • C07F9/00—Compounds containing elements of Groups 5 or 15 of the Periodic System
    • C07F9/02—Phosphorus compounds
    • C07F9/547—Heterocyclic compounds, e.g. containing phosphorus as a ring hetero atom
    • C07F9/6561—Heterocyclic compounds, e.g. containing phosphorus as a ring hetero atom containing systems of two or more relevant hetero rings condensed among themselves or condensed with a common carbocyclic ring or ring system, with or without other non-condensed hetero rings
    • C07F9/65616—Heterocyclic compounds, e.g. containing phosphorus as a ring hetero atom containing systems of two or more relevant hetero rings condensed among themselves or condensed with a common carbocyclic ring or ring system, with or without other non-condensed hetero rings containing the ring system having three or more than three double bonds between ring members or between ring members and non-ring members, e.g. purine or analogs
    • C—CHEMISTRY; METALLURGY
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    • C07H—SUGARS; DERIVATIVES THEREOF; NUCLEOSIDES; NUCLEOTIDES; NUCLEIC ACIDS
    • C07H19/00—Compounds containing a hetero ring sharing one ring hetero atom with a saccharide radical; Nucleosides; Mononucleotides; Anhydro-derivatives thereof
    • C07H19/02—Compounds containing a hetero ring sharing one ring hetero atom with a saccharide radical; Nucleosides; Mononucleotides; Anhydro-derivatives thereof sharing nitrogen
    • C07H19/04—Heterocyclic radicals containing only nitrogen atoms as ring hetero atom
    • C07H19/16—Purine radicals
    • C07H19/20—Purine radicals with the saccharide radical esterified by phosphoric or polyphosphoric acids

Description

1362934 (1) 九、發明說明 【發明所屬之技術領域】 本發明大體關於具有抗病毒活性且尤其具有抗—HI V 性質之化合物。 【先前技術】
愛滋病（AIDS )爲全世界主要的公共衛生問題。雖 然以HIV病毒爲標的的藥物已廣泛使用且已顯示療效， 但毒性及抗性病毒株之發展使這些藥物的使用受限。可測 定HI V病毒存在、不存在或量之分析法則具有實際之用 途以供尋求抑制劑及供診斷HIV之存在。 人類免疫缺乏病毒(HI V)感染及相關之疾病爲全世界 主要的公共衛生問題。一般公認，反轉錄病毒人類免疫缺 乏病毒第1型（HIV-1)，靈長類慢病毒（lentivirus)科中的 —成員（DeClercq Έ,{\99 A)Annal s of the New York A cademy of Science, 724:438-456; Barre-Sinoussi F(1 996) Lancet, 348:31-35)，爲後天免疫缺乏症候群（愛滋病）之病原 (Tarrago et al. FASEB Journal 1 994, 8:497-503)。愛滋病 爲HIV-1重覆複製且免疫力降低的結果，最主要爲CD4 + 淋巴球數的下降。成熟的病毒具有編碼15個蛋白之單股 RNA 基因組（Frankel et al.(1998) Wnnwa/ Review <?/
Biochemistry, 67:1-25; Katz et al. ( 1 994) Annual Review 〇/ jB / o c/i e m i· i , 63:133-173)，包括三種關鍵酵素：（i)蛋 白酶（Prt)(von der Helm K ( 1 996) -5- ⑧ (2) 1362934 3 7 7:7 65 -774); (ii)反轉錄酶（RT)(Hottiger et al. ( 1 996) Biological Chemistry Hoppe - S ey l e r, 377:97-120) » 一 種反 轉錄病毒所獨有之酵素；及（iii)整合酶（Asante et al. (1999) Advances in Virus Research 52: 351-369; Wlodawer A (1999) Advances in Virus Research 52: 335-350;
Esposito et al. (1 999) A dv art c e s i n Virus Research 52: 319-333)蛋白酶負責病毒先質多聚蛋白之處理過程，整合 酶負責將雙股DN A形式之病毒基因組整合成宿主DN A而 反轉錄酶爲病毒基因組複製中之關鍵酵素。病毒複製中， 反轉錄酶充作RNA —及DNA -依賴性DNA聚合酶以將單 股RNA基因組轉換成雙股DNA。既然病毒編碼性反轉錄 酶（RT)在病毒之天然繁殖期間可促成特異性反應，故反轉 錄酶爲供治療HI V感染及相關疾病之重要醫療標的。 將源自一些感染性及非感染性HIV分離體中之完整 基因組進行序列分析後，可使病毒之構造及其於感染物種 中複製及成熟所必需之分子型式相當地清楚。HIV蛋白酶 爲供將病毒gag及gag-pol多聚肽進程至病毒體之蛋白中 所必需 L. Ratner，et al·, Nature, 313: 277-284 (1985); L. Η· Pearl 及 W. R. Taylor，Nature, 3 29: 3 5 1 ( 1 98 7)。HIV 顯現與於其它反轉錄病毒中所見者相同之gag / pol / env 組織 L. Ratner, et al.，above; S. Wain-Hobson，et al·，
Cell, 40: 9- 1 7 ( 1 9 8 5); R. Sanchez-Pescador, et al.,
Science，227: 484-492 ( 1 985);及 M. A_ Muesing, et al·， Nature，3 1 3 : 4 5 0-45 8 ( 1 98 5 )。 -6- ⑧ (5) 1362934 導致藥劑系統遞送至身體不必要且通常不期望的細胞及組 織中。此可導致不利之藥物副作用且通常限制可投服之藥 物（例如細胞毒性劑及其它抗癌症或抗病毒藥）之劑量。 比較之下’雖然口服藥物一般認爲是方便且經濟的投服方 法’但口服可導致（a )藥物通過細胞及組織障壁例如血 /腦 '上皮、細胞膜而吸收，導致不期望之系統分佈，或 者（b)藥物於胃腸道內暫時居留。因此，主要的目標係 # 發展可專一性地針對細胞及組織爲標的之藥劑。此種治療 之優點爲避免此些藥劑不適當地遞送至其它細胞及組織諸 如未感染之細胞中而產生一般之生理學效應。以細胞內爲 標的之作用可藉由可令生物學活性藥劑於細胞內側累積或 1 滯留之方法及組成物而達成。 '【發明內容】 本發明提供具有HIV活性之新穎化合物，亦即新穎 # 之人類反轉錄病毒RT抑制劑。因此，本發明化合物可抑 制反轉錄病毒RT，故可抑制病毒之複製。彼等有用以治 療受人類反轉錄病毒諸如人類免疫缺乏病毒（HI V-1或 HIV-2病毒株）或人類T-細胞白血病病毒（HTLV-1或 HTLV-II)所感染之人類病患。本發明包括新穎之膦酸酯 HIV RT抑制劑化合物及已知之經認可及實驗之蛋白酶抑 制劑之膦酸酯類似物。本發明化合物隨意地提供如下所示 之細胞累積作用。 本發明大體關於醫療化合物在細胞內側之累積及滯留 -9- ⑧ (6) 1362934 。本發明尤其關於在受HIV感染之細胞內獲得高濃度含 膦酸酯之分子。以細胞內爲標的之作用可藉由可令生物活 性藥劑於細胞內側累積或滞留之方法及組成物而達成。此 有效之對準標的法可應用至各種不同之醫療調合物及步驟 上。 本發明組成物包括具有至少一個膦酸酯基團之新穎 RT化合物。本發明包括所有已知之經認可及實驗之具有 φ 一個膦酸酯基團之蛋白酶抑制劑。 本發明之一觀點包括具有式I、II及1A 一1J之化合 物。 式1A - U之化合物，其藥學上可接受之鹽或溶劑化 ’物’
-10 - ⑧ (7)1362934
II
υ
A 爲·
-11 - 2 (8) 1362934 Y1 獨立地爲 Ο、s、N ( Rx) 、N(0) ( Rx)、 N ( ORx ) 、N(0) ( ORx )或 N(N(RX) ( Rx ))； Y2 獨立地爲一個鍵、〇、c ( Rx ) ( Rx ) 、N ( Rx ) 、N(0) ( Rx ) 、N(ORx) 、N(0) ( ORx ) 、N(N(
Rx) ( Rx ) )、-S(0)m2-S-S(0)m2-S(0)m2-;
Rx獨立地爲H、R1、R2、W3、保護基團、或如下式 • 者：
Ry 其中：
Ry獨立地爲Η、W3、R2或保護基團； R1獨立地爲Η或具1至18個碳原子之烷基； R2獨立地爲Η、R1、R3或R4，其中每一個R4獨立地 經〇至3個R3基團取代，或者兩個R2基團於碳原子處接 合以形成具3至8個原子之環且環可經0至3個R3基團 取代； R3爲R3a、R3b、R3e、R3d或R3e，惟當R3結合至雜 原子上時，則R3爲R3e或R3d ; R3a 爲 F、Cl、Br、I、- C N、N 3、-Ν Ο 2 -、- O R!或- 〇R6a ； -12- ⑧ (11) 1362934 列4 )至1 Ο )之嘌呤。以意指下列10 )者最佳η 1 ) Β爲雜環型胺鹼。 專利說明書中，"雜環型胺鹼〃定義爲包含一或多個 氮之單環型、二環型或多環型環系統。例如，Β包括在核 酸、核-酸及核-中所發現之天然存在之雜環，及其類似 物。
2) Β擇自
其中： • U'G及J各自獨立地爲cH或Ν; D 爲 N、CH、C-CN' C-N02、C-Cu 烷基' C-NHC〇NH2、C-C〇NTllT丨 2、c_CSNTiiTm、c_c〇〇T"、 C-C( = NH)NH2、c-淫基 ' c_Ci_3 院氧基、胺基、c_Ci-4 烷胺基、C—二（c,.4烷基）胺基 唑-2-基）' C— (1，3 C —鹵素、C— (1，3 —噁 噻唑—2—基）或C 一（咪唑—2—基 );其中烷基乃未經取件十4_ ^___ _ , Μ代或經一至二個獨立地擇自鹵素.、 烷氧基之基團所取代； 胺基、羥基、羧基及C Ε爲Ν或CT5 ; W爲0或S ; -15- (12) 1362934 1Ί爲H、C,.6烷基、C2.6烯基、C2-6炔基、（：卜4烷胺 基、CF3或鹵素； T2 爲 H、OH、SH、NH2、C,.4 烷胺基、二（Ci.4 烷基 )胺基、C3-6環烷胺基、鹵基、C,.4烷基、C,.4烷氧基或 CF3 ; τ3爲Η、胺基、Ci.4烷胺基、C3-6環烷胺基或二（ C 1 - 4院基）胺基；
T4爲Η、鹵基、CN、羧基、Ch4烷氧羰基、Ν3、胺 基' Cm烷胺基、二（Cm烷基）胺基、羥基、Cm烷氧 基、Ci-6烷硫基、Cu烷磺醯或（<^-4烷基）〇_2胺甲基； τ5獨立地爲Η或C^.6烷基且 T6爲Η、CF3、Ch烷基、胺基、Cb4烷胺基、C3.6 環烷胺基或二（C! -4烷基）胺基； 3 ) B擇自
其中： T10 爲 Η、OH、F、Cl、Br、I、0T17 ' SH、ST17、 -16- (13) 1362934 Ν Η 2 或 Ν Η T , 8 ; Τη 爲 Ν、CF、CC1、CBr、Cl、CT19、CST19 或 C 0 T ] 9 » τ12 爲 Ν 或 CH ; ΤΙ3 爲 Ν、CH、CCN、CCF3、CCeeCH 或 CC(O) NH2 ;
T14 爲 H、OH' NH2、SH ' SCH3 ' SCH2CH3 ' SCH2C ξ CH、SCH2CH = CH2、SC3H7 ' NH ( CH3) 、N ( CH3) 2 、NH ( CH2CH3) ' N ( CH2CH3 ) 2 ' NH ( CH2C ξ CH )、 NH ( CH2CH = CH2 ) ' NH ( C3H7 )或鹵素（F、Cl、Br 或 I ); T15 爲 H ' OH、F、Cl、Br、I、SCH3、SCH2CH3、 SCH2CeCH、SCH2CH = CH2、SC3H7、OT17' NH2 或 NHT18 :且 ΤΊ 6 爲 O、S 或 Se ; T17 爲 Cu 烷基（包括 CH3、CH2CH3、CH2CeCH、 ch2ch = ch2、及 c3h7 );
Ti8 爲 Ci.6 烷基（包括 CH3、CH2CH3、CH2CeCH、 ch2ch=ch2' 及 c3h7); T,9爲H、Cm烷基、c2 9烯基、c2 9炔基或c7-9芳 基—烷基’未經取代或經〇只、〇、>^、尸、（：1、：81'、或1 取代（包括 CH3' CH2CH3、CH = CH2、CH = CHBr、 CH2CH2C1 ' CH2CH2F ' CH2C= CH ' CH2CH = CH2 ' C3H7 ' CH2〇H ' CH2OCH3 ' CH2OC2H5 ' CH2〇Cs CH ' -17- (14) 1362934 CH2OCH2CH = CH2 ' CH2C3H7、CH2CH2OH、CH2CH2OCH3 ' CH2CH2〇C2H5 ' CH2CH2OC=CH' CH2CH2〇CH2CH = CH2 、ch2ch2oc3h7 ; 4) B爲腺嘌呤、鳥嘌呤、胞嘧啶、尿嘧啶、胸腺嘧 啶、7 —去氮腺嘌呤、7—去氮鳥嘌呤、7_去氮—8_氮雜 鳥嘌呤、7—去氮一 8—氮雜腺嘌呤、肌苷、雲翳菌素、硝 基吡咯、硝基吲哚、2 —胺基嘌呤' 2 _胺基—6 _氯基嘌 # 呤、2,6 —二胺基嘌呤、次黃嘌呤、假尿核苷、假胞嘧啶 、假異胞喃陡、5 -丙炔基胞嚼淀、異胞嚼陡、異鳥嘌玲 、7_去氣鳥嘌玲、硫基嚼陡、6_硫基鳥曝哈、6_硫 基胸腺喃B疋、4 一硫基尿嚼陡、—甲基鳥嘿u令、甲 基腺曝哈、V —甲基胸腺嘴d定、5,6 —二氫胸腺喃υ定、5,6 - -二氫尿嘧啶、4 一甲基吲哚或吡唑並[3，4-d]喷D定； 5 ) B爲 次黃嘌呤、
胸腺嘧啶、 尿哺陡、 黃嘌呤、 2—胺基嘌呤、2,6 —二胺基嘌呤、2 —胺基一 6 一氯基 嘌呤、次黃嘌呤 '肌苷、或黃嘌呤之8 -氮雜衍生物； 腺嘌呤、鳥嘌呤、2—胺基嘌呤、2，6~二胺基嗓玲、 2—胺基—6 —氯基嘌呤 '次黃嘌呤、肌苷、或黃嘌呤之7 —去氮一 8 —氮雜衍生物； ⑧ -18- (23) 1362934 -乙基（-CH2CH2-) ，1,3-丙基（-CH2CH2CH2-) ，1,4 —丁基（-CH2CH2CH2CH2-)等。 ^烯撐"意指具2— 18個碳原子之不飽和、支或直鏈 或環型烴基團，且其具有兩個藉由母烯之相同或兩個不同 之碳原子中移除兩個氫原子後所衍出之兩個單價基團中心 。典型之烯撐基團包括，但不限定於，1,2-乙撐 (-CH = CH-)。 φ *炔撐〃意指具2 - 18個碳原子之不飽和、支或直鏈 或環型烴基團，且其具有兩個藉由母炔之相同或兩個不同 .之碳原子中移除兩個氫原子後所衍出之兩個單價基團中心 。典型之炔撐基團包括，但不限定於’乙炔（-c三c-) ’ “ 炔丙基（-CH2CeC-)，及 4 -戊炔基（-CH2CH2CH2Cs 、 CH-)。 "芳基"意指藉由母芳族環系統之單一碳原子中移除 一個氫原子後所衍出之具有6 - 20個碳原子之單價芳族烴 ® 基團。典型之芳基團包括，但不限定於，由苯、經取代苯 、萘、蒽、聯苯中所衍出之基團。 "芳烷基〃意指非芳型烷基團’其中一個鍵結至碳原 子（通常終端或sp3碳原子）上之氫原子乃被芳基團所替 代。典型之芳烷基團包括，但不限定於，苄基、2 —苯基 乙一1_基、萘甲基、2 —萘基乙一1—基、萘並苄基’ 萘並苯基乙一 1_基等。芳烷基團包含6至20個碳原子’ 例如芳烷基團中之烷基部分包括烷基、烯基或炔基爲1至 6個碳原子且芳基部分爲5至14個碳原子。 ⑧ (24) 1362934 ^經取代烷基〃，〜經取代芳基〃及"經取代芳烷基 〃分別意指烷基，芳基及芳烷基，其中有一或多個氫原子 各自獨立地經非氫之取代基所替代。典型之取代基包括， 但不限定於，—X，- R，— 〇·，— OR，_SR，- S·，
-NR2-，- NR3 ' = NR , - CX3，- CN，- OCN，— SCN ，一N=C=p，- NCS，- NO，一N〇2，= N2，一N3， NC(=0) R. _c(=0) R> - C(=0) NRR-S (=〇) 2cr，s(=o) 2〇H，- S(=〇) 2R，- OS (=〇) 2〇R，一S(=0) 2NR，- S(=0) R，- 〇p (=〇) 02RR，- P ( = 0 ) 02RR - P ( = 0 ) (0·) 2，— p C = 〇 ) (OH) 2，一 C(=0) R，- C(=0) X， C ( S ) R » - C(0) OR，- C(O) Ο、- C(S) OR，-C(〇) SR，- C(S) SR，- C(0) NRR，- C(S) NRR ’ 一C(NR) NRR，其中每一個X獨立地爲鹵素；F、Cl 、：Br或I;且每一個R獨立地爲—Η、烷基、芳基、雜環 '保護基團或前藥部分。烷撐、烯撐及炔撐基團亦可同樣 地經取代。 本文中所用之"雜環〃包括述於Paquette, Leo Α.; Principle of Modern Heterocyclic Chemistry (W. A. Benjamin, New York, 1 968)，尤其第 1、3、4、6、7 及 9 章；The Chemistry of Heterocyclic Compounds，A Series of Monographs" ( j 〇 h n W i 1 e y & S 〇 n s，N e w Y o r k，1 9 5 0 至 今）’尤其第 13、14、16、19 及 28 章；及 >/· J/n. C/jew. kc· (1960) 82:5566中之實例及非限定之雜環。本發明之 -28- (25) 1362934 一特別實施例中，"雜環〃包括本文中所定義之'' 碳環〃 ，其中一或多個（例如1、2、3或4個）碳原子業已經雜 原子（例如〇、N或S )所替代。 雜環之實例包括（但不限定於）吡啶基、二氫吡啶基 、四氫吡啶基（哌啶基）、噻唑基、四氫噻吩基、硫經氧 化之四氫噻吩基、嘧啶基、呋喃基、噻吩基、吡咯基、吡 唑基、咪唑基、四唑基、苯並呋喃基、硫茚基、吲哚基、 φ 吲哚滿基、喹啉基、異喹啉基、苯並咪唑基、哌啶基、4 一哌啶嗣基、吡咯啶基、2—吡咯酮基、吡咯啉基、四氫 呋喃基、四氫喹啉基、四氫異喹啉基、八氫喹啉基、八氫 異喹啉基、佐辛基、三嗪基、6H — 1,2,5 —噻二嗪基、 _ 2H,6H_ 1，5,2-二噻嗦基、噻吩基、噻蒽基、Dtfc喃基、異 - 苯並呋喃基、色烯基、咕噸基、吩噻噁基、2H_吡咯基 、異噻唑基、異噁唑基、吡嗪基、噠嗪基、吲哚嗪基、異 吲哚基、3 Η _吲哚基、1 Η _吲嗖基、嘌呤基、4 Η — D奎嗪 Φ 基、酞嗪基、萘啶基、喹噁啉基、喹唑啉基、噌啉基、蝶 啶基、4aH_咔唑基、咔唑基、召—咔啉基、菲啶基、吖 啶基、嘧啶基、菲繞啉基、吩嗪基、吩噻嗪基、呋喃基、 吩噁嗪基、異色滿基、色滿基、咪唑啶基、咪唑啉基、吡 唑啶基、吡唑啉基、哌嗪基、吲哚啉基、異吲哚啉基、奎 寧環基、嗎啉基、噁唑啶基、苯並三唑基、苯並異噁唑基 、羥吲哚基、苯並噁唑啉基、靛紅基及雙-四氫呋喃基： (26) 1362934 舉例（但不限定）而言，碳鍵結性雜環乃在吡啶之2 、3、4、5或6位置，噠嗪之3、4、5或6位置，嘧啶之 2、4、5或6位置，吼嗪之2、3、5或6位置，呋喃、四 氫呋喃、噻呋喃、噻吩、吡咯或四氫吡咯之2、3、4或5 位置，噁唑、咪唑或噻唑之2'4或5位置，異噁唑、吡 唑或異噻唑之3、4或5位置，氮丙啶之2或3位置，雜 氮環丁烷之2' 3或4位置，哇啉之2、3、4、5、6、7或 ^ 8位置或異D奎啉之1'3、4、5、6、7或8位置鍵結。更 典型之碳鍵結性雜環包括2 -吡啶基、3_吡啶基、4一 D比 D定基' 5 _吼D定基、6 -吼D定基、3 —噠嗪基、4 _噠Π秦基、 5—噠嗪基、6 —噠嗪基、2 —嘧啶基、4 —嘧啶基、5_嘧 陡基、ό —喃Π定基、2 — D|t嗪基、3 — D[t嗪基、5 — D比嗪基、 - 6 —吼嗪基、2 —噻哩基、4 —噻哩基或噻哩基。 舉例（但不限定）而言，氮鍵結性雜環乃在氮丙啶、 雜氮環丁院、吼略、吼略症、2 - Dtt略啉、3 — Dtfc略啉、咪 ® 唑、咪唑啶'2 —咪嗖啉、3 —咪唑啉、吡唑、吡唑啉、2 —毗唑啉、3 —吡唑啉、哌啶、哌嗪、吲哚、吲哚琳、1 H -问丨哩之1位置’異吲哚或異吲哚啉之2位置，嗎啉之4 位置及咔唑或β-咔啉之9位置鍵結。更典型之氮鍵結性 雜環包括1—氮丙啶基、1—雜氮環丁烷基、丨—吡咯基、 1 一咪唑基、1 —吡唑基及1 _哌啶基。 "碳環〃意指在單環時具有3至7個碳原子，在二環 時具有7至12個碳原子且在多環時具有至多2〇個碳原子 之飽和、不飽和或芳族環。單環型碳環具有3至6個環原 -30- (27) 1362934 子’更常具有5或6個環原子。二環型碳環具有7至12 個環原子，例如排列成二環[4,5]、[5,5]、[5,6]或[6,6]系 統’或者具有9或10個環原子而排列成二環[5,6]或[6,6] 系統。單環型碳環之實例包括環丙基，環丁基、環戊基、 1 一環戊—1 —烯基' 1 一環戊—2 -烯基、1 一環戊—3 —烯 基、環己基、1 一環己—1—燃基、1_環己一2 —嫌基、1 一環己~3—烯基、苯基 '螺基及萘基。 φ &連結者〃意指含有共價鍵或鏈或原子基團之化學部 分，其可將膦酸酯基團共價接合至藥物上。連結者包括取 代基A1及A3之部分，其包括諸如以下等部分：重覆單位 之烷氧基（例如聚乙烯氧基、PEG、聚甲烯氧基）及烷胺 ^ 基（例如聚乙烯胺基、Jaffamine ™ ):及二酸酯及醯胺 t 類包括琥珀酸酯、琥珀醯胺、二羥基乙酸酯及己醯胺。 所謂"手性〃乃意指對其鏡像夥伴具有不可重疊性質 之分子，而所謂"非手性〃則意指可與其鏡像夥伴重疊之 φ 分子。 所謂"立體異構體〃意指化合物具有相同之化學架構 , ，但原子或基團在空間之排列不同。 a非對映異構體〃意指具有二或多個手性中心之立體 異構體，且其分子彼此間並非鏡像。非對映異構體具有不 同的物理性質，例如熔點、沸點、光譜性質及反應力。非 對映異構體之混合物可藉高解析度分析步驟諸如電泳及層 析法予以分離》 "對映體〃意指化合物之兩種立體異構體’其彼此之 -31 - ⑧ (28) 1362934 間爲不可重疊之鏡像。 所謂^治療"有關疾病或病況之程度乃包括預防疾病 或病況之發生’抑制疾病或病況，消除疾病或病況，及/ 或減輕疾病或病況之一或多種症狀。 本文中所用之立體化學定義及慣例通常遵循S. P. Parker, Ed., McGraw-Hill Dictionary of Chemical Terms ( 1 984) McGraw-Hill Book Company, New York;及 Eliel， E.及 W i 1 e n，S ·，S t e r 〇 c h e m i s t r y o f 〇 r g a n i c C o m p o u n d s (1994) John Wiley & Sons, Inc.，New York。許多有機化 合物係以旋光形式存在，亦即彼等具有旋轉平面偏振光之 平面之能力。在旋光化合物之說明中，字首D及L或R ^ 及S係用以意指分子關於其手性中心之絕對構型。字首d ^ 及1或（+)及（_)則指出化合物所致之平面偏振光之 旋轉現象，以（-)及1代表化合物爲左旋。字首爲（+ )或d之化合物爲右旋。既定之化學結構方面，這些立體 ® 異構體係相同，惟彼等彼此爲鏡像。立體特異異構體亦可 稱爲對映體，而這些異構體之混合物通常稱爲對映體混合 έ 物。50: 50之對映體混合物通常稱爲消旋混合物或消旋 物，其可能在化學反應或過程中沒有立體選擇或立體特異 性時發生。所謂"消旋混合物〃或"消旋物"乃指兩種對 映體類別之等莫耳混合物，不具旋光性。 保護基團 本發明全文中，保護基團包括前藥部分及化學保護基 -32- ⑧ (29) 1362934 團。 保護基團爲可取得’普遍已知及使用，且在合成步驟 期間’亦即製備本發明化合物之路徑及方法期間隨意地用· 以預防保護基團之側反應。就大部分而言，決定哪些基團 待保護，當進行保護作用時，化學保護基團"PG 〃之特 性乃依待保護之反應化學（例如酸性、鹼性、氧化性、還 原性或其它狀況）及所欲之合成方向而定。如果化合物經 φ 多重PG所取代，則PG不需相同，且通常不相同。pg通 常用以保護官能基團諸如羧基、羥基 '硫基、或胺基團， .故可預防側反應或另外促成合成效率。進行去保護以得游 離去保護基團之次序乃依所欲之合成方向及所遭遇之反應 ^ 狀況而定，且可依技藝'者所決定之任何次序發生。 * 本發明化合物之各種不同之官能基團可經保護。例如 ，供一 0H用之保護基團（無論是否爲羥基、羧酸、膦酸 或其它官能基）包括"醚一或酯一形成性基團〃。醚一或 • 酯-形成性基團可充作本文所示合成反應圖中之化學保護 基團。然而，就熟知技藝者已知，一些羥基及硫基保護基 團既非醚-形成性亦非酯-形成性基團，且包括下列所討 論之醯胺。 極大量之羥基保護基團及醯胺-形成性基團及相關之 化學裂解反應乃述於 Protective Groups in Organic Synthesis, Theodora W. Greene (John Wiley & Sons, Inc., New York，1 99 1, ISBN 0-47 1 -6230 1 -6) ("Greene")。亦參 見 Kocienski, Philip J.; Protecting Groups (Georg Thieme -33- ⑧ (30) 1362934
Verlag Stuttart, New York, 1994)，其乃整體倂入文中以 供參考。尤其 Chapter 1, Protecting Groups: An Overview, pages 1-20, Chapter 2, Hydroxyl Protecting Groups, pages 21-94， Chapter 3， Diol Protecting Groups, pages 95-117， Chapter 4， Carboxyl Protecting Groups, pages 118-154, Chapter 5, Carbonyl Protecting Groups pages 155-1 84。供羧酸、膦酸、磺酸用之保護基團及供酸 φ 用之其它保護基團請參見下示之Greene。.此些基團之實 例包括，但不限定於，酯、醯胺及醯肼等。 醚一及酯一形成性保護基團 ^ 酯-形成性保護基團包括：（1)膦酸酯一形成性保 " 護基團諸如胺基膦酸酯、硫代膦酸酯、膦酸酯及雙-胺基 膦酸酯；（2)羧酸酯_形成性基團，及（3)硫酯_形成 性基團，諸如磺酸酯、硫酸酯及亞磺酸酯。 ® 本發明化合物之隨意膦酸酯部分可爲或可不爲前藥部 分，亦即彼等可能受或可能不受水解或酵素性裂解作用或 修飾作用所影響。某些膦酸酯部分於大部分或幾乎所有代 謝狀況下均安定。例如，二烷基膦酸酯，其中烷基團具有 二或多個碳，可因爲徐緩之水解速率而具有可感知之安定 性。 在膦酸酯前藥部分之文節中，有大量之結構不同之前 藥業已述及供滕酸所用（Freeman及R〇ss in Progress in Medicinal Chemistry 34: 112-147 ( 1997))且涵蓋在本 (31) 1362934 發明之範圍內。例示之膦酸酯-形成性基團爲具有下式之 亞結構A3中之苯基碳環：
其中Ri可爲Η或C1-C12院基；ml爲1、2、3、4、5 、6、7或8且苯基碳環經0至3個R2基團取代。當Y, 爲〇時，形成乳酸酯，當Υι爲N(R2) 、N( 0R2 )或 N ( N ( R2 ) 2時，Μ產生胺基膦酸酯。 在此酯-形成角色中，保護基團通常結合至任何酸性 基團諸如（但不限定於）_ C02H或―C(S) 0Η基團上 ，因而形成一 C02Rx，其中Rx乃如同本文中所定義》 保護基團之實例包括·’ C3-C12雜環（上述）或芳基。這些芳族基團隨意地 爲多環型或單環型。實例包括苯基，螺基，2—或3_吡 咯基，2 —及3—噻吩基，2-及4 一咪唑基，2_、4_及 5 -噁唑基，3 —及4 -異噁唑基，2—、4 一及5 -噻唑基 ，3_、4_及5 —異噻唑基’ 3 —及4 —吡唑基，1_、2_ 、3 -及4 —咄啶基，及1—、2—、4 —及5 —嘧啶基。 C3-C12雜環或芳基，且經鹵基、R1、 C12烷撐、C12烷氧基、CN、N〇2、OH、羧基、羧酸 酯、硫赶、硫酯、CpCu鹵烷基（1— 6個鹵素原子）、 -35- ⑧ (32) 1362934 C2—Cl2烯基或C2— C12炔基。此些基團包括2_、： 4 一烷氧基苯基（G-Cu烷基），2—、3 —及4 -甲 苯基，2_、3_及4 —乙氧基苯基，2,3—、2,4—、 、2,6—、3,4_及 3,5 —二乙氧基苯基，2_及3-乙 _4_羥苯基，2 —及3_乙氧基一 4_羥苯基，2_及 乙氧基_5—羥苯基，2_及3 -乙氧基—6—羥苯基 、3 —及4—0 —乙醯基苯基，2-、3 —及4 —二甲胺 基，2_、3_及4_甲疏基苯基，2_、3—及4_鹵 (包括2_、3_及4 一氟苯基及2-、3 —及4 一氯苯 ，2,3- 、2,4- 、2,5- 、2,6— 、3,4-及 3,5 —二甲 ，2,3 —、2,4—、2,5 —、2,6 —、3,4 —及 3,5 -雙羧 * 苯基，2,3—、2,4_、2,5_、2,6—、3,4—及3,5_ - 氧基苯基，2,3 —、2,4 —、2,5 _、2,6 —、3,4-及
二鹵基苯基（包括2,4—二氟苯基及3,5-二氟苯基 -、3 -及4 -鹵烷基苯基（1至5個鹵素原子，G # 烷基包括4一三氟甲苯基），2_、3 _及4_氰苯基 、3 —及4 —硝苯基，2-、3-及4_鹵烷基苄基（1 個鹵素原子，C^—Cu烷基包括4_三氟甲基苄基及： 3 —及 4 一三氯甲苯基），4—N_甲基哌啶基，3_：N 基哌啶基，1 -乙基哌嗪基，苄基，烷基水楊基苯基 一 C4烷基包括2—、3 —及4_乙基水楊基苯基），： 3—及4—乙醯基苯基，1,8—二羥萘基（-C1GH6-OH) 氧基乙基[C6-C9芳基（包括苯氧基乙基）]，2,2' — 基聯苯基，2_、3_及4_N,N_二烷胺基酚， 卜及 氧基 2.5 — 酯基 3 -，2 -基苯 苯基 基） 苯基 乙基 二甲 3.5 -)，2 -C12 ，2 - 至5 I — > j —甲 (C, I —、 及芳 二羥 -36- ⑧ (33) 1362934 -C6H4CH2-N(CH3) 2，三甲氧基苄基，三乙氧基苄基，2 —烷基吡啶基（C, - C4烷基）；
2 —羧苯基之C4-C8酯；及Ci-Cd烷撐—C3— C6芳基（ 包括节基、—CH2 —哦略基、—CH2 —嚷吩基、—CH2 —味 哩基、一CH2 —嚼哗基、一 CH2 —異嚼吨基、一CH2 —噻哩 基、一CH2 -異噻唑基、一CH2 -吡唑基、〜CH2 —吡啶基 及一CH2 —嘧啶基）且其於芳基部分中經3至5個幽素原 子或1至2個擇自鹵素、Ci—Cu烷氧基（包括甲氧基及 乙氧基）、氰基、硝基、OH、Ci— Ci2鹵垸基（1至6個 鹵素原子；包括一 CH2CC13) 、C, — C12烷基（包括甲基 及乙基）、C2— C12烯基或C2— C12炔基所取代；烷氧基 乙基[Ci-Ce烷基包括 一CH2-CH2— 〇— CH3(甲氧基乙 基）];經上述供芳基用之任何基團尤其是0H或1至3 園素原子取代之院基（包括—CH3、— CH(CH3) 2、 -C ( CH3 ) 3、- CH2CH3 ' - ( CH2 ) 2CH3 ' -(CH2 ) 3CH3 ' - ( CH2 ) 4CH3 ' - ( CH2 ) 5CH3 ' -CH2CH2F ' - CH2CH2CI ' - CH2CF3 及—CH2CC13 ); v_y ;—N_2_丙基嗎啉基、2,3 —二氫基—6 -羥基茚、芝麻 -37- ⑧ (34) 1362934 酚、兒茶酚單酯、—CH2-C(0) — NCR1) 2、 -CH2 - S ( Ο ) ( R1 ) ^ - CH2 - S ( 0 ) 2 ( R1 )、 -ch2 - ch ( oc ( o ) ch2r' ) 、—ch2(oc(o) ch2r' )、膽固醇酯、烯醇丙酮酸酯（HOOC-C(=CH2) —） 、甘油； 5或6個碳之單醣、雙醣或寡醋（3至9個單醣殘基 )； φ 三酸甘油酯諸如α — D—沒一二甘油酯（其中含有甘 油酯之脂肪酸通常爲天然存在之飽和或不飽和C2.26、 <：6.,8或C6.ie脂肪酸諸如亞油酸、月桂酸、肉豆蔻酸、棕 櫚酸、硬脂酸、油酸、棕櫚油酸、亞麻酸等脂肪酸，彼等 * 乃經由三酸甘油酯之甘油基氧而連接至母化合物上； * 磷脂，其乃經由磷脂中之磷酸酯而連接至羧基團上； 醜基（示於 Clayton et al·，为 Chemo. ( 1 974) 5 (6): 670-67 1 )之圖 1 中）； Φ 環型碳酸酯諸如（5-Rd_2 -合氧基_1，3 -二噁茂 燃一 4 —基）甲醋（S a k a m 〇 t 〇 e t a 1.，C Λ e w. P//a r m · 5 w / /. ( 1 984) 3 2 (6) 224 1 -2248 )，其中、爲 R!、R4 或芳基； 及 /"\ -ch2c(o)n^^o 本發明化合物中之羥基團隨意地經WO 91/2 1 604中 所揭示之基團III、IV或V中之一者，或經異丙基取代。 表A列出保護基團酯部分之實例，其（例如）可經 由氧而鍵結至— c(o) Ο-及—p(o) (〇—）2基團上 ⑧ -38- (35) 1362934 。一些醯胺化物亦顯示可直接鍵結至—C(0)—或 -P(0) 2 上。結構 1— 5、8-10 及 16、17、19-22 之 酯係藉令本文中具有游離羥基之化合物與相關之鹵化物（ 氯化物或醯基氯等）及N，N-二環己基_N—嗎啉甲脒（ 或其它鹼諸如DBU、三乙胺、CsC03、Ν,Ν —二甲基苯胺 等）於Ν，Ν-二甲基甲醯胺（或其它溶劑諸如乙腈或Ν — 甲基吡咯酮）中起反應而合成。當待保護之化合物爲膦酸 • 酯時’結構5— 7、11、12、21及23— 26之酯係藉令醇或 醇化物鹽（如爲化合物諸如1 3、1 4及1 5，則令相關之胺 )與單氯膦酸酯或二氯膦酸酯（或其它活化膦酸酯）起反 應而合成。 ⑧
(36)1362934
表A 10. -CH2-0-C(0)-C(CH3)3 11. -CH2-CCI3 12. -C6H5 13. -NH-CH2-C(0)0-CH2CH3 14. -N(CH3)-CH2-C(0)0-CH2CH3 15. -NHRi 16. -CH2-0-C(0)-Ci〇Hi5
1. -CH2-C(0)-N(R])2 * 2. -CH2-S(0)(Ri) 3. -CH2-S(0)2(Ri) 4. -CH2-0-C(0)-CH2-C6H5 5. 3-膽固醇酯 6. 3-吡啶基 7. N-乙基嗎啉基 8. -CH2-〇-C(0)-C6H5 9. -CH2-0-C(0)-CH2CH3 17. -CH2-0-C(0)-CH(CH3)2 18. -CH2-C#H(0C(0)CH2Ri)-CH2--(0C(0)CH2Ri)*
19. 22.
# 一手性中心爲（R ) 、（ S )或消旋物。 適於供本文中使用之其它酯乃述於EP 63 2048中， 保護基團亦包括t雙重酯〃形成性前官能基諸如 -40- ⑧ (37)1362934 -CH2〇C(0)OCH3， Ο -CH2SCOCH3, -CH2〇CON(CH3)2 或結構一CIUR1 或 W5) Ο ( (CO) R37)或-CHCR1 或 W5) ( (CO) OR38)之烷基一或芳基-醯氧基烷基團（ 連接至酸性基團之氧上），其中R37及R38爲烷基、芳基 或烷芳基團（參見美國專利第4968788號）。尺37及R38 經常爲龐大的基團諸如分支烷基、鄰位_經取代芳基、間 位-經取代芳基或其組合，包括具1至6個碳原子之正、 第二、異一及第三烷基。其實例爲戊醯氧基甲基團。彼等 特別適於與前藥一起供口服。此些有用之保護基團之實例 爲烷基醯氧基甲酯及其衍生物，.包括一 CH( C2CH2OCH3
)oc ( O ) C ( ch3) 3， -CH2OC ( O) C,〇H,5 ' -CH2OC ( O) C ( CH3) 3 ' -CH ( CH2OCH3 ) oc ( 0 ) c ( ch3) 3， -CH ( CH ( CH3 ) 2 ) OC ( O ) C ( CH3 ) 3， -CH2OC ( O) CH2CH ( CH3) 2 5 -ch2oc ( o) c6h,, > -CH2OC ( O) C6H5 ' -CH2OC ( 0) C,〇Hi5 ' -CH2OC ( O) CH2CH3 ' -CH2OC (0) CH ( CH3) 2 > -CH2OC ( 0 ) C ( CH3 ) 3 及- CH20C ( 0) CH2C6H5〇 一些實施例中，經保護之酸性基團爲酸性基團之酯且 爲含羥基之官能基之殘基。其它實施例中，胺基化合物乃 用以保護酸官能基。適當之含羥基或胺基之官能基之殘基 -41 · (38) 1362934 乃示於上或見於WO 95/0 7920中。尤其是胺基酸、胺基 酸酯、多聚肽或芳基醇之殘基。典型之胺基酸、多聚肽及 羧基一酯化胺基酸殘基乃以基團L1或L2述於 WO 95/07920 第 11-18 頁及相關內容中。WO 95/0 7920 明白地教示膦酸之醯胺化物，但此些醯胺化物當然係以本 文中所示之任何酸基團與WO 95/07920中所示之胺基酸 殘基形成。 φ 供保護酸性官能基用之典型酯亦述於 WO 95/07920 中，同樣地，相同的酯當然可以本文中所述之酸性基團與 ’920公告中之膦酸酯形成。典型之酯基團至少於 WO 95/07920 第 89-93 頁（於 R31 或 R35 內）、第 105 頁 ' 之表及第21- 23頁（以R代表）定義。尤其爲未經取代 - 芳基諸如苯基或芳烷基諸如苄基，或經羥基-、鹵基-、 烷氧基-、羧基-及/或烷酯羧基-取代之芳基或烷芳基 ，特別是苯基、鄰位—乙氧基苯基、或（^一（：4烷酯羧基 # 苯基（水楊酸酯烷酯）等之酯。 經保護酸性基團，尤其當使用 WO 95/0792〇之酯或 醯胺時，乃有用以作爲供口服用之前藥。然而，欲使本發 明化合物有效藉經口路徑投服，不必然要將酸性基團保護 。當具有保護基團（尤其胺基酸醯胺化物或經取代及未經 取代芳酯）之本發明化合物系統或經口投服時，彼等可於 活體內水解性裂解以產生游離酸。 有一或多個酸性羥基經保護。如果有一個以上之酸性 羥基經保護時，乃使用相同或互異之保護基團，例如酯可 -42- ⑧ (39) 1362934 互異或相同，或者可使用混合型醯胺化物及酯。 述於Greene (第14— 118頁）中之典型羥基保護基 團包括經取代甲基及烷基醚，經取代苄基醚，甲矽烷基醚 ，酯類包括磺酸酯及碳酸酯。例如： •醚類（甲基、第三丁基、烯丙基）； •經取代甲基醚類（甲氧基甲基、甲硫基甲基、第三 丁硫基甲基、（苯基二甲基甲矽烷基）甲氧基甲基、苄氧 • 基甲基 '對位_甲氧基苄氧基甲基、（4 -甲氧基苯氧基 )甲基、癒瘡木酚甲基、第三丁氧基甲基、4 一戊烯氧基 甲基、甲矽烷氧基甲基、2 —甲氧基乙氧基甲基、2，2,2— 三氯乙氧基甲基、雙（2_氯乙氧基）甲基、2_ (三甲基 '甲矽烷基）乙氧基申基、四氫吡喃基、3 -溴基四氫吡喃 • 基' 四氫噻喃基、1 一甲氧基環己基、4 —甲氧基四氬吡喃 基、4一甲氧基四氫噻喃基、—二氧撐、1_[(2—氯 基一4 一甲基）苯基]-4 -甲氧基哌啶一4 —基、1,4 一二 • 噁烷一 2~基、四氫呋喃基、四氫噻呋喃基、2,3,3a，4,5, 6,7,7a —八氫一 7,8,8_三甲基_ 4,7 —甲撐苯並呋喃—2_ 基））； •經取代乙基醚類（1—乙氧基乙基、1 一（2 一氯乙 氧基）乙基、丨一甲基一1—甲氧基乙基、丨―甲基―丨一苄 氧基乙基、1 一甲基_1_苄氧基—2 —氟乙基、2,2,2—三 氯乙基、2~三甲基甲矽烷基乙基、2—（苯基硒基）乙基 )， •對位-氯苯基、對位一甲氧基苯基、2,4 一二硝基 -43- ⑧ (40) 1362934 苯基、苄基； •經取代苄基醚類（對位一甲氧基苄基、3，4 一二甲 氧基节基、鄰位-硝苄基、對位-硝苄基、對位-鹵苄基 、2，6_二氯基苄基 '對位_氰苄基、對位一苯基苄基、2 —及4 —吼啶甲基、3_甲基一 2 —吡啶甲基w一氧撐、二 苯甲基、p，p，—二硝基二苯甲基、5_二苯並環庚基、三苯 甲基、α -萘基二苯甲基、對位—甲氧基苯基二苯甲基、 Φ 二（對位~甲氧基苯基）苯甲基、三（對位-甲氧基苯基 )甲基、4~ (4，—溴苯醯甲氧基）苯基二苯基甲基， 4,4·，4" —參（4,5一二氯酞醯亞胺基苯基）甲基、4,4’，4"_ 參（乙醯丙醯氧基苯基）甲基、4,4'，4”一參（苄氧基苯基 ' )甲基、3—(咪唑一1—基甲基）雙（4，，4"一二甲氧基苯 ν 基）甲基、1,1—雙（4 —甲氧基苯基）一Γ —芘甲基、9 — 蒽基、9~ (9_苯基）咕噸基、9— (9 —苯基_10—合氧 基）蒽基、1，3_苯並二噻茂烷一 2—基、苯並異噻唑基 • 二氧撐）； •甲矽烷基醚類（三甲基甲矽烷基、三乙基甲矽烷基 、三異丙基甲矽烷基、二甲基異丙基甲矽烷基、二乙基異 丙基甲矽烷基、二甲基乙基甲矽烷基 '第三丁基二甲基甲 矽烷基、第三丁基二苯基甲矽烷基、三苄基甲矽烷基、三 一對位一二甲苯基甲矽烷基、三苯基甲矽烷基、二苯基甲 基甲矽烷基、第三丁基甲氧基苯基甲矽烷基）； •酯類（甲酸酯、苯醯甲酸酯、乙酸酯、氯乙酸酯、 二氯乙酸酯、三氯乙酸酯、三氟乙酸酯、甲氧基乙酸酯、 -44- ⑧ (41) 1362934 三苯基甲氧基乙酸酯、苯氧基乙酸酯、對位-氯基苯氧基 乙酸酯、對位一聚一苯基乙酸酯、3_苯基丙酸酯、4 —合 氧基戊酸酯（乙醯丙酸）、4,4一 （乙撐二硫基）戊酸酯 、特戊酸酯、金剛酸酯、巴豆酸酯、4-甲氧基巴豆酸酯 '苯甲酸酯、對位一苯基苯甲酸酯、2,4,6 -二甲基苯甲 酸酯）； •碳酸酯類（甲酯、9 -芴甲酯、乙酯、2,2,2 -三氯 φ 乙酯'2—(三甲基甲矽烷基）乙酯、2_ (苯磺醯）乙酯 、2—(三苯膦基）乙酯、異丁酯、乙烯酯、烯丙酯、對 位一硝基苯酯、苄酯、對位一甲氧基苄酯、3,4 -二甲氧 基苄酯、鄰位一硝基苄酯、對位一硝基苄酯、硫碳酸S-^ 苄酯、4一乙氧基一 1—萘酯、二硫碳酸甲酯）； 、•具有協助裂解能力之基團（2 -碘基苯甲酸酯、4一 疊氮基丁酸酯、4_硝基一 4 一甲基戊酸酯、鄰位一（二溴 甲基）苯甲酸酯、2 —甲醯苯磺酸酯、碳酸2— （甲硫基 • 甲氧基）乙酯、4—(甲硫基甲氧基）丁酸酯、2_ (甲硫 基甲氧基甲基）苯甲酸酯）；各種酯類（2,6—二氯基—4 —甲基苯氧基乙酸酯、2,6_二氯基一 4_ (1，1,3,3—四甲 基丁基）苯氧基乙酸酯、2,4—雙（1，1_二甲基丙基）苯 氧基乙酸酯、氯基二苯基乙酸酯、異丁酸酯、單琥珀酸酯 、（£)-2 -甲基一2 - 丁烯酸酯、鄰位一(甲氧羰基） 苯甲酸酯、對位一聚一苯甲酸酯、α -萘甲酸酯、硝酸酯 、Ν,Ν，Ν’，Ν’ —四甲基二胺基磷酸烷酯、# -苯基胺基甲酸 酯、硼酸酯、二甲基硫代磷酸酯、2,4—二硝苯基次磺酸 -45- ⑧ (42) 1362934 酯）；及 •磺酸酯（硫酸酯、甲磺酸酯、苄磺酸酯、甲苯磺酸 酯）。 典型之1，2-二醇保護基團（其中兩個〇H基團通常 與保護基團結合一起）乃述於Greene第118 - 142頁中且 包括環型縮醛及縮酮（甲叉 '乙叉、1 一第三丁基乙叉、1 —苯基乙叉、（4 —甲氧基苯基）乙叉' 2,2,2 —三氯乙叉 φ 、異丙叉、環戊叉、環己叉、環庚叉、苄叉、對位一甲氧 基苄叉、2,4 -二甲氧基苄叉、3，4_二甲氧基苄叉、2 — 硝基苄叉）；環型原酸酯（甲氧基甲叉、乙氧基甲叉、二 甲氧基甲叉' 1—甲氧基乙叉、1_乙氧基乙叉' 1，2—二 * 甲氧基乙叉、α —甲氧基苄叉、1_ ( iV,>—二甲胺基）乙 ' 叉衍生物、α - -二甲胺基）苄叉衍生物、2—氧雜 環戊叉）：甲矽烷基衍生物（二-第丁基甲矽烷叉基團、 1，3 — （1,1，3,3-四異丙基二矽氧烷叉），及四_第三丁 ® 氧基二矽氧烷一1,3—二叉），環型碳酸酯，環型硼酸酯 、删酸乙酯及硼酸苯酯。 更典型之1,2-二醇保護基團包括示於表Β中者，更 尤其爲環氧化物、異丙叉、環型縮酮及環型縮醛。 -46 ⑧ 1362934 (43) B 表 Λ ο
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爲 9 R 中 其 基 烷 胺基保護基團 另一組保護基團包括述於Greene第3 1 5 — 3 85頁之任 何典型胺基保護基團。其包括： •胺基甲酸酯類：（甲酯及乙酯、9 一芴甲酯、9(2 —礦基）芴甲酯、9— (2,7_二溴基）芴甲酯' 2,7—二 —第三 丁基—[9_ ( 二合氧基一 1〇，1〇1〇1〇一四 氫噻噸基）]甲酯、4 一甲氧基苯醯甲酯）； •經取代乙基：（2,2,2 —三氯乙基、2 —三甲基甲矽 甲基一2 -鹵乙基、1,1—二甲基一2,2 -二溴 二甲基一 2,2,2 —三氯乙基、1 一甲基一1— (4 —聯苯基）乙基、1- (3,5 —二一第三丁苯基）一1_甲 基乙基'2〜（2ι —及4，_吡啶基）乙基、2_ 一二 環己基甲酿胺基）乙基、第三丁基、1_金剛烷基、乙烯 基、燦丙基、1—異丙基烯丙基、肉桂基' 4_硝基肉桂基 -47- 院基乙基、2—苯乙基、I— (1—金剛烷基）一1 一甲基乙 基、1,1 - 乙基 (44) 1362934 、8—喹啉基、#一羥基哌啶基、烷二硫基、苄基 '對位一 甲氧基苄基、對位-硝苄基、對位-溴苄基、對位一氯苄 基、2,4 —二氯苄基、4 一甲亞磺醯苄基、9_蒽甲基、二 苯甲基）； •具有協助裂解能力之基團：（2 —甲硫基乙基、2_ 甲磺醯乙基、2-(對位一甲苯磺醯）乙基、2_[(1,3_ 二噻烷基）]甲基、4 —甲硫基苯基、2，4 一二甲硫基苯基 φ 、2 -磷甕基乙基、2 —三苯基磷甕基異丙基、1,1—二甲 基一 2—氰乙基、間位—氯基一對位-醯氧基苄基、對位 一（二羥氧硼基）苄基、5—苯並異噁唑基甲基、2—(三 氟甲基）一6 —色酮基甲基）； * •可進行光解性裂解作用之基團：（間位一硝苯基、 ^ 3,5 —二甲氧基苄基 '鄰位—硝苄基、3，4 一二甲氧基一 6 -硝苄基、苯基（鄰位一硝苯基）甲基）：脲型衍生物（ 吩噻嗪基—（10)—羰基、ΛΤ —對位一甲苯磺醯胺羰基、 # V-苯胺硫羰基）； •各種胺基甲酸酯類：（第三戊酯、硫代胺基甲酸S 一苄酯、對位~氰苄酯、環丁酯、環己酯、環戊酯、環丙 基甲酯、對位一癸氧基苄酯、二異丙基甲酯' 2,2—二甲 氧羰基乙烯酯、鄰位—（iV,W—二甲基甲醯胺基）苄酯、 1,1—二甲基~3 一 二甲基甲醯胺基）丙酯、1，1 一 二甲基丙炔酯 '二（2—吡啶基）甲酯、2 —呋喃基甲酯、 2 —碘乙酯、異冰片酯、異丁酯、異菸鹼酯、對位一 （P’ 一甲氧基苯偶氮基）苄酯、1 一甲基環丁酯、1 一甲基環己 -48 - (45) 1362934 酯、1—甲基—1〜環丙基甲酯、甲基(3,5—二 甲氧基苯基）乙酯、1一甲基_1一（對位一苯偶氮基）乙 酯、1—甲基—1〜苯乙酯、1_甲基一 1_ (4_吡啶基） 乙酯、苯酯、對位〜（苯偶氮基）苄酯、2,4,6_三—第 三丁苯酯、4_ (3甲銨）苄酯、2 4 6 一三甲基苄酯）； •醯胺類（W〜甲醯、乙醯、；V 一氯乙醯、N —三 氯乙醯、三氟乙醯' 苯乙醯、"一 3_苯丙醯、W - # 皮考啉醯、"_3\吡啶基甲醯胺、w—苯醯苯基丙胺醯、 "一苯醯、#—對位〜苯基苯醯）； •具有協助裂解能力之醯胺類：（TV-鄰位—硝苯基 乙醯、斤一鄰位一硝苯氧基乙醯、乙醯乙醯、UT-二 # 硫基苄氧羰胺基）乙醯、w_3_ (對位一羥苯基）丙醯、 . 3—(鄰位一硝苯基）丙醯、；v— 2—甲基一2—(鄰位 -一硝苯氧基）丙酿、N_2 —甲基一 2—(鄰位一本偶氮基 苯氧基）丙醯、ΑΓ— 4_氯丁醯、iV— 3_甲基—3 —硝基丁 # 醯 ' "二鄰位—硝基肉桂醯、乙醯蛋胺酸、# —鄰位一 硝基苯醯、鄰位—（苯醯氧基甲基）苯醯、4,5一二苯 基—3 —噁唑啉-2 —酮）； •環型亞醯胺衍生物：（# —酞醯亞胺、# —二硫雜 琥珀醯、2,3—二苯基馬來醯、ΛΓ — 2,5 —二甲基吡咯基 、W—l，l，4,4 —四甲基二甲矽烷基氮雜環戊烷加合物、5_ 經取代之1,3 —二甲基_1，3,5_三氮雜環己一2 —酮、5 — 經取代之1,3 —二苄基_1，3,5_三氮雜環己一 2_酮、1一 經取代之3，5 —二硝基一 4 一吡啶酮基）； -49- (46) 1362934 • 烷基及iV —芳基胺類：（iV_甲基、iV_烯丙基 、7V_[2_ (三甲基甲矽烷基）乙氧基]甲基、N_3_乙醯 氧基丙基、iV -（ 1_異丙基一 4 —硝基_2_合氧基—3_ 吡略啉一 3_基）、四級銨鹽、#一苄基、二（4 —甲 氧基苯基）甲基、5_二苯並環庚基、iV-三苯甲基、 (4 —甲氧基苯基）二苯甲基、N—9 —苯芴基、；V — 2,7 —二氯基-9—芴基甲叉、二茂鐵基甲基、汉一2_ φ 吡啶甲基胺N1—氧化物）； .亞胺類：（#— ι，ι_二甲硫基甲叉苄叉、；V _對位一甲氧基苄叉、# 一二苯基甲叉' [(2 —吡啶基 )采基]甲叉、W,iV'，Ar -二甲胺基甲叉、ΑΓ,ΑΓ -異丙叉、
> ΑΓ—對位一硝基苄叉、ΑΓ_水楊叉、iV_5-氯基水楊叉、TV • _ (5—氯基_2—羥苯基）苯甲叉、iV_ (5_氯基一2_ 羥苯基）苯甲叉、#_環己叉）； •烯胺衍生物：（#— (5,5 —二甲基_3_合氧基_1
• #一金屬衍生物（#_甲硼烷衍生物、#_二苯基烴 基硼酸衍生物、iV— [苯基（五羰基鉻一或一鎢）]羰基、# 一銅或W—辞整合物）； •N—N衍生物：（#_硝基、亞硝基、N —氧化 物）； • N—P衍生物（# —二苯膦醯、W —二甲硫膦醯、# _二苯硫基膦醯、W-二烷基磷醯、；V —二苄基磷醯' W — 二苯基磷醯）； -50- ⑧ (47) 1362934
• N— Si衍生物、N_S衍生物及N —亞磺醯衍生物 :(#_苯亞磺醯、#_鄰位一硝基苯亞磺醯、#_2,4_ 二硝基苯亞磺醯、；V —五氯苯亞磺醯、Ν_2 —硝基_4_ 甲氧基苯亞磺醯、#_三苯甲亞磺醯、#_3_硝基吡啶亞 磺醯）：及磺醯衍生物（N—對位一甲苯磺醯、# 一苯 磺醯、#—2,3,6_三甲基_4一甲氧基苯磺醯、#_2,4,6_ 三甲氧基苯磺醯、#_2,6 —二甲基一 4_甲氧基苯磺醯、iV —五甲基苯磺醯、W_2,3,5,6 —四甲基_4_甲氧基苯磺醯 、#_4_甲氧基苯磺醯、TV— 2,4,6—三甲基苯磺醯、 2,6_二甲氧基_4一甲基苯磺醯、#_2,2,5,7,8_五甲基 色滿一6 —磺醯、iV—甲磺醯、iV — /3 —三甲基甲矽烷基乙 磺醯、；V—9-蒽磺醯、7V— 4 一（4’，8'—二甲氧基萘甲基） 苯磺醯、#一苄磺醯、#一三氟甲磺醯、# 一苯醯甲磺醯） 更典型之經保護胺基團包括胺基甲酯類及醯胺類，更 尤其爲_NHC(0) R1或— NsCVnCR1) 2。另一種保護 基團（亦有用以作爲供胺基及一NH ( R5 )用之前藥）爲 0
例如參見 Alexander, J. et al. ( 1 9 9 6) J · Med· Chem. 39: 480-486 。 胺基酸多肽保護基團及軛合物 -51 - ⑧ (48) 1362934 本發明化合物之胺基酸或多肽保護基團具有 R15NHCH (R16) C(0) —，R15爲H、胺基酸或多肽殘基 、或R5，且W6乃定義於下。 R16爲低級烷基或經胺基、羧基、醯胺、羧酯、羥基 、C6 — C7芳基、胍基、咪唑基、吲哚基、锍基、亞碾及 /或烷磷酸酯取代之低級烷基（<^一（：6) 亦與胺基 酸αΝ —起形成脯胺酸殘基（R1()=_CH2) 3_)。然而， φ R1通常爲天然存在之胺基酸之側基團諸如H，- CH3， CH ( CH3 ) 2，- CH2 - CH ( CH3) 2，— chch3 - ch2-C H 3 ' — C H 2 _ C 6 H 5 > — C H 2 C H 2 _ S 一 C H 3 J 一 C H 2 Ο H > —CH ( OH) - CH3，一 CH2- SH，CH2- C6H4OH，一 CH2 • - CO- NH2，一 CH2 - CH2 - CO - NH2，一 ch2- cooh， ‘ 一CH2 — CH2 - COOH，- ( CH2 ) 4- NH2 及一(CH2 ) 3 - N.H_C(NH2) NH2。R10亦包括1_胍基丙_3 —基、节基 、4 —羥苄基、咪唑_4 一基、吲哚一 3 —基、甲氧基苯基 # 及乙氧基苯基。 另一組保護基團包括含胺基之化合物之殘基、尤其是 胺基酸、多肽、保護基團、一 NHS02R、NHC(O) R、 -N(R)2、NH2、*-NH(R) (Η)，因而例如藉令羧 酸與胺起反應，亦即偶合，以形成例如於C ( 0 ) nr2中 之醯胺。膦酸可與胺起反愁以形成例如於一 P (〇 ) (OR) ( NR2)中之胺基膦酸酯。 胺基酸通常具有結構R17c(0) CH(R16) NH_ ’其 中R17爲_0H、— OR、胺基酸或多肽殘基。胺基酸爲低 -52- (49) 1362934 分子量之化合物，小於約10 00 MW且含有至少一個胺基 或亞胺基團及至少一個羧基團。胺基酸通常可於自然界中 發現，亦即可於生物學物料諸如細菌或其它微生物、植物 、動物或人類中檢出。適當的胺基酸通常爲《胺基酸，亦 即化合物之特徵爲有一個胺基或亞胺基氮原子藉由單一經 取代或未經取代之0：碳原子而與一個殘基團中之碳原子分 開。其尤其爲疏水性殘基諸如單-或二一院基或芳基胺基 # 酸、環烷基胺基酸等。這些殘基藉由增加母化合物的分配 係數而促成細胞滲透力。典型之殘基並不含有锍基或胍基 取代基。 天然存在之胺基酸殘基爲於植物、動物或微生物，尤 ” 其於其蛋白中所天然發現之彼些殘基。多肽實質上最常由 - 此些天然存在之胺基酸殘基所組成。這些胺基酸爲甘胺酸 、丙胺酸、纈胺酸、亮胺酸、異亮胺酸、絲胺酸、蘇胺酸 、半胱胺酸、蛋胺酸、谷胺酸'天冬胺酸、賴胺酸、羥基 • 賴胺酸、精胺酸、組織胺酸、苯丙胺酸、酪胺酸、色胺酸 、脯胺酸、天冬醯胺、谷醯胺及羥基脯胺酸。此外，非天 然之胺基酸例如纈丙胺酸、苯基甘胺酸及高精胺酸等亦涵 蓋在內。本發明中所用之所有胺基酸可爲D—或L 一光學 異構體。此外，其它擬肽亦有用於本發明中。一般之回顧 請參見 B. Weinstein, eds., Marcel Dekker, New York, p. 267 (1983)= 當保護基團爲單一胺基酸殘基或多肽時，彼等乃隨意 地於R3處經本發明化合物中之A 1、A2或A3取代基所取 -53- ⑧ (50) 1362934 代。這些軛合物係藉在胺基酸（或例如多肽之C-端胺基 酸）之羧基團間形成醯胺鍵而形成。同樣地，軛合物乃藉 在R3與胺基酸或多肽之胺基團間形成。通常，母分子之 任何位置中僅有一個位置經本文中所述之胺基酸所醯胺化 ，然而在一個以上之允許位置置入胺基酸亦在本發明之範 圍內。R3之羧基團一般係以胺基酸醯胺化。胺基酸之α -胺基或α -羧基團或多肽之終端胺基或羧基團通常乃鍵 φ 結至母官能基上，亦即胺基酸側鏈中之羧基或胺基團通常 並不用以與母化合物形成醯胺鍵（雖然這些基團可能需要 在如下進一步述及之軛合物之合成期間予以保護）》 有關胺基酸或多肽之含羧基之側鏈方面，羧基團當然 ， 可任予保護（例如以R1保護），以R5酯化或予以醯胺化 - 。同樣地，胺基側鏈R16可隨意地經R1保護或以R5取代 〇 此與側鏈胺基或羧基團形成之酯或醯胺鍵，與與母化 Φ 合物形成之酯或醯胺一樣，可隨意地於活體內或於試管內 於酸性（pH < 3 )或鹼性（pH > 5 )狀況下水解。另外， 彼等於人類胃腸道中具實質安定性，但可於血液或於細胞 內環境中酵素水解。酯或胺基酸或多肽醯胺化物亦有用以 作爲供製備含游離胺基或羧基團之母分子用之中間體。母 化合物之游離酸或鹼，例如，可藉慣用之水解步驟輕易地 由本發明之酯或胺基酸或多肽軛合物中形成。 當胺基酸殘基含有一或多個手性中心時，則可使用任 何D、L、內消旋、蘇或赤（如合適）消旋物、scaiemates -54 - (51) 1362934 或其混合物。通常’如果中間體欲非酵素性水解（例如當 使用醯胺作爲供游離酸或游離胺用之化學中間體），則D 異構體有用。另一方面，L異構體因可接受非酵素及酵素 性這兩種水解作用而富多樣性，且較易有效以藉由胃腸道 中之胺基酸或二肽基運送系統而運送。 適當之胺基酸之實例（其殘基以rx或Ry代表）包括 下列者： Φ 甘胺酸； 胺基聚羧酸類，例如天冬胺酸、/3 -羥基天冬胺酸、 谷胺酸、Θ -羥基谷胺酸、yS -甲基天冬胺酸、β 一甲基 谷胺酸、—二甲基天冬胺酸、r —羥基谷胺酸 '泠， • 7·-二羥基谷胺酸、/?—苯基谷胺酸、甲叉谷胺酸、 - 3 —胺基己二酸、2_胺基庚二酸、2_胺基辛二酸及2 — 胺基癸二酸； 胺基酸醯胺類，例如谷醯胺及天冬醯胺； Φ 聚胺基_或多元_單羧酸類諸如精胺酸、賴胺酸、/3 一胺基丙胺酸、r 一胺基丁胺酸、鳥胺酸、瓜胺酸、高精 胺酸、高瓜胺酸、羥基賴胺酸、別羥基賴胺酸 '及二胺基 丁酸； 其它鹼性胺基酸殘基諸如組織胺酸； 二胺基二羧酸類諸如α，α:’ —二胺基琥珀酸、α，α· —二胺基戊二酸、α，α，一二胺基己二酸、α，α，一二胺 基庚二酸、α，α：’一二胺基—沒―羥基庚二酸、αα，一 二胺基辛二酸、α，α：，—二胺基壬二酸及α，α，_二胺基 ⑧ -55- (52) 1362934 癸二酸； 亞胺基酸類諸如脯胺酸、羥基脯胺酸、別羥基脯胺酸 、7 —甲基脯胺酸 '哌可酸、5 —羥基哌丁酸、及氮雜環 丁烷一 2—羧酸； 單一或二—烷基（通常C, — C8分支或正鏈）胺基酸 諸如丙胺酸、纈胺酸、亮胺酸、烯丙基甘胺酸、丁胺酸、 正纈胺酸、正亮胺酸、庚胺酸' α —甲基絲胺酸、α —甲 基—甲基一r —經基戊酸、α —甲基一α —甲基一δ —羥基戊酸、α —甲基一α —甲基一ε —羥基己酸、異纈 胺酸、〇：_甲基谷胺酸、α —胺基異丁酸、α —胺基二乙 基乙酸、α —胺基二異丙基乙酸、α_胺基二正丙基乙酸 ‘ 、胺基二異丁基乙酸、α —胺基二正丁基乙酸、α_ ' 胺基乙基異丙基乙酸、α —胺基正丙基乙酸、α_胺基二 異戊基乙酸、α —甲基天冬胺酸、甲基谷胺酸、1一 胺基環丙烷-1-羧酸、異亮胺酸、別異亮胺酸 '第三亮 ^ 胺酸、yS —甲基色胺酸及胺基—乙基一沒一苯基 丙胺酸； yS —甲基絲胺醯； 脂族α —胺基—々—羥基酸類諸如絲胺酸、沒一羥基 亮胺酸、Θ -羥基正亮胺酸、/3 -羥基正纈胺酸及α—胺 基—/3 —羥基硬脂酸； α -胺基’ a —、r —、6 —或ε —羥基酸類諸如高 絲胺酸、δ -羥基正纈胺酸、r 一羥基正纈胺酸及ε —羥 基正纈胺酸殘基；刀豆胺酸及刀豆酸；r _羥基鳥胺酸。 -56- ⑧ (53) 1362934 2_己糖胺酸類諸如D—葡萄糖胺酸或D_半乳糖胺 酸； α —胺基-硫赶類諸如青黴胺、β -硫赶正纈胺 酸或/3_硫赶丁胺酸； 其它含硫之胺基酸殘基包括半胱胺酸；高半胱胺酸、 冷一苯基蛋胺酸、蛋胺酸、S_烯丙基—L —絲胺酸亞硯2 -硫赶組織胺酸、胱硫醚，及半胱胺酸或高半胱胺酸之硫 φ 赶醚； 苯基丙胺酸、色胺酸及經環取代之α -胺基酸諸如苯 基—或環己胺基酸；α —胺基苯乙酸、α _胺基環己基乙 酸及α _胺基一沒-環己基丙酸；苯基丙胺酸類似物及含 • 芳基、低級烷基、羥基、胍基、氧基烷基醚、硝基、硫或 - 經鹵基取代之苯基之衍生物（例如酪胺酸、甲基酪胺酸及 鄰位一氯基 '對位—氯基、3,4 —二氯基、鄰位一、間位 —或對位一甲基一、2,4,6 —三甲基一' 2 —乙氧基一5 — 0 硝基一、2 —羥基一 5—硝基—及對位一硝基一苯基丙胺酸 ):呋喃基一、噻吩基一、吡啶基-、嘧啶基嘌呤基 一或萘基-丙胺酸；及色胺酸類似物及衍生物包括犬尿素 '、3_羥基犬尿素、2 —羥基色胺酸及4一羧基色胺酸； α —胺基經取代之胺基酸包括肌胺酸（Ν -甲基甘胺 酸）、Ν—苄基甘胺酸、ν—甲基丙胺酸、Ν-苄基丙胺酸 、Ν—甲基苯基丙胺酸、Ν—苄基苯基丙胺酸、Ν —甲基纈 胺酸及Ν-苄基纈胺酸；及 α —羥基及經取代α 一羥基胺基酸類包括絲胺酸、蘇 ⑧ -57- (54) 1362934 胺酸、別蘇胺酸、磷酸絲胺酸及磷酸蘇胺酸。 多肽爲胺基酸之聚合物，其中一個胺基酸單體中之羧 基團乃藉由醯胺鍵而鍵結至下一個胺基酸單體之胺基或亞 胺基團上。多肽包括二肽、低分子量多肽（約1500 -5000 MW)及蛋白質。蛋白質隨意地含有3、5、10、50 、75、100或更多個殘基，且實質上與人類、動物、植物 或微生物蛋白具有序列-同源性，彼等包括酵素（例如過 φ 氧化氫酶）以及免疫原諸如KLH，或期望能引發免疫反 應之任何型式之抗體或蛋白。多肽之性質及特性可廣泛變 化。 多肽醯胺化物有用以作爲引發抗體之免疫原，其中抗 * 體乃供對抗多肽（如果其在所投服之動物體內無致免疫性 - )或對抗本發明化合物殘基上之表位。 可結合至非肽基之母化合物上之抗體乃（例如）於母 化合物之診斷及製造中用以將母化合物由混合物中分離出 Φ 。在密切同源之動物體內，母化合物與多肽之軛合物通常 比多肽更具致免疫性，因此使多肽更具致免疫性以促進其 抗體之產生。因此，多肽或蛋白在常用以引發抗體之動物 體內（例如兔 '鼷鼠、馬或鼠）不需具有致免疫性，但終 產物軛合物則必需於這些動物之至少一者中具有致免疫性 。多肽在鄰近於酸性雜原子之第一及第二個殘基之間之月太 鍵處隨意地含有肽解酵素裂解位。此裂解位乃藉由酵素-識 別結構例如藉肽解酵素所識別之殘基之特定序列而成側翼 ⑧ -58- (55) 1362934 供裂解本發明多肽軛合物之肽解酵素已詳知’且尤其 包括羧基肽酶。羧基肽酶藉移除C一端殘基而將多肽消化 ，且於許多狀態下，尤其對C —端序列具特異性。此酵素 及其基質必要物通常係已詳知。例如，二肽（具有既定配 對之殘基及游離羧基端）乃經由其α—胺基團而共價鍵結 至本文化合物之磷或碳原子上。在W!爲鱗酸酯之實施例 中，此肽預期藉由適當之肽解酵素而裂解，留下近側殘基 φ 中之羧基以自動化地將胺基膦酸鍵裂解。
適當之二肽基團（以其單字母密碼命名）爲ΑΑ，AR ，AN，AD，AC，ΑΕ，AQ，AG，AH，ΑΙ，AL，ΑΚ，AM ，AF，AP，AS，AT，AW，AY，AV，RA，RR，RN，RD 11 ，RC，RE，RQ，RG，RH，RI，RL，RK，RM，RF，RP
. ，RS，RT，RW，RY，RV，NA，NR，NN，ND，NC，NE
，NQ，NG，NH，NI，NL，NK，NM，NF，NP，NS，NT
，NW > NY， NV， DA， DR， DN， DD， DC， DE， DQ， DG， DH ，DI ，DL， DK > DM， DF， DP， DS， DT， DW， DY， DV ，C A ，CR ，CN > CD CC， CE， CQ， CG， CH， Cl， CL CK CM CF > CP， CS， CT， CW， CY， CV， EA， ER ，EN ，ED ，EC ，EE EQ， EG - EH， El， EL， EK， EM ，EF ，EP ES， ET， EW， EY， EV， QA， QR， QN， QD ，QC ，QE ，QQ QG QH， QI， QL， QK， QM， QF， QP ，QS QT， QW， QY， QV > GA， GR， GN， GD， GC， GE ，GQ ，GG ，GH ，GI， GL， GK， GM， GF， GP， GS， GT ，GW ，GY ，GV ，HA ，HR ，HN ，HD ，HC ，HE -59- (56) 1362934
，HQ，HG，HH，HI，HL，HK，HM，HF，HP，HS，HT ，HW，HY， HV， IA， IR，IN ，ID ，IC ，IE ， IQ ， IG， IH， II，IL， IK， IM， IF，IP ，IS ，IT ，IW ，IY， IV， LA， LR，LN ，LD ，LC ，LE， LQ ’ LG ，LH ，LI， LL， LK， LM，LF ，LP ，LS ，LT， LW， LY， LV， KA， KR， KN， KD，KC ，KE ，KQ ，KG， KH， KI， KL， KK， KM， KF， KP，KS ，KT ，KW ，KY， KV， MA ，MR ，MN ，MD ，MC，ME， MQ， MG， MH，MI，ML， MK， MM， MF，
MP，MS，MT，MW，MY，MV，FA，FR，FN，FD，FC ，FE ， FQ ， FG ， FH ， FI ， FL ， FK ， FM ， FF ， FP ， FS ， FT ， FW ， FY ， FV ， PA ， PR ， PN ， PD ， PC ， PE ， PQ ， PG，PH，PI，PL，PK，PM，PF，PP，PS，PT，PW，PY ，PV，SA，SR，SN，SD，SC，SE，SQ，SG，SH，SI， SL，SK，SM，SF，SP，SS，ST，S W，S Y，S V，T A，T R ，TN，TD，TC，TE，TQ，TG，TH，TI，TL，TK，TM ，TF，TP，TS，TT，TW，TY，TV，WA，WR，WN，WD ，WC，WE，WQ，WG，WH，WI，WL，WK，WM，WF， WP，WS，WT，WW，WY，WV，YA，YR，YN，YD，YC ，YE，YQ，YG，YH，YI，YL，YK，YM，YF，YP，YS ，YT，YW，YY，YV，VA，VR，VN，VD，VC，VE， VQ，VG，VH，VI，VL，VK，VM，VF，VP，VS，VT， VW，VY 及 vv。 三肽殘基亦有用以作爲保護基團。當膦酸酯待保護時 ，序列一 X4 - pro — X5 _ (其中X4爲任何胺基酸殘基且 -60- ⑧ (57) (57)1362934 X5爲胺基酸殘基、羧酯、或氫）乃藉由管腔之羧基酶裂 解而得具游離羧基之X4，其繼而預期可自動化地將胺基 膦酸鍵裂解。X5之羧基團則隨意地以苄基進行酯化。 二肽或三肽類可以已知之運送性質及/或對可影響運 送至腸黏膜或其它細胞型式中之肽酶之易感性爲基礎而選 定。缺乏α _胺基團之二肽及三肽爲供於腸黏膜細胞之刷 狀緣膜中所發現之肽運送體用之運送基質（Bai，J.P.F.， ( 1 992) 9:969-978 )。故有運送能力之肽可用 以增強醯胺化物之生物利用率。具有一或多個D構型胺 基酸之二或三肽亦可與肽之運送體相容，故可用於本發明 之醯胺化物中。D構型之胺基酸可用以降低二或三肽藉由 刷狀緣常見之蛋白酶諸如胺基肽酶N而水解之易感性。 此外，二或三肽另可以其對藉由腸腔中常見之蛋白酶而水 解之個別抗性爲基礎而選定。例如，缺乏asp及/或glu 之三肽或多肽爲不適合供胺基肽酶用之基質，於疏水性胺 基酸（leu、tyr、phe、val、trp)之 N —端側鏈上缺乏胺 基酸殘基之二或三肽爲不適合供肽鏈內切酶用之基質，而 於游離羧基端、於倒數第二位置上缺乏pro殘基之肽則爲 不適合供羧基肽酶P用之基質。類同之考量亦可應用至對 藉由細胞質、腎、肝、血清或其它肽酶所致之水解作用具 相對抗性或相對易感性之肽之選擇上。此不良裂解性之多 肽醯胺化物爲免疫原或有用以結合至蛋白上以製備免疫原 -61 - ⑧ (58) 1362934 本發明之特殊實施例 本文中所述之供基團、取代基及範圍用之特殊數値， 以及本發明之特殊實施例僅供說明之目的；彼等並不排除 其它定義數値或在定義數値範圍內之其它數値。 本發明之一特殊實施例中，A1具有下式：
A3
本發明之另一特殊實施例中，A1具有下式：
本發明之另一特殊實施例中，A1具有下式：
本發明之另一特殊實施例中，A1具有下式： -62- (59) (59)1362934
本發明之另一特殊實施例中，A1具有下式：
且W5a爲碳環或雜環，其中W5a獨立地經0或1個R2基 團取代。Μ 1 2a之特殊數値爲1。 本發明之另一特殊實施例中，A1具有下式：
本發明之另一特殊實施例中，A1具有下式：
本發明之另一特殊實施例中，A1具有下式： -63- ⑧ (60) 1362934
其中w5a爲獨立地經0或1個R2基團取代之碳環； 本發明之另一特殊實施例中，A1具有下式：
2 其中 丫21)爲 〇 或 N(R2):且 M12d 爲 1、2、3、4、5、6 、7 或 8。 本發明之另一特殊實施例中，A1具有下式：
其中W5a爲獨立地經0或1個R2基團取代之碳環； 本發明之另一特殊實施例中，A1具有下式：
其中W5a爲碳環或雜環，其中W5a獨立地經0或1個 R2基團取代。 ⑧ -64- (61) 1362934 本發明之另一特殊實施例中，A1具有下式：
其中 Y2b 爲 〇 或 N(R2):且 M12d 爲 1、2、3、4、5、6 、7 或 8。
本發明之一特殊實施例中，A2具有下式：
本發明之另一特殊實施例中，A2具有下式：
本發明之另一特殊實施例中，M12b爲1。 本發明之另一特殊實施例中，Ml 2b爲0，Y2爲一個 鍵且W5爲碳環或雜環，其中W5乃隨意且獨立地經1、2 或3個R2基團取代。 ⑧ -65- (62) 1362934 本發明之另一特殊實施例中，A2具有下式：
其中W5a爲碳環或雜環，其中W5a乃隨意且獨立地經1、 2或3個R2基團取代。 # 本發明之另一特殊實施例中，M12a爲1。 本發明之另一特殊實施例中，A2擇自苯基、經取代 苯基、苄基、經取代苄基、吡啶基及經取代吡啶基。 本發明之另一特殊實施例中，A2具有下式：
本發明之另一特殊實施例中，A2具有下式：
本發明之另一特殊實施例中，M12b爲1。 -66- ⑧ (63)1362934 本發明之一特殊實施例中，A3具有下式：
本發明之另一特殊實施例中，A3具有下式：
本發明之另一特殊實施例中，A3具有下式：
其中丫13爲0或S;且丫23爲0、N(RX)或S。 本發明之另一特殊實施例中，A3具有下式： ⑧ 1362934
其中且Y2b爲〇或N ( Rx )。 本發明之另一特殊實施例中，A3具有下式：
其中 Y2b 爲 0 或 N(RX):且 M12d 爲 1、2、3、4、5、6 、7 或 8。
本發明之另一特殊實施例中，A3具有下式：
其中 Y2b 爲 〇 或 N(Rx);且 M12d 爲 1、2、3、4、5、6 、7 或 8。 本發明之另一特殊實施例中，M12d爲1。 本發明之另一特殊實施例中，A3具有下式： -68- ⑧ (65)1362934
,RX 本發明之另一特殊實施例中， A3具有下式：
本發明之另一特殊實施例中， 本發明之另一特殊實施例中， W5爲碳環。 A3具有下式：
本發明之另一特殊實施例中， 本發明之另一特殊實施例中， W5爲苯基。 A3具有下式： -69 - ⑧ (66)1362934 γ13
其中丫13爲Ο或S;且丫23爲0、N(RX)或S。 本發明之另一特殊實施例中，A3具有下式：
其中且Y2b爲0或N ( Rx )。
本發明之另一特殊實施例中，A3具有下式：
其中 丫21)爲 0 或 N(RX):且 M12d 爲 1、2' 3、4、5、6 、7 或 8。 本發明之另一特殊實施例中，R1爲H。 本發明之另一特殊實施例中，A3具有下式= -70- ⑧ (67)1362934
其中苯基碳環乃經0、1、2 本發明之另一特殊實施
本發明之另一特殊實 R2 /OR1 或3個R2基團取代。 例中，A3具有下式： •R2 -OR1 例中，A3具有下式：
本發明之另一特殊實 一 OR1 例中，A3具有下式： -71 - ⑧ (68)1362934
OR1
本發明之另一特殊實施例中，A3具有下式：
2 .
本發明之另一特殊實施例中，A3具有下式：
其中Yla爲〇或S;且丫23爲0、N(RX)或S。 本發明之另一特殊實施例中，A3具有下式：
⑧ (69) 1362934 其中爲〇或5;丫21)爲〇或N(R2):且Y2e爲0、N (Ry )或 S。 本發明之另一特殊實施例中，A3具有下式：
其中Yla爲〇或S; 丫25爲0或N(R2) ; 丫2£1爲0或N(
Ry ):且 M12d 爲 1、2、3、4、5、6、7 或 8。 本發明之另一特殊實施例中，A3具有下式：
其中 Y2b 爲 〇 或 N(R2):且 M12d 爲 1、2、3、4、5、6 、7 或 8。 本發明之另一特殊實施例中，A3具有下式：
其中Y2b爲〇或N ( R2 ) -73- 2 1362934 (7 \
中 例
中 M12a
式 下 有 具 3 A
式 下 有 具 3 A 本發明之另一特殊實施例中，A3具有下式 via r2
RV 其中丫13爲Ο或S;且丫23爲0、N(R2)或S 本發明之另一特殊實施例中，A3具有下式
Y
Ry 2c
其中 Ylag 0 或 S; 丫21)爲 0 或 N(R2);且 γκ 爲 Ο、N
(Ry)或 S ⑧ -74- (71)1362934 本發明之另一特殊實施例中，A3具有下式：
其中Yla爲〇或5;丫21)爲0或N(R2) ;丫2(1爲0或N(
Ry ):且 M12d 爲 1、2、3、4、5、6、7 或 8。 本發明之另一特殊實施例中，A3具有下式：
其中 丫21?爲 〇 或 N(R2):且 M12d 爲 1' 2、3、4、5' 6
其中Y2b爲0或N ( R2 )。 本發明之另一特殊實施例中，A3具有下式： -75- (72) 1362934
其中 Y2b 爲 0 或 N(RX):且 M12d 爲 1、2、3、4 、7 或 8。 本發明之另一特殊實施例中，A3具有下式：
OR1 φ 其中苯基碳環乃經〇、1、2或3個R2基團取代。 本發明之另一特殊實施例中，A3具有下式：
其中苯基碳環乃經〇、1、2或3個R2基團取代。 -76- (73)1362934 本發明之另一特殊實施例中，A3具有下式
OR1 Φ 本發明之一特殊實施例中，具有下式： 〇
, II
-^-(CH2)—P—0—R
其中每一個R獨立地爲（C^-Ce)烷基。 R1、W3
本發明之一特殊實施例中，Rx獨立地爲Η、 、保護基團、或下式：
其中：
Ry獨立地爲Η、W3、R2或保護基團； R1獨立地爲Η或具1至18個碳原子之烷基； 乃獨立
R2獨立地爲Η、 R1、R3或R4，其中每一個R -77- ⑧ (74) 1362934 地經〇至3個R3基團取代或者於碳原子處結合，兩個R2 基團形成具3至8個碳之環且環可經0至3個R3基團取 代； 其中R3乃如同本文中所定義。 本發明之一特殊實施例中，Rx具有下式： R2
其中Yla爲〇或S;且Y2e爲〇、N(Ry)或S。 本發明之一特殊實施例中，Rx具有下式： R2 v2d
其中丫13爲Ο或S;且、2<1爲Ο或N(Ry)。 本發明之一特殊實施例中，Rx具有下式： R2
Ο 本發明之一特殊實施例中，1^爲氫或具1至10個碳 -78- (75) 1362934 之烷基。 本發明之一特殊實施例中，Rx具有下式： R2
0
本發明之一特殊實施例中，Rx具有下式：
本發明之一特殊實施例中，Rx具有下式：
本發明之一特殊實施例中，Y1爲◦或S。 本發明之一特殊實施例中，Y2爲〇、N(Ry)或S。 本發明之一特殊實施例中，Rx爲下式之基團： -79- ⑧ (76) 1362934
M1a M1b M12c M1c M1d M1e ; 其中mla、mlb、mlc、mid及mle獨立地爲0或1 ; ml2c 爲 0、1、2、3、4、5、6、7、8、9、10、11或
Ry爲Η、W3、R2或保護基團； 其中W3、R2、Y1及Y2乃如同本文中所定義； 惟： 如果 mla、ml2c 及！nld 爲 0 時，則 mlb、_mlc 及 m 1 e 爲 0 ; 如果mla及ml2c爲0且！nld不爲0時，貝lj mlb及 m 1 c 爲 0 ;
如果mla及mid爲0且ml2c不爲0時，貝[J mlb爲0 且mlc及mle中至少有一者爲0; 如果mla爲0且ml2c及mid不爲0時，貝!J mlb爲0 如果ml2c及mid爲0且mla不爲0時，貝!J mlb、 mlc及mle中至少有二者爲0; 如果ml2c爲0且mla及mid不爲0時，貝U mlb及 mlc中至少有一者爲0;且 如果mid爲0且mla及ml2c不爲0時，貝lj mlc及 mle中至少有一者爲0。 -80- ⑧ (77) 1362934 本發明化合物中，W5碳環及W5雜環可獨立地經〇至 3個R2基團取代。W5可爲含有單-或二環型碳環或雜環之 飽和、不飽和或芳族環。W5可具有3至1〇個環原子例如 3至7個環原子。當含有3個環原子時，W5環爲飽和； 當含有4個環原子時’ W5環爲飽和或單_不飽和，當含 有5個環原子時’W5環爲飽和，或單—或二一不飽和， 且當含有6個環原子時’則爲飽和、單—或二一不飽和、 φ 或爲芳族。 W5雜環可爲具有3至7個環節（2至6個碳原子及1 至3個擇自N、〇、P及S之雜原子）之單環或爲具有7 至10個環節（（4至9個碳原子及1至3個擇自N、〇、 · P及S之雜原子）之二環。W5雜環型單環可具有3至6 . 個環原子（2至5個碳原子及1至2個擇自N、〇及S之 雜原子）：或5或6個環原子（3至5個碳原子及1至2 個擇自N及S之雜原子）。\¥5雜環型二環具有7至10個 # 環原子（6至9個碳原子及1至2個擇自N、0及S之雜 原子）且排列成二環[4,5]、[5,5]、[5,6]或[6,6]系統；或 9至10個環原子（8至9個碳原子及1至2個擇自n及S 之雜原子）且排列成二環[5,6]或[6,6]系統。W5雜環可經 由碳、氮、硫或其它原子藉由安定之共價鍵鍵結至Y2上 〇 w5雜環包括（例如）批11 定基、一氫吼陡基異構體、 哌啶、噠嗪基、嘧啶基、吡嗪基、s 一三嗪基、噁唑基、 咪唑基、噻唑基、異噁唑基、吡唑基、異噻唑基、呋喃基 -81 - ⑧ (78) 1362934 、噻呋喃基、噻吩基、及吡咯基。W5亦包括，但不限定 於諸如：
W5碳環及雜環可獨立地經0至3個如上所定義之R3 基團取代。例如經取代W5碳環包括：
經取代苯基碳環之實例包括： -82- ⑧ (79) (79)1362934
連結基團及連結者 本發明提供軛合物，其包含HIV抑制化合物，此化 合物乃隨意地直接（例如經由一個共價鍵）或經由連結基 團（亦即連結者）連結至一或多個膦酸酯基團上。連結者 之特性並不苛定，惟其不會干擾含化合物之膦酸酯充作醫 療劑之能力。膦酸酯或連結者可於化合物之任何具有合成 力之位置處藉移除化合物之氫或任何部分以提供供膦酸酯 或連結者連接用之開放價而連結至化合物（例如式A化 合物）上。 本發明之一實施例中，連結基團或連結者（其可稱之 爲^L〃 ）可包括本文中所述之所有A^A^A2或W3或 其一部分。 本發明之另一實施例中，連結基團或連結者具有約 20道耳吞至約4 00道耳吞之分子量。 本發明之另一實施例中’連結基團或連結者具有約5 埃至約300埃之長度。 本發明之另一實施例中’連結基團或連結者乃將藥物 -83- ⑧ (80) (80)1362934 及PCrY1)殘基分隔約5埃約2 00埃（內含）之長度。 本發明之另一實施例中，連結基團或連結者爲具有2 至25個碳原子之二價、分支或未分支、飽和或不飽和烴 鏈，其中一或多個（例如1、2' 3或4個）碳原子乃隨意 地經（_〇) —所替代，且其中鏈乃隨意地於碳上經一或 多個（例如1、2、3或4個）擇自（C^-Ce)烷氧基、（ C3 - C6)環烷基、烷醯、（C,— C6)烷醯氧基 、（：C，一 C6)烷氧羰基、（C^—Ce)烷硫基、疊氮基、氰 基、硝基、鹵基、羥基、合氧基（=0)、羧基、芳基、 芳氧基、雜芳基及雜芳氧基之取代基所取代》 本發明之另一實施例中，連結基團或連結者具有式W 一 A，其中 A 爲（C, — C24)烷基、（C2-C24)烯基、（ C2—C24)炔基、（C3— C8)環烷基、（C6— C1())芳基或 其組合，其中 W 爲—N(R) C(=0) —、一 C(=0) NR —、一〇c(=o) —、— c ( = Ο ) Ο —、— Ο —、— S —、 -S ( Ο ) -、- S ( Ο ) 2 —、— N(R) —、- C(=0) 一 、或一直鍵；其中每一個R獨立地爲H或烷 基。 本發明之另一實施例中，連結基團或連結者爲由肽中 所形成之二價基團。 本發明之另一實施例中，連結基團或連結者爲由胺基 酸中所形成之二價基團。 本發明之另一實施例中，連結基團或連結者爲由聚-L~谷胺酸、聚—L_天冬胺酸、聚_L —組織胺酸、聚— -84 - ⑧ (81) 1362934 L —鳥胺酸 '聚—L —絲胺酸、聚一 l —蘇胺酸、聚_L — 酪胺酸、聚一L 一亮胺酸、聚—l 一賴胺酸—L 一苯丙胺酸 、聚—L —賴胺酸或聚一L —賴胺酸—L —酪胺酸中所形成 之二價基團。 本發明之另一實施例中，連結基團或連結者具有式w _ (CH2) n，其中 n 爲一 N(R) C(=0) - ' — C(=〇) NR-、- 〇C ( =0 ) — ' - C ( =〇 ) 〇-、- 〇 -、—s — ' ~S(〇) —、— S(O) 2—、— C ( = O ) —、— N ( R ) 一或一直鍵；其中每一個R獨立地爲H或（C, — C6)烷 基。 本發明之另一實施例中，連結基團或連結者爲甲撐、 乙撐或丙撐。 本發明之另一實施例中，連結基團或連結者乃經由連 結者中之碳原子而接合至膦酸酯基團上。 # 細胞內標的 本發明化合物中經隨意置入之膦酸酯基團可於活體內 、於彼等達到期望之作用位（亦即細胞內側）以後之階段 裂解。於細胞內側之一作用機轉可能需要第一次之裂解（ 例如藉酯酶）以得帶負電之"鎖定〃中間體。故本發明化 合物中之終端酯基團之裂解可得不安定之中間體’其乃釋 出帶負電之t鎖定"中間體。 通過細胞內側後，膦酸酯或前藥化合物之細胞內酵素 裂解或修飾作用可導致經裂解或修飾之化合物藉由"牽制 -85- ⑧ (82) 1362934 ”機轉而產生細胞內累積。經裂解或修飾之化合物可繼而 藉由電荷、極性或其它物理性質之顯著變化（與膦酸酯藥 物進入細胞之速率相比之下，此變化乃降低經裂解或修飾 之化合物退出細胞之速率）而^鎖定〃細胞。可達到療效 之其它機轉亦可行。可利用本發明鱗酸酯前藥化合物進行 酵素活化機轉之酵素包括，但不限定於，醯胺酶、酯酶、 微生物酵素、磷脂酶、膽鹼酯酶及磷酸酶。 經由前述已知，許多不同之藥物可根據本發明而衍出 。許多此類藥物特別於本文中述及。然而，供根據本發明 而衍生之藥物家族及其特殊成員之討論僅只說明，而非涵 蓋全部。 . HIV抑制性化合物 本發明化合物包括彼些具有HIV抑制活性者。本發 明化合物隨意地帶有一或多個（例如1、2、3或4個）膦 % 酸酯基團，其可爲前藥部分。 所謂、HIV抑制性化合物〃包括彼些可抑制HIV之 化合物。 本發明化合物通常具有約400 amu至約10,000 amu 之分子量；本發明之特殊實施例中，化合物具有小於約 5 000 amu之分子量；本發明之另一特殊實施例中，化合 物具有小於約2500 amu之分子量；本發明之另—特殊實 施例中，化合物具有小於約1000 amu之分子量；本發明 之另一特殊實施例中’化合物具有小於約800 amu之分子 ⑧ (83) 1362934 量；本發明之另一特殊實施例中，化合物具有小於約600 amu之分子量；本發明之另一特殊實施例中，化合物具有 小於約600 amu且大於約400 amu之分子量。 本發明化合物通常亦具有小於約5之logD (極性） 。本發明之一實施例中提供I〇gD小於約4之化合物；本 發明之另一實施例中提供logD小於約3之化合物；本發 明之另一實施例中提供logD大於約_5之化合物；本發 φ 明之另一實施例中提供logD大於約-3之化合物；且本 發明之另一實施例中提供logD大於約0且小於約3之化 合物》 在本發明化合物內之擇定取代基係以遞迴程度存在。 * 本文全文中，"遞迴取代基〃意指取代基可列舉其本身之 - 另一種例子。因爲此些取代基之遞迴特性，故理論上可有 許多之取代基存在於既定之實施例中。例如，Rx可含有 Ry取代基。Ry可爲R2，其繼而可爲R3。如果所選擇之 # R3爲R3e，則可選擇第二個例子之Rx。熟知醫藥化學技藝 者已知，此些取代基之總數乃藉由所欲化合物之期望性質 而合理限制。此些性質包括，舉例（但不限定）而言，諸 如分子量、溶解度或log P、應用性質諸如對抗所欲標的 之活性，及實際性質諸如合成容易度等。 舉例（但不限定）而言，W3、Ry及R3在某些實施例 中均爲遞迴取代基。通常每一者在既定之實施例中可獨立 地存在 20、19、18、17、16、15、14、13、12、11、 、9、8、7、6、5、4、3、2、1 或 0 次。尤其，每一者在 -87- ⑧ (84) 1362934 既定之實施例中可獨立地存在I2或更少次。尤其，在既 定之實施例中，W3存在〇至8次’ Ry存在0至6次且R3 存在0至10次。更尤其’在既定之實施例中’ W3存在0 至6次，Ry存在〇至4次且r3存在0至8次。 遞迴取代基爲本發明所欲之觀點。熟知醫藥化學技藝 者已知此些取代基之變通性。有關遞迴取代基於本發明實 施例中存在之程度，總數係依上述決定。 φ 當本文所述化合物經一個以上之相同命名之取代基（ 例如"R1 "或"R0a〃 ）取代時，則此些基團當然可相同 或互異，亦即每一個基團係獨立擇定。波浪線意指接合至 鄰接基團 '部分或原子上之共價鍵位置。 • 本發明之一實施例中，化合物爲分離及純化形式。所 - 謂'"分離及純化〃通常意指化合物實質上不含生物學物料 '(例如血液、組織、細胞等）。本發明之一特殊實施例中 ’此稱謂意指本發明化合物或軛合物至少約50重量％不 • 含生物學物料；另一特殊實施例中，此稱謂意指本發明化 合物或軛合物至少約75重量％不含生物學物料；另一特 殊實施例中’此稱謂意指本發明化合物或軛合物至少約 90重量％不含生物學物料；另—特殊實施例中，此稱謂 意指本發明化合物或軛合物至少約98重量％不含生物學 物料；且另一實施例中，此稱謂意指本發明化合物或軛合 物至少約99重量％不含生物學物料。另一特殊實施例中 ’本發明提供業已合成製備（例如活體外）之本發明化合 物或軛合物。 -88 - ⑧ (85) 1362934 細胞累積 一實施例中，本發明提供可於人類PBMC (周邊血液 單核細胞）中累積之化合物》PBMC意指具有圓形淋巴細 胞及單核細胞之血液細胞。在生理學上，PBMC爲對抗感 染之機轉中之必要組份。PBMC可由正常健康給血者之肝 素化全血或由血塊黃色層中藉標準密度梯度離心法分離、 φ 由分界面採收，清洗（例如磷酸鹽緩衝鹽水）及於冷凍媒 介中貯存。PBMC可於多孔式盤中培養。於各個不同之培 養時間點，將上層液移出以供估測，或者可採收細胞及予 分析(Smith R. etal (2003) Blood 1 02 (7): 2532-2540 )。 * 此實施例之化合物可進一步包含膦酸酯或膦酸酯前藥。尤 - 其，膦酸酯或膦酸酯前藥可具有本文所述之A3結構。 與不具有膦酸酯或膦酸酯前藥之化合物類似物相比之 下，本發明化合物一般證實可改善化合物或化合物細胞內 φ 代謝物於人類PBMC中之細胞內半衰期。半衰期通常可增 加至少約50%，尤其至少50 — 100%，更尤其至少約100 %，甚尤其大於100%。 本發明之一實施例中，與不具有膦酸酯或膦酸酯前藥 之化合物類似物相比之下，化合物代謝物於人類PBMC中 之細胞內半衰期可獲得改善。此實施例中，代謝物可於細 胞內產生，例如在人類PBMC內產生。代謝物可爲膦酸酯 前藥在人類PBMC內之裂解產物。隨意含膦酸酯之膦酸酯 前藥可裂解以形成於生理學pH下具有至少一個負電荷之 -89- ⑧ (86) 1362934
代謝物。膦酸酯前藥可在人類PBMC內酵素裂解以形成P 一 OH形式之具有至少一個活性氫原子之膦酸酯。 立體異構體 本發明具有手性中心，例如手性碳或磷原子。故本發 明化合物包括所有立體異構體包括對映體、非對映異構體 及構形異構體之消旋混合物。此外，本發明化合物包括於 φ 任何或所有不對稱、手性原子處之富集或解析光學異構體 。換言之，由敘述中明顯可知之手性中心係以手性異構體 或消旋混合物之形式提供。消旋及非對映異構體混合物， 以及已分離或合成之個別光學異構體（實質上不含其對映 * 體或非對映異構體夥伴）均在本發明之範圍內。消旋混合 - 物乃經由詳知之技術分離成其個別、實質光學純異構體， 諸如以旋光添加劑例如酸或鹼所形成之非對映異構體鹽分 離，其後反轉換回旋光物質。大部分情況下，期望之光學 • 異構體係使用立體特異反應由期望原物料之適當立體異構 體開始而合成。 某些狀況下，本發明化合物亦可以互變異構體形式存 在。雖然僅有一種非定域化之共振結構可敘述，但所有之 形式均在本發明之範圍內。例如，烯-胺互變異構體可存 在以供嘌呤、嘧啶、咪唑、胍、脒及四唑系統用且所有其 可能之互變異構體形式均在本發明之範圍內。 鹽及水合物 ⑧ (87) (87)1362934 本發明組成物隨意地包含本文化合物之鹽，尤其是含 ’例如，Na+、Li+ ' K+、Ca + 2及Mg + 2之藥學上可接受之 無毒性鹽》此些鹽可包括彼些藉將適當陽離子（諸如鹼及 鹼土金屬離子或銨及四級胺基離子）與酸陰離子部分（通 常爲羧酸）組合所衍出者。如果期望水溶性鹽，則以單價 鹽較理想。 金屬鹽通常係藉令金屬氫氧化物與本發明化合物起反 應而製得。可以此方式製得之金屬鹽之實例爲含有Li+、 Na +及K+之鹽。較不可溶之金屬鹽可藉將適當之金屬化合 物加入以由較可溶之鹽溶液中沉澱出。 此外，鹽可藉將某些有機及無機酸例如氫氯酸、氫溴 酸、硫酸、磷酸或有機磺酸加至鹼性中心（通常爲胺）或 至酸性基團中而形成。最後，本文中之組成物當然包含未 離子化以及偶極離子形式之本發明化合物，以及與化學計 量之水組合成之水合物之形式。 母化合物與一或多個胺基酸形成之鹽亦涵蓋在本發明 之範圍內。上述之任何胺基酸均適當，尤其是經發現作爲 蛋白質組份之天然存在之胺基酸，然而胺基酸通常爲帶有 具鹼性或酸性基團之側鏈者，例如賴胺酸、精胺酸或谷胺 酸，或帶有具中性基團之側鏈者諸如甘胺酸、絲胺酸、蘇 胺酸、丙胺酸、異亮胺酸或亮胺酸。 抑制HIV之方法 本發明之另一觀點係關於抑制HIV活性之方法，其 • 91 - (88) 1362934 包含將懷疑含有HIV之樣品以本發明組成物治療之步驟 〇 本發明組成物可充作HIV抑制劑，充作供此抑制劑 用之中間體或具有如下所述之用途。抑制劑通常結合至肝 表面上或肝腔內的位置上。於肝中結合之組成物可以各種 不同程度之可逆性結合。具實質不可逆性結合力之彼些化 合物爲供本發明法中所用之理想候選者。一旦標記後，具 φ 實質不可逆結合力之組成物乃有用以作爲供檢測HIV之 探子。因此本發明係關於檢測懷疑含有HIV之樣品中之 NS3之方法，其包含以下之步驟：將懷疑含有HIV之樣 品以含有結合至標記上之本發明化合物之組成物處理；再 觀察樣品對標記活性之效應。適當之標記已於診斷領域中 * 詳知且包括安定之游離基團、螢光團、放射性同位素、酵 素' 化學發光基團及色原。本文中之化合物係以慣用之方 式使用官能基團諸如羥基或胺基予以標記。 # 本發明全文中，懷疑含有HIV之樣品包括天然及人 造物料諸如活生物體；組織或細胞培養物；生物學樣品諸 如生物學物料樣品（血液、血清、尿、腦脊髓液、淚液、 痰 '唾液、組織樣品等）；實驗室樣品；食物、水或空氣 樣品；生物產物樣品諸如細胞萃取物，尤其是合成期望糖 蛋白之重組細胞等。樣品通常爲懷疑含有HIV者。樣品 可含於任何介質包括水及有機溶劑/水混合液中。樣品包 括活生物體諸如人類，及人造物料諸如細胞培養物。 本發明之處理步驟包含將本發明組成物加至樣品中或 -92- (99) 1362934 以治療或預防病毒、寄生蟲或細菌感染或相關病況或供治 療腫瘤或相關病況之藥劑包括3'-疊氮基- 3’-去氧胸腺 嚼陡核脊（齊多夫定（zidovudine) 、AZT) ，2’ —去氧 —3’一硫雜胞苷（3TC) ，2’，3’_ 二去氧 _2',3’一 二去氫 腺苷（D4A) ，2’，3·—二去氧—2'，3’—二去氫胸腺嘧啶核
苷（D4T)，亞伯卡韋（carbovir)(環型2'，3’一二去氧 _2’，3'_二去氫鳥苷），3'—疊氮基_2'，3’一二去氧尿苷 ，5_氟基胸腺嘧啶核苷，（E) _5 —（2 —溴乙烯基）_ 2'—去氧尿苔（BVDU) ，2—氯基去氧腺符，2 —去氧助 間型黴素，5 —氟基尿嘧啶，5 —氟基尿苷，5—氟基一 2’ 一去氧尿苷，5 —三氟甲基—21—去氧尿苷，6—氮雜尿苷 ，5—氟基乳清酸，胺甲蝶呤，三乙醯尿苷，1 一（2· —去 氧一2'—氟基一1_/3 —阿拉伯糖苷基）_5—碘基胞苷（ FIAC )，四氫一咪唑並（4,5，Ι — jk) 一（1，4)—苯並二 氮平—2(1H) —硫酮（TIBO) ，2'— 正—環型 GMP，6 -甲氧基嘌呤阿拉伯糖苷（ara_M) ，6 —甲氧基嘌呤阿 拉伯糖苷2’_ 0—戊酸酯、胞嘧啶阿拉伯糖苷（ara — C ) ，2’，3’-二去氧核苷諸如2’，3’-二去氧胞苷（（1(1(：)， 2’，3’一二去氧腺苷（ddA)及2',3’一二去氧肌苷（ddl)， 無環型核苷諸如阿昔洛韋（acyclovir )、平昔洛韋（ penciclovir)、法昔洛韋（famciclovir)、更昔洛韋（ ganciclovir ) 、 HPMPC 、 PMEA 、 PMEG 、 PMPA 、 PMPDAP、FPMPA、HPMPA、HPMPDAP、 ( 2R,5R ) - 9 一四氫一 5 — （膦醯甲氧基）一 2 —呋喃基腺嘌呤、（ -103- ⑧ (100) 1362934 2R，5R) — 1—四氫一 5—（膦醯甲氧基）—2—呋喃基胸腺 嘧啶，其它抗病毒劑包括利巴韋林（ribavirin )(腺嘌呤 阿拉伯糖有^ 、2—硫基一 6—氮雜尿苷、殺結核菌素（
tubercidin)、金精三羧酸、3一去氮新平辛、新平辛（ neoplanocin)、金剛乙胺（rimantidine)、金剛（ adamantine)及膦甲酸三鈉（foscarnet)，抗細菌劑包括 殺細菌性氟咱諾嗣（環丙沙星（ciprofloxacin)、培氟沙 星（pefloxacin )等），胺基糖苷殺細菌性抗生素（鏈黴 素、健他黴素、阿米卡辛等），Θ -內醯胺酶抑制劑（頭 孢靈素、青黴素等），其它抗細菌劑包括四環素、異菸鹼 醯肼（isoniazid)、利福平（rifampin)、頭孢哌酮（ cefoperazone)、克雷索黴素（ciaithromycin)及阿索黴 素（azithromycin )，抗寄生蟲或抗黴菌劑包括戊烷脒（ 1,5-雙（4’-胺基苯氧基）戊烷）、9_去氮肌苷、磺胺 甲卩惡哩（sulfamethoxazole)、擴胺嚼陡（sulfadiazine) 、口奎匹拉明（quinapyramine)、奎寧、氟可那哗（ fluconazole) ' 酮康唑（ketocQnazole)、伊曲康哩（ itraconazole) ' 兩性黴素 B( Amphotericin B) 、5 -氟 基胞嘧啶、克黴唑（clotrimazole )、十六基磷酸膽鹼及 制菌黴素（nystatin )。腎排泄抑制劑諸如丙磺舒（ probenicid)，核苷運送抑制劑諸如雙嘧達莫（ dipyridamole)、克冠二氮平（dilazep)及硝苄硫基肌苷 ，免疫調節劑諸如FK506、環孢靈素A ( cyclosporin A ) 、胸腺肽α -1 (thymosina-1)，細胞激肽包括TNF及 -104- ⑧ (101) 1362934 TGF—召，干擾素包括 IFN— α、IFN— /3 ，及 IFN— 7"， 間白素包括各種不同之間白素，巨噬細胞/顆粒性白血球 集落因子包括GM— CSF、G—CSF、M— CSF，細胞激肽 拮抗劑包括抗一TNF抗體，抗一間白素抗體，可溶性間白 素受體，蛋白激酶C抑制劑等。 此外，表98及99中所揭示之針對HIV之醫療劑可 與本發明化合物組合使用。例如表98揭示例示之HIV/ AIDS療法，表99則揭示例示之HIV抗病毒劑以及其對 應之美國專利號。
Table 98 - Exemplary HIV/AIDS Therapeutics 鲁 ϋ期 _名 通用名 品牌名 醫療群 作用群之機轉 機構 已卜.市-1987 ΑΖΤ BW-A509U CpdS !&棘_顿核苷 齊多夫定 (Zidovudine) AZTEC Retrovir 抗-H1V劑 反轉錄酶抑制劑 GlaxoSmithKline (Originator) 已上市- 1992 NSC- 606170 Ro-24- 2027/000 Ro-242027 二去氣胞苷 扎西他箔 (Zalcitabine) Hrvid 抗-HIV劑 反轉錄酶抑制劑 National Cancer Institute (US) (Originator) Roche ddC ddCyd 已上市- BMY-27857 西尼夫定 Zerit 抗.HIV劑 反轉錄酶抑制劑 Bristol*Myers 1994 (Saniivudine) Squibb (Originator) DTH 司他夫定 化學遞 INSERM (Stavudine) 送系統 (Originator)
d4T -105- ⑧ (102)1362934 B±市- ddeThd BMY-40900 去雛苷 Videx 抗 反特娜 Bristol-Myers 1991 DDI NSC- 612049 (Didanosioe) 二去餓杳 Squibb (Originator) Bristol-Myers Squibb (Orphan Drug) d2l ddlno B±市- rlL-2 Aldesleukin Macrolin tfi-HJVm IL-2 Chiron 1989 rhlL-2 重組間白索-2 Proleukin 乳癌醫療 (Originator) Nat. Inst. Allergy & Infectious Dis.
白血病β療 黑鱗娜療 症候群醜 骨傾性白 療 淋巴瘤B療 腎癌醫療 已上市-1995
已上市· 1989 R-56 沙克那韋甲礎麵 Fortovase 抗-HIV劑 HIV蛋白酶 Chugai (Sa〇uinavir mesilate) 抑制劑 Pharmaceutical (Originator) Ro-31- Invirase Chugai 8959/003 Fortovase Pharmaceutical (Orphan Drug) Roche (soft gel capsules) (Originator) Λ31白血球 Alferon 抗細 Guangdong Tsm-a LDO 倾毒藥 Alferon N 抗-HIV劑 HemispheRx CAi@白血球 衍生¢) Gel Alferon N Injection mm Interferon Sciences 抗 病雜 (Originator) Altemol ⑧ (103)1362934
Cellferon 窃满毒薬 娜純
治療女性 mm 礙
B±市· 1996 BI-RG-587 BIRG-0587 那雜平 (Nevirapine) Viramune 抗-HIV劑 反轉娜 抑刪 Boehringer Ingelheim (Originator) Nippon Boehringer Ingelheim Roxane 已上市-1999 1592U89 sulfate 阿巴卡韋硫酸鹽 (Abacavir sulfate) Ziagen 抗-HIV劑 反mm 抑制劑 GlaxoSmithKline (Originator) GlaxoSmithKline (Orphan Drug) 第Ι/Π期 CD4-lgG CD4·触 AIDS 藥 Genentech (Originator) rCD4-lgG 飾CD4·免 挪蛋白G Nat. Inst. Allergy & Infectious Dis. Μ可溶 14CD4· 免^蛋白G 已上市-1995 (O-BCH-189 (-)-SddC 拉米夫定 (Lamivudine) 3TC Epivir 抗-HIV劑 反轉郷 獅劑 GlaxoSmithKline Shire BioChem (Originator) 3TC Epivir- HBV mmm mm GG-714 Heptodin GR- 109714X Heptovir ⑧ (104)1362934 BCH-790 (fomer code)
Lamivir Zeffix
Zefix
制期 KNI-272 達丁-272 (Kyoostatiih272) NSC- 651714 已上市- (-)-FTC 恩凼他濱 2003 (Erotiicitabme) 524W91 524W91 註冊前 AG-1661 HIV-1 mm RG-83894 抗-HlVffl HIV蛋白酶 mm Japan Energy (Originator) Coviracil 抗-HIV劑 反轉娜 _劑 Emory University (Originator) Emtriva 抗-BMffP炎 mmm Gilead Japan Tobacco Rescri ptor 抗-HIVffl 反mm 獅劑 Agouron Pfizer (Originator) Pfizer (Orphan Drug) Remune AIDS 酿 Immune Response (Originator) Roemmers Trinity Medical Group Crixivan 抗-HTV劑 HIV蛋白酶 Banyu mm Merck & Co. (Originator) 抗-HIV劑 反轉纖 Russian 抑制劑 Academy of Sciences (Originator) 抗-HIV劑 反轉娜 獅劑 Advanced Life Sciences 治離綱 Sarawak MediChem 抗-HIV劑 抗福 Λϋ化單 株抗體病 * 毒入口抑 制劑 US Department of Health & Human Services (Originator) Biogen Idee (Originator) Tanox Agenerase Prozei 抗-HIV劑 H1V蛋白酶 抑制劑 GlaxoSmithKline Kissei * 已上市· 1996 RG-83894· 103 L-735524 MK-639 印娜韋 Qndmavir sulfate) 節期 phAZT emmmm (Azidotbyinidioe (txapboBSe) • 尼可韋 (Nicavir) 第Π期 NSC- 675451 (WBCrr (nto^hstid) 晰麵A ((+>Calanolide A) NSC-664737 (racemate) 卡臟A (Calanolide A) 第Π期 5A8 Hu-5A8 TNX-355 已上市· 1999 141W94 KVX478 練那韋 (Amprenavir) 1362934 (105) VX-478 B±m- 1998 DMP-266 棚韋侖 (Efaviieziz) L-743726 L-743725 ((+)- enantiomer) L-741211 (racemate) B±市-1996 A-84538 ABT-538 和腳韋 (Ritonavir) • 已上市· 1997 AG-1343 LY-312857 财那韋 (Ndfinavir mesilate) AG-1346 (free base) 細I期 PRO-2000 * PRO-2000/5 娜期 Gd-Tex GdT2B2 PCI-0120 釓-德W (Gadolinium tex_yriii) 難沙芬乱 (Motexafin gadolinium)
Vertex (Originator)
Stocrin 抗-HIVffl 反轉娜 Banyu Sustiva Banyu (Orphan Drug) Bristol-Myers Squibb (Originator) Norvir 抗-HIV劑 HIV蛋白 Abbott _制劑 (Originator) Dainippon Pharmaceutical Viracept HIV蛋白 Agouron m^mm (Originator) Japan Tobacco Mitsubishi Pharma Roche 抗-HIV劑 病毒入口 抑制劑 Indevus Medical Research Council Paligent (Originator) Xcytrin 抗-HIV劑 National Cancer Institute Pharmacyclics 強· (Originator) 腦癌《療 mm 質删胞 娜療 之醜 肺癌S療 淋巴球性白 細賊
淋巴瘤醜 -109 - ⑧ (106)1362934 癌醜mmmm mmmm s療 已上市· 2003 DP-178 恩福韋地 (Eniuviitide)
Fuzeon
抗-HIVJW 病挪合 獅劑 R-698 平他福地 (Pentaiuside)
Duke University (Originator) Roche
T-20
Trimeris (Originator)
BC-IL 血塊飽 層間白索
MultiKine AIDS 藥
Cel-Sci (Originator) University of Maryland 子宮頚癌 B療 翻鹏 B療 細期 FP-21399 mmim 醜 抗-HIV劑
mm AXD-455 抗-HIV劑 去氧亥普 齡成_mm EMD Lexigen (Originator) Fuji Photo Film (Originator) Axxima CNM493 絲裂原活 化蛋白激
Cytokine PharmaSciences -氧化箱合 制劑
Picower Institute for Medical Research (Originator) 腎癌s療 -110 ⑧ (107) 1362934
細期 ALA/AC AIDSffiffi ANRS
MN120 TMGMP ALVAC Merck & Co. vCP205 vCP205 Nat. Inst. Allergy & Infectious Dis.
Sanofi Pasteur (Originator) • Virogenetics (Originator) Walter Reed Army Institute • mm CY-2301 EP HIV- 1090 EP-1090 Theradigm- AIDS 疫苗 HIV DNA麟 Epimmune (Originator) IDM Nat. Inst. Allergy & Infectious Dis. Ψ National Institutes of Health 第π期 CD4-lgG2 抗-HIV劑 病毒入口 mm Epicyte • PRO-542 Formatech GTC Biotherapeutics 細 UC-781 抗-HIV劑 反轉娜 Progenies (Originator) Biosyn 殺触酬 Cellegy mm ProVax AIDS^S Uniroyal (Originator) University of Pittsburgh (Originator) Progenies ⑧ (108)1362934 第Π期 ACH- 126443 mam (Elvudtabine) 抗-HIVffl DSAm^m mm Achillion L-D4FC 抗 病雜 反轉娜 mm Vion beta-L-Fd4C Yale University (Originator) mm CV-N 藍藻抗^毒蛋白N (CyanoviriD N) 抗-HIVffl 病毒入a mm Biosyn ms^wm National Cancer Institute (US) (Originator)
已上市· PNU- 提普那韋 Aplivus 2005 140690 (Tipranavir) U-140690 PNU- 140690E (diNa salt) mm ADA 偶氣甲酸胺 (AzodicaitxJD aimide) 抗-HIV劑 NSC- 674447 已上市_ 2001 Bis(POC)PM PA 麟福韋雙異 丙隨氧基甲酯 富馬酸鹽 (Tenofovir disoproxil Vi read AIDS 蕖 GS4331-05 抗-HIV劑 第π期 PA-457 抗-HIV劑 YK-FH312 第Π期 SP-01
Anticort 抗·Ηΐν 劑 HIV蛋白酶
Boehringer Ingelheim
Pfizer (Originator)
National Cancer Institute (US) (Originator) Rega Institute for Medical Research (Originator) 反轉錄酶 Gilead 抑制劑 (Originator)
Japan Tobacco Japan Tobacco (Orphan Drug) 病毒成熟 Biotech 抑制劑 Research Laboratories (Originator) Panacos
University North Carolina, Chapel Hill (Originator)
ViroLogic HMG-CoA Altachem 還原酶 mRNA 表麵制劑
SP-01A 病毒入口 Georgetown 姑制劑 University (Originator)
112- (109)1362934
Samaritan Pharmaceuticals 已上市-2003 BMS-232632- 05 CGP-73547
Reyataz
抗-HIVW HIV蛋白驊
Bristol-Myers Squibb Bristol-Myers Squibb (Orphan Drug)
Novartis (Originator) BMS-232632 (free base) 已上市- AZT/3TC 拉米夫忠齊多夫定 Combivir 抗-HIVSi 1997 (Lamivudine/Zido vudine) 反轉凝I GlaxoSmithKline 抑如劑 (Originator)
齊多夫定啦米夫定
第m 期 AIDSVAX B/B
Genentech (Originator)
AIDSVAX gp120 B/B
Nat. Inst. Allergy & Infectious Dis. VaxGen
節I 期 （-)-BCH-
10652 (-)-dOTC AVX-754 BCH-10618 SPD-754
第Π 期 D-D4FC DPC-817 抗-HIV劑 反轉娜 W劑 Avexa Shire Pharmaceuticals (Originator) Reverset 抗-HIV劑 DNA聚合 酬制劑 反轉娜 mm Bristol-Myers Squibb (Originator) Incyte Pharmasset
RVT 第Ι/Π期 beta-D- D4FC VIR-201 臨歸 DDE-46 WH1-07
細胞凋亡 誘導劑
Virax (Originator) Paradigm Pharmaceuticals Parker Hughes Institute (Originator) ⑧ (110)1362934
半肤胺酸蛋白mmim 半既胺酸蛋白 半纖酸蛋白 贿抑獅 g^glj HI-113 仙肢 (Sanqridinc) STAMP 史酿定 (Stampidine) 反轉餓
Parker Hughes Institute (Originator)
d4T· pBPMAP
臨獅 WH卜05 臨獅 1F7 CTB-1 MAb1F7 δνΗΐνιι 陰道 抗-HIVffl 抗CUfFife 病毒楽
Paradigm Pharmaceuticals Parker Hughes Institute (Originator) ImmPheron
Immune Network InNexus Sidney Kimmel Cancer Center (Originator) University of British Columbia
已申請IND MD1-P 抗·HivSil wmm 獅挪 治療嚢性 雌搬 治療融 性休克 節期 PA-14 抗-HIV劑 抗-CD195 (CCR5) PRO-140 Λϋ化 雜抗體
Dana-Farber Cancer Institute
Medical Discoveries (Originator)
Epicyte
Progenies (Originator) -114 ⑧ (111)1362934 病毒入口
Protein Design Labs
EpiBr HE-2000
Immunitin 抗"HivJH Inactivin 抗 病酿
Colthurst (Originator) Edenland mm
Hollis-Eden (Originator)
軔期 ALVAC VCP1452 治療囊性ismm. 刪 AIDS 雖
ANRS VCP1452
Nat Inst. Allergy & Infectious Dis.
Sanofi Pasteur (Originator) Virogenetics (Originator) mm
(±)-FTC
Racivir 抗·Ηΐν 劑
Pharmasset (Originator)
PSI-5004 抗mm 第π期 mmmm (Cellulose sulfate UsherceU) 女性 醉劑m&wm 病毒入口 Polydex 如滴劑 (Originator) 第撕 SF-2 rgp120 AIDS 脑
Chiron (Originator) rgp120 SF-2
Nat. Inst. Allergy & Infectious Dis. 節期 MIV-150 抗-HIV劑 殺赃刪 反轉娜 圆劑
Medivir (Originator) Population Council ⑧ (112)1362934 娜期 第m 期 10D1 mAb
抗-HIV^ 抗· Amerimmune CD11a/CD18 (LFA-1) (Originator) 鼠 辦 Cytodyn 抗-ΗΐνϊϊΙ 抗 *CD152 BristoHVIyers (CTLA-4) Squibb 乳湖9療’ λΜ m 抗體 Medarex (Originator)
MDX-010 MDX- CTLA4 MDX-101 (formerly) 第mm 期 1018-iss ISS-1018 願部癌 娜療 黒 棚 癌 腎癌轚療 AIDS 藥
Medarex (Orphan Drug) National Cancer Institute 甚核脊酸 Dynavax (Originator)
Gilead
munm HGTV43 飾期 R-147681 (D_viiine) TMC-120 第π期 DPC-083 已上市-2000 拉米夫定/ 齊多夫定 阿巴卡韋 抗-mv劑 丁 riz 丨 vir 抗·ΗΐνΒ!ΐ 過敏性奥 Sanofi Pasteur mm 免獅酬 淋巴瘤B療 mm
Stealth 抗-HIV劑 Enzo (Originator)
Vector 基因統
抗-HIV劑 反轉娜 IPM mmm ms&^m Janssen (Originator)
Tibotec (Originator) 反轉錄酶 Bristol-Myers 剤 Squibb (Originator)
GlaxoSmithKline (Originator) -T16-
(113)1362934
Lexiva 抗-HIVffl HIV蛋白酶 GlaxoSmithKline (FfKamprenavTr calcium) mm (Originator) 已上市- 908 2003
GW- 433908G
Telzir 化學逸 銳統
Vertex (Originator) GW-433908 (mm ) VX-175 mmm 第I期
DNAHIV ADI獅
GlaxoSmithKline 第ID期
PowderJed HIV PowderMed DNA赌 (Originator) PC-515 Carraguard 殺微生物剤 Population Council (Originator) R-165335 伊妥雜 (Etravirine) 抗-HIV劑 反轉娜 mm Janssen (Originator) TMC-125 Tibotec (Originator) SP-1093V 抗-HIV劑 DNA McGill University mm 反mm mm Supratek (Originator) mm 臨獅
Genentech (Originator) VaxGen
AIDSVAX
B/E
AIDSVAX
gp120B/E
Walter Reed Army Institute 已上市· ΑΒΤ-378/Γ 洛匹那韋/利托那韋 Kaletra 抗-HIV剤 mv蛋白酶 Abbott 2000 (Lopinavir/ mm (Originator) ABT- ritonavir) 治療嚴 Gilead 378/利棚韋 mm 症候群 (SARS), 第I期 BCH-13520 抗-HIV劑 反轉獅 Shire 獅劑 Pharmaceuticals (Originator) SPD-756 獅期 BAY-50- 阿達吉白索a： 抗-HIV劑 IL-2 Bayer 4798 (Adargileukin alia) mmwm (Originator) 節期 204937 mm 抗-HIV劑 反轉娜 画劑 GlaxoSmithKline
-117- (114)1362934 MIV-210
Medivir (Originator) 第m 期 BufferGel 第撕 Ad5-FLgag
Ad5-gag mnm alvac
E120TMG 醜 mfm Johns Hopkins University (Originator) National Institutes of Health ReProtect (Originator) AIDS疫苗 Merck & Co. (Originator) DNA贿 AIDS 雖 Nat. Inst. Allergy & infectious Dis.
ALVAC VCP1521
Sanofi Pasteur (Originator) VCP1521
Virogenetics (Originator) 第Π期 MVA-BN Nef MVA-HIV-1 LAI-nef MVA-nef AIDS疫苗
Walter Reed Army Institute Bavarian Nordic (Originator) 茹期 DNA/MVA 多蛋白 SHIV-89.6 DNA/MVA 雌 AIDS疫苗
Emory University (Originator) GeoVax
Nat. Inst. Allergy & Infectious Dis. 第Π 期 ΜνΑΉΐνΑ AIDS 疫苗 Impfstoffwerk
Dessau-Tomau
GmbH (Originator)
International AIDS Vaccine
Initiative
Uganda Virus
Research
Institute
University of
Oxford 第I期 LFn-p24 HIV-Therapore AIDS疫苗
Avant (Originator) Nat. Inst. Allergy & Infectious Dis. -118- ⑧ (115)1362934
Walter Reed Army institute
C31G 格 (Glyminox)
Oramed
Biosyn (Originator)
SAWY
Cellegy 抗徴菌劑m&mm 性感染 餌期 BRI-7013
VivaGel fir道 mm
SPL-7013 SDS SLS 月桂基硫^
Invisible Condom 抗-HIV剤
Biomolecular Research Institute (Originator) Starpharma Universite Laval (Originator) 抗-職獅 病雜mmmm
陰道 第Ι/Π期 2F5 抗-HIV 劑 Λϋ Epicyte
病毒入□ Polymun 獅I劑 (Originator) Universitaet Wien (Originator) AK-671 恩蛮韋洛 抗-HIV劑 化學麵 Schering-Plough (Ancriviroc) CCR5 (Originator) mm SCH- 病毒入口 351125 抑制劑 ⑧ (116)1362934
SCH-C
Schering C
第I期 DNA/PLG m. 第1期 AAV2-gag- PR-DELTA- RT tgAAC-09 tgAAC09 AAV 卸期 AVX-101 AVX-101 VEE 節期 gp160 MN/LAI-2
臨臟 THPB 2·ΟΗ，丙基· β-mmm 0-(2- 麵基> β- 環糊精 Trap) HPB 臨獅 MPI-49839 節期 BMS- 378806 BMS-806 細 T-麵 HIV挪 娜期 TMC-114 UIC-94017 達魯那韋 (Danmavir) AIDS疫苗 Chiron (Originator) DNA賴 Nat. Inst. Allergy & Infectious Dis. AIDS 雖 International AIDS Vaccine Initiative dna Targeted Genetics (Originator) AIDS疫苗 DNA醋 AlphaVax (Originator) Nat. Inst. Allergy & Infectious Dis. AIDS疫苗 ANRS Sanofi Pasteur (Originator) Walter Reed Army Institute 抗-HIV劑 Cyclodextrin Technologies Development (Originator) 抗-HIV劑 Myriad Genetics (Originator) 抗-HIV劑 病毒入口 mm Bristol-Myers Squibb (Originator) AIDS疫苗 抗-HIV劑 HIV蛋白酶 mm Hadassah Medical Organization (Originator) Weizmann Institute of Science Johnson & Johnson Tibotec (Originator) -120- (117) 1362934
University of
Illinois (Originator) MV-026048 抗-HIVffl 反轉挪 mm Medivir (Originator) Roche mm K5-N,OS(H) 抗-HIVffl 血管顿 mm Glycores 2000 • mmm 病翻合 mmm San Raffaele Scientific Institute Universita degli Studi di Bari (Originator) Universita degli Studi di Brescia (Originator) mm UK-427857 (Maraviroc) 抗-HIV劑 化學脈 CCR5 洁剛 病毒入口 mm Pfizer (Originator) 節期 BILR-355 抗-HIV劑 反轉綱 mm Boehringer Ingelheim (Originator) - BILR-355- BS • 已上市-2004 阿巴卡韋硫酸鹽/ 拉米夫定 (Abacavir sulfate/ lamivudine) Epzicom 抗-HIV劑 反轉娜 mm GlaxoSmithKline (Originator) Kivexa • 臨獅 DermaVir AIDS疫苗 Genetic Immunity (Originator) mmm 2G12 DNA酿 抗-HIV劑 Λϋ單 株抗想 Research Institute Genetic Human Ther. Epicyte 病毒入口 mm Polymun (Originator) Universitaet Wien (Originator) 繊 L- 000870810 抗-HIV劑 HIV整雜 _剤 Merck & Co. (Originator) L-870810 ⑧ -121 - (118)1362934 第]期 L-870812 抗-Hivffl HIVM合SI Merck & Co. 抑軸^ (Originator) 第1 期 VRX496
SAMMA 第I 期 Ad5gag2 MRKAd5
MRKAd5gag 抗-HIV® University of Pennsylvania 反義轚療 VIRxSYS (Originator) 獅 病毒入口 Mount Sinai mm School of Medicine (Originator) Rush University Medical Center (Originator) AIDS疫苗 Merck & Co. (Originator) Nat. Inst. Allergy & Infectious Dis. Sanofi Pasteur mm BG-777
抗-HIV劑
Virocell (Originator) IS感
臨臟 mm Panjab (Sulphonated University Hespeiidio) (Originator) 抗-HIV劑 第Π 期 695634 GW-5634 $娜 m
GlaxoSmithKline (Originator) GW-695634 第Π 期 GW-678248 GW-8248 臨床前 R-1495 抗-HIV^ 反轉錄藤 GlaxoSmithKline 劑 (Originator) 抗-Hiv劑 反轉細 Medivir 抑制劑 -122- ⑧ (119)1362934 mm SMP-717 細期 AMDO70 臨床前 TGF-alpha
Roche 抗 抗-HIVSi 反轉娜 mm Advanced Life Sciences (Originator) m-mm CXCR4 (SDF-1) 病毒入口 mm AnorMED (Originator) Nat. Inst. Allergy & Infectious Dis. 抗-HIVSI National Institutes of Health Centocor Kaleidos Pharma
National Cancer
Institute (US) (Originator)
National
Institutes of
Health (Originator) 第Π期 873140 抗-HIV劑化學激肚 GlaxoSmithKline CCR5 拮謂 AK-602 病毒入口 Ono (Originator) 抑制剤 GW-873140 ONO-4128 第I 期 TAK-220
抗-HIV劑化學激肚 Takeda CCR5 (Originator) mtm 病毒入口 獅剤 已上市 AIDS疫苗 Immunitor (V«l Immunitor) 治療AIDMI 關麵症 (Originator) 卸期 TAK-652 抗-HIV劑 itmsk Takeda CCR5 捨酬 (Originator) 病毒入口 _劑 已申請IND R15K BlockAide/ 抗-HIV劑 病毒入口 Adventrx CR mm Pharmaceuticals -123- ⑧ (120)1362934 第Π期 R-278474 里普韋林 (Rilpivirise) TMC-278 反轉餓 M.D. Anderson Cancer Center (Originator) Janssen (Originator) KPC-2 INK-20 mm CCR5 mAb
CCR5mAb00 4 MIV-170 第I期 DP6*001 HIV DNA m 第Π 期 AG-001859
AG-1859mum 臨臟 抗-HIVJS Kucera Pharmaceutical (Originator) 抗·Ηΐν劑 化學遞 縣統 Kucera Pharmaceutical (Originator) 抗-HIV剤 抗-CD195 (CCR5) Human Genome Sciences (Originator) λΜ wm 抗體 病毎入口 抗-HIV剤 反mm 抑制劑 Medivir (Originator) AIDS 麵 Advanced BioScience DNA贿 CytRx 抗-HIV劑 H1V蛋白酶 抑制劑 University of Massachusetts (Originator) Pfizer (Originator) GTU- MuttiHIV AIDS疫苗 FIT Biotech (Originator) EradicAide DNA贿 AIDS疫苗 International AIDS Vaccine Initiative Adventrx Pharmaceuticals M.D. Anderson G3nce「Center (Originator) 已上市-2004 醯氣基甲酯富馬 麵恩曲他演 (Tenofovir disoproxil fumaratt/ontricit abine)
Truvada 抗-HIV劑 反轉 _ Gilead 獅!ί 劑 (Originator) Japan Tobacco ⑧ (121)1362934
TPFA
BlockAide/V 病毒入口 Adventrx P 抑獅 Pharmaceuticals (Originator) Thiovir 抗-HIVffl 反轉娜 mm Adventrx Pharmaceuticals 子宮頸癌醜
National Cancer Institute
University of Southern California (Originator)
期 MetX Metabol’rteX 抗
Tripep (Originator)
alpha-HGA 臨獅 NV-05A 抗-HIV劑 反轉鱗 Idenix mm (Originator) 第 Ι/Π 期 IR-103 AIDS疫苗
Immune Response 臨床前 MX-100 抗-HIV劑 HIV蛋白酶 Pharmacor 抑制劑 (Originator) PL-100
Procyon Biopharma (Originator) 第I期
節期 SCH-D
Sch-417690
ViroLogic 抗-HIV劑 Fresenius (Originator) 基因S療 Georg-Speyer- Haus (Originator) 抗-HIV劑 化學職 Schering-Plough CCR5 mm 病毒入口 wmm (Originator) 臨獅
ImmunoVex- AIDS 疫苗 HIV
BioVex (Originator) mm cYT-99-007 rhlL-7 抗-HIV劑
Cytheris (Originator) Nat. Inst. Allergy & Infectious Dis. National Cancer Institute 節期 EMo- AIDS疫苗 Chiron gp140/MF59 (Originator) ⑧ (122) 1362934
Nat. Inst. Allergy & Infectious Dis. 第π期 BMS- 488043 KP-1212 SN-1212 mrmm 抗·HIVJB 病毒入口 mm Bristol-Myers Squibb (Originator) Koronis (Originator) AMD-887 抗-Hivm 化mm： CCR5 mm AnorMED (Originator) 病毒入口 mm 第I期 KP-1461 抗-HIViH Koronis (Originator) • SN-1461 化學 雌 系統 臨獅 臨獅 APP-069 DES-10 抗-HIV剤 抗疱疹 病翻 抗-HIV劑 AusAm Biotechnologies (Originator) National Institutes of Health Aphios (Originator) 臨獅 PC-815 MIV- 150/角叉菜膠 抗-HIV劑 Medivir (Originator) 臨獅 FGI-345 MIV-150/PC- 515 抗-HIV劑 Population Council (Originator) Functional Genetics (Originator) • 臨獅 RPI-MN 抗-HIV劑 Nutra Pharma (Originator) ReceptoPharm (Originator) 臨獅 替諾福韋雙異丙酸氧 基甲酯富馬酸鹽/恩 曲他濱/依發韋侖 (Tenofovir dispproxiJ iiimarate/emtricit abine/efaviicnz) 抗-HIV劑 反mm mmm Bristol-Myers Squibb (Originator) Gilead (Originator) Merck & Co. (Originator) 臨床前 MVA-BN HIV AIDS 鋪 Bavarian Nordic (Originator) mmu MVA-BN HIV AIDS 雖 Bavarian Nordic (Originator) -126- ⑧ (123)1362934 mm PBS-119 節I期 HINM Tat 類雜脑 激劑 Phoenix
Biosciences (Originator) AIDS 疫Neovacs
Tat mm m 第ΠΙ期 TNP 胸膝核蛋白 VGV-1 第I 期 VCR_ADV- 014
Sanofi Pasteur Univ. Maryland Biotechnology Institute Viral Genetics AIDS 雌 GenVec (Originator) Nat. Inst. Allergy & Infectious Dis. 抗·Ηΐν劑 治觸 Georgetown University (Originator) Samaritan Pharmaceuticals 抗·Ηΐν劑 HIV整合酶 w劑 Gilead AIDS 雌 癌mm Japan Tobacco (Originator) Argos Therapeutics (Originator) VRC- HIVADV014-
00-VP 臨床前 SP-010 SP-10 獅期 GS-9137 JTK-303 第Ι/Π期 RNA-負雛 讎
腎癌發療 節期 IFN-a 細胞激肽蛋 白複合物 (IFN-aljiia kinoid)
Antiferon AIDS 賴 系統性紅 斑性獅 用劑
Neovacs (Originator) Sanofi Pasteur 第Π期
DNA.HIVA HIVA AIDS疫苗 DNA酿
International AIDS Vaccine Initiative ML Laboratories (Originator) Uganda Virus Research Institute University of Oxford -127- ⑧ (124)1362934 mm DEBIO-025 抗-HIV剤
Debiophamn (Originator) UNIL-025 病翻 性中風 mm HIV赌 AIDS疫苗
Bema Biotech (Originator)
MV-HIV 825780 C-1605 DNA脑mmm AIDS 藥
GlaxoSmithKline (Originator) Merck & Co. (Originator)
ADMVA AIDS疫苗
Aaron Diamond AIDS Research Center BL-1050 AIDS m
Impfstoffwerk Dessau-丁ornau GmbH (Originator) International AIDS Vaccine Initiative BioLineRx
Hebrew University (Originator) Yissum
CAP 病毒入口 抑制劑
New York Blood Center 陰道 臨麵 QR-437 抗-HIV劑
Quigley Pharma (Originator) MRKAd5 HIV-1 gag/pol/nef AIDS 贿
Merck & Co. (Originator) -128- ⑧ (125)1362934
MRKAd5 mm HIV-1 trivalent MRKAd5gag/ pol/nef 臨獅 臨獅 PL-337 第1期 DNA-C
Nat. Inst. Allergy & Infectious Dis.
CarryVac- H!V AIDS疫苗 Tripep (Originator) Vaccine Research Institute of San Diego HIV-RAS AIDS 藥 Tripep (Originator) 抗-HIV劑 AIDS疫苗 HIV蛋白酶 mm Procyon Biopharma (Originator) EuroVacc Foundation
DNA-HIV-C 第Π期 Lipo-5
節期 Lipo-6T 第撕 EnvPro 第撕 TCB-M358 第撕 TBC-M335 第1 期 TBC-F357
Universitaet
Regensburg (Originator)
AIDS 雌 ANRS
INSERM (Originator)
Nat. Inst. Allergy & Infectious Dis.
Sanofi Pasteur (Originator)
AIDS 麵 ANRS
INSERM (Originator)
Sanofi Pasteur (Originator) AIDS 疫苗 St. Jude
Children's Res.
Hosp. (Originator) AIDS 疫苗 Nat. Inst. Allergy & Infectious Dis.
Therion (Originator) AIDS 疫苗 Nat. Inst. Allergy & Infectious Dis.
Therion (Originator) AIDS 疫苗 Nat. Inst. Allergy & Infectious Dis. •129 ⑧ (126)1362934
Therion (Originator) 第I期 TBC-F349 AIDS 酿
Nat. Inst. Allergy & Infectious Dis. 第1期 TBC- M358/TBC- M355 AIDS 脑
Therion (Originator) Nat. Inst. Allergy & Infectious Dis.
Therion (Originator) Nat. Inst. Allergy & Infectious Dis. 節期 TBC- AIDS疫苗 F357/TBC-F349
第I期
HIV CTL MEP AIDS疫苗
Therion (Originator) Nat. Inst. Allergy & Infectious Dis. 第I 期 VRC-DNA- 009 VRC· HIVDNA009- 00-VP .臨床前 REP-9
Wyeth Pharmaceuticals (Originator) AIDS 疫苗 National Institutes of Health (Originator) DNA赖 抗-HIV劑雜苷酸 REPLICor (Originator)
贿毒藥 臨床前 PPL-100 抗-HIV劑 HIV蛋白酶 Procyon 抑制劑 Biopharma (Originator)
系統 獅期 BI-201 抗·Ηΐν剤
Biolnvent (Originator) -130- ⑧ (127) 1362934 表99 -例示之HIV抗病毒劑及專利號碼
Ziagen (阿巴辛韋硫酸鹽（Abacavir sulfate)，美國 專利 5,034,394 號）
Epzicom (阿巴节韋硫酸鹽（Abacavir sulfate) / 拉 米夫定（Lamivudine)，美國專利5,034,394號） — Hepsera (阿德福韋雙異戊醯氧甲酯（Adefovir dipivoxil)，美國專利 4,724,233 號）
Agenerase (安普那韋（Amprenavir)，美國專利 5,646，180 號）
Reyataz (阿托那韋硫酸鹽（Atazanavir sulfate)， 美國專利5,849,9 1 1號）
Rescriptor (地拉韋陡甲擴酸鹽·（ Delaviridine • mesilate )，美國專利 5,563,142 號）
Hivid (二去氧胞苷；扎西他濱（Zalcitabine )，美 國專利5,028,595號） • Videx (二去氧肌苷；去羥肌苷（Didanosine )，美 國專利4,89 1,759號）
Sustiva (依發韋侖 （Efavirenz )，美國專利 5,519,021 號）
Emtriva (恩曲他濱（Emtricitabine)，美國專利 6,642,245 號）
Lexiva (福善那韋銘（Fosamprenavir calcium)，美 國專利6,636,989號）
Virudin ; Triapten ; Foscavir (膦甲酸三鈉（ -131 - ⑧ (128) 1362934 foscarnet sodium)，美國專利 6,476,009 號）
Crixivan (印地那韋硫酸鹽（indinavir sulfate)，美 國專利5,4 13,999號）
Epivir (拉米夫定 （Lamivudine)，美國專利 5,047,407 號）
Combi vir (拉米夫定（Lamivudine )/齊多夫定（ Zidovudine)，美國專利 4,724,232 號）
Aluviran (洛匹那韋（Lopinavir))
Kaletra (洛匹那韋 （Lopinavir) /利托那韋 ( Ritonavir)，美國專利 5,541,206 號）
Viracept (尼非那韋甲擴酸鹽（Nelfinavir mesilate) ，美國專利5,484,926號）
Viramune (那韋拉平 （Nevirapine)，美國專利 5,366,972 號）
Norvir (利托那韋 （Ritonavir)，美國專利 5,541,206 號）
Invirase ; Fortovase (沙克那韋甲擴酸鹽 （ Saquinavir mesilate)，美國專利 5，196,438 號）
Zerit (司他夫定（Stavudine)，美國專利 4,978,655 號）
Truvada (替諾福韋雙異丙醯氧基甲酯富馬酸鹽（ Tenofovirdisoproxilfumarate) / 恩曲他濱（ Emtricitabine )，美國專利 5,210,085 號）
Aptivus (替普那韋(Tipranavir)) -132- ⑧ (129) 1362934
Retrovir (齊多夫定 （Zidovudine)，美國專利 4,724,232 號） 本發明化合物之代謝物 本文所述化合物之活體代謝產物亦落在本發明之範圍 內。此些產物可能（例如）由所投服化合物之氧化、還原 、水解、醯胺化、酯化等主要由於酵素化過程所致之作用 φ 而產生。因此，本發明包括藉由含令本發明化合物與哺乳 類接合一段足以產生其代謝產物之時間之過程而產生之化 合物。此些產物之鑑定通常係先製備經放射標記（例如 C 1 4或H3 )之本發明化合物，將其以可檢測之劑量（例如 * 大於約〇·5毫克/公斤）非經腸服予動物諸如鼠、鼷鼠、 * 天竺鼠、猴、或人類’令其有足夠發生代謝的時間（通常 約3 0秒至3 0小時）’再將其轉換產物由尿 '血液或其它 生物學樣品中分離出。既然這些產品已被標記，故可輕易 ® 分離出（另外可藉使用可結合至殘留於代謝物中之表位上 之抗體而予以分離）。代謝物的結構係以慣用之方式例如 以質譜或核磁共振分析法測定。代謝物之分析通常以與熟 知技藝者所詳知之慣用藥物代謝硏究相同之方法進行。這 些轉換產物只要不另於活體內存在，均可有用以供本發明 化合物之醫療投藥方面之診斷分析，即使彼等本身不具有 HIV-抑制活性亦然。 供測定化合物於替代性胃腸分泌物中之安定性之方法 係已知。當於3 7 °C下保溫1小時後，其中小於5 〇莫耳百 ⑧ -133- (130) 1362934 分比之經保護基團於替代性腸液或胃液中去保護，則此化 合物在本文中定義爲於胃腸道中具安定性。化合物僅對胃 腸道具安定性，此並不意味彼等不能於活體內水解。本發 明之膦酸酯前藥通常於消化系統中具安定性，但於消化腔 、肝或其它代謝器官中，或者一般而言於細胞內實質水解 成母藥。
本發明化合物之例示製法 本發明亦關於本發明組成物之製法。組成物係藉有機 合成中任何可應用之技術製得。有許多此些技術已於技藝 中詳知。然而，許多已知之技術詳細說明於Compendium of Organic Synthetic Methods (John Wiley & Sons, New York)，Vol. 1· Ian T. Harrison 及 Shuyen Harrison，1971; Vol· 2., Ian T. H a r r i s ο n 及 S h u y e η H a r r i s ο n，1 9 7 4 ; V o 1. 3， Louis S. Hegedus 及 Leroy Wade, 1 977; Vol. 4，Leroy G. We d e, j r., 1 980; Vol· 5，Leroy G. Wede，Jr.，1 984;及 Vol. 6，Michael B. Smith;以及 March，J.，Advanced Organic Chemistry, Third Edition, (John Wiley & Sons, New York, 1 985)， Comprehensive Organic Synthesis. Selectivity, Strategy & Efficiency in Modern Organic Chemistry. In 9 Volumes, Barry M. Trost， Editor-in-Chief (Pergamon Press, New York，1993 printing )中。 本發明組成物之一些例示製法提供如下。這些方法欲 闡述此些製法之特性而不欲限制可應用方法之範圍。 -134- ⑧ (131) 1362934 通常’反應狀況諸如溫度、反應時間、溶劑、逐步處 理步驟等’爲供進行特定反應之技藝中所常見者。所引用 之參考資料以及其中所引用之資料乃含有此些狀況之詳細 說明。通常溫度爲-100 °C至200 °c，溶劑爲質子惰性或質 子性，且反應時間爲10秒至10天。逐步處理通常包括令 任何未反應之試劑中止反應，其後分界於水/有機層系統 中（萃取），再將含有產物之層分離出。 Φ 氧化及還原反應通常於幾近室溫（約20 °C)下進行 ’然供金屬氫化物還原反應則經常將溫度降至〇。(：至-1 〇 〇 °C，溶劑在供還原反應方面通常爲質子惰性，且供氧化反 應方面可爲質子性或質子惰性。反應時間則予調整以達期 * 望之轉換作用。 * 縮合反應通常於幾近室溫下進行，然而供非均衡化、 動力控制性縮合反應方面，則亦常見減溫（0 °c至-1 00 °c )。溶劑可爲質子性（常見於均衡反應中）或質子惰性（ * 常見於動力控制性反應中）。 標準合成技術諸如共沸移除反應副產物及使用無水反 應狀況（例如惰性氣體環境）爲技藝中所常見且當可應用 時則予應用。 反應圖及實例 這些例示方法之一般觀點乃述於下及於實例中。下列 方法中之每一種產物在用於接續方法之前，乃隨意地予以 分離、離析/或純化。 ⑧ -135- (132) 1362934 通常’反應狀況諸如溫度、反應時間、溶劑、逐步處 理步驟等，爲供進行特定反應之技藝中所常見者。所引用 之參考資料以及其中所引用之資料乃含有此些狀況之詳細 說明。通常溫度爲-100 °C至200。(：，溶劑爲質子惰性或質 子性，且反應時間爲10秒至10天。逐步處理通常包括令 任何未反應之試劑中止反應，其後分界於水/有機層系統 中（萃取），再將含有產物之層分離出。 Φ 氧化及還原反應通常於幾近室溫（約201)下進行 ’然供金屬氫化物還原反應則經常將溫度降至〇 °c至_ i 0 0 °C ’溶劑在供還原反應方面通常爲質子惰性，且供氧化反 應方面可爲質子性或質子惰性。反應時間則予調整以達期 * 望之轉換作用。 - 縮合反應通常於幾近室溫下進行，然而供非均衡化' 動力控制性縮合反應方面，則亦常見減溫（〇 t至_丨00。(3 )°溶劑可爲質子性（常見於均衡反應中）或質子惰性（ Φ 常見於動力控制性反應中）。 標準合成技術諸如共沸移除反應副產物及使用無水反 應狀況（例如惰性氣體環境）爲技藝中所常見且當可應用 時則予應用。 所謂"處理〃，當與化學合成操作連接使用時，則意 指接合、混合 '反應、令其反應、令其接合、及技藝中常 見之顯示可將一或多種化學實體以使其轉換成—或多種其 它化學實體之方式處理之其它說法。此意指，將化合物一 以化合物二處理〃與，令化合物一與化合物二起反應〃、 •136- ⑧ (133) 1362934 "令化合物一與化合物二接合〃以及有機合成技藝中供合 理地顯示可將化合物一以化合物二"處理"、"反應〃、 "令其反應"之其它語句的意思是相同的。例如，處理意 指令有機化學品起反應之合理及常用方式。除非另有指定 ，否則欲有當量濃度（〇.〇1M至10M，通常0.1M至1M) 、溫度（-1〇〇°C 至 250°c ’ 通常-78°C 至 100°c，最好 ot： 至100°C )，反應容器（通常爲玻璃、塑膠、金屬製）、 φ 溶劑、壓力、氣壓（通常以氣體供氧及水不敏感性反應用 或以氮或氬供氧及水敏感性反應用）等。有機合成技藝中 已知之類似反應之知識則用以選擇在既定方法中供〜處理 〃用之狀況及儀器。尤其，熟知有機合成技藝者可以技藝 * 中之知識爲基礎而選擇合理預期能成功地進行所述方法之 • 化學反應用之狀況及儀器* 每一種例示反應圖及實例（其後稱之爲1例示反應圖 〃）之改良均導致特定例示物料之各種不同類似物產生。 Φ 上文所引用之說明適當有機合成方法之引證則可應用至此 些改良中。 每一個例示反應圖中，最好將反應產物彼此分離及/ 或由原物料中分離出。將每一步驟或步驟系列中之期望產 物藉技藝中常見之技術予以分離及/或純化（其後稱爲分 離）達期望之同質程度。此些分離法通常包括多相萃取法 、由溶劑或溶劑混合液中之結晶法、蒸餾法、昇華法或層 析法。層析法可包括任何層析法成員例如：逆相及正相； 篩析；離子交換；高、中及低壓液態層析法及儀器；小規
-137- (134) 1362934 模分析；模擬移動床（SMB)及製備薄層或厚層層析法， 以及小規模薄層及急驟層析法。 其它種類之分離法包括將混合物以選擇以供將期望產 物、未反應原物料及反應副產物等試劑結合或用其它方法 分離之試劑處理。此些試劑包括吸附劑諸如活性碳、分子 篩、離子交換介質等。此外，如爲鹼性物料、則試劑可爲 酸，如爲酸性物料、則試劑可爲鹼，試劑亦可爲結合試劑 φ 諸如抗體、結合蛋白、選擇性螯合劑諸如冠醚，液態/液 態離子萃取試劑（LIX )等。 適當分離法之選擇乃依所涉及物料之特性而定。例如 ’沸點’蒸餾及昇華法中之分子量，層析法中之極性官能 基團存在與否，多相萃取法中酸性及鹼性介質中之物料安 ' 定性等。熟知技藝者將採用最適當之技術以達期望之分離 作用。 單一立體異構體，例如對映體（實質不含其立體異構 ® 體）’可藉將消旋混合物使用諸如形成非對映異構體之方 法、使用旋光解析劑予以解析（Stereochemistry of Carbon Compounds, ( 1962) by E. L. Eliel, McGraw Hill; Lochmuller, C. H., ( 1975) J. Chromatogr. , 1 1 3: (3) 282-3 02 )。本發明手性化合物之消旋混合物可藉適當之方法 予以分離及離析，包括：（1 )以手性化合物形成離子性 、非對映異構體鹽，再藉分步結晶或其它方法予以分離， (2 )以手性衍生性試劑形成非對映異構體化合物，將非 對映異構體分離，再轉換成純立體異構體，及（3)將實 -138- ⑧ (135) 1362934 質純或富集之立體異構體於手性狀況下直接分離。 於方法（1)下’非對映異構體鹽可藉令對映體純質 之手性驗諸如番木繁鹼、奎寧、麻黃素、馬錢子驗、α -甲基—苯基乙胺（安非他命）等與帶有酸性官能基之 不對稱化合物諸如羧酸或磺酸起反應而形成。非對映異構 體鹽可藉分步結晶或離子層析法而誘導分離。供胺基化合 物光學異構體之分離方面，加入手性羧酸或磺酸諸如樟腦 φ 磺酸、酒石酸、扁桃酸或乳酸則可形成非對映異構體鹽。 另外’於方法（2)下，令待解析之基質與手性化合 物之一種對映體起反應以形成非對映異構體配對（Eliel， E.及 Wilen， S. ( 1 994) Stereochemistry of Organic Compounds, John Wiley & Sons, Inc., p.322) ° 非對映異 ’ 構體化合物可藉令不對稱化合物與對映體純質之手性衍生 性試劑諸如薄荷基衍生物起反應，其後將非對映異構體分 離再水解以得游離、對映體富集之咕噸而形成。測定手性 # 純度之方法包括製成消旋化合物之手性酯諸如薄荷酯例如 於鹼之存在下之（一）氯甲酸薄荷酯，或Mosher酯，乙 酸α —甲氧基一α —(三氟甲基）苯酯（Jacob II. ( 1 982) 入Org. Cftem. 47:4 1 65 )，再以NMR光譜分析兩種構形異 構體之存在。構形異構體化合物之安定非對映異構體可遵 循供分離構形異構體萘基—異喹啉之方法（Hoye，T.，W0 96/151 1 1 )藉正相及逆相層析予以分離及離析。方法（3 )係將兩種對映體之消旋混合物藉使用手性固定相進行層 析(Chiral Liquid Chromatography ( 1 989) W. J. Lough, -139 - (136) 1362934
Ed. Chapman 及 Hall, New York; Okamoto, (1 990) J- of 513:375-378)而予以分離。富集或純化對映 體可藉用以區分其它具不對稱碳原子之手性分子之方法諸 如旋光及圓二色譜予以區分。 實例一般類 本發明化合物之一些例示製法乃示於本文中，例如於 φ 實例中。這些方法欲說明此類製法之特性而不欲限製可應 用方法之範圍。某些本發明化合物可用以作爲供製備本發 明其它化合物用之中間體。例如，本發明之各種不同膦酸 酯化合物之交互轉換作用乃述於下。 ， 膦酸酯 R-連結-P(〇) (〇1^)2，11-連結—？（〇)( OR1) ( OH)及R—連結一P ( Ο) (OH)2之交互轉換 下列反應圖32- 38說明一般結構R —連結—P(0) # (OR1) 2之製法，其中各R1基團可相同或互異。接合至 膦酸酯上或至其先質上之R1基團可使用已確立之化學轉 變法而改變。膦酸酯之交互轉換反應乃示於反應圖S32中 。反應圖32中之R基團代表於本發明化合物或於其先質 中之次結構，亦即藥物"骨架"，而取代基連結一 P(0 )(OR1) 2乃接合至其上。在進行膦酸酯交互轉換成用 之合成路徑中，R中之某些官能基團可予以保護。供既定 膦酸酯轉變作用所用之方法乃依取代基R1之特性以及膦 酸酯所接合之基質之特性而定。膦酸酯之製備及水解乃述 -140- (137) 1362934 於 Organic Phosphorus Compounds, G. M. Kosolapoff, L, Maeir, ed s, Wiley, 19 7 6, p. 9ff 中 °
通常，膦酸酯之合成係藉將親核性胺或醇與對應之膦 酸酯親電性先質偶合而達成。例如，將氯膦酸酯加至核苷 之5’一羥基上爲供製備核苷膦酸單酯之已詳知方法。活化 之先質可藉一些已詳知之方法製得。有用以供合成前藥之 氯膦酸醋係由經取代_1，3 -丙二醇中製得（Wissner, et al，（ 1 992) /. Md. Chm. 35:1 650 )。氯膦酸酯係藉將對 應之氯磷雜環戊烷（其係藉令經取代二醇與三氯化磷起反 應而得）予以氧化而得（Anderson, et al, (1984)入Med. Chem.. 49:1 304 )。此外，氯膦酸酯劑可藉將經取代1,3 _ 二醇以磷醯氯處理而得（Patois, et al，（1990)人C/iem. kc. Perhn /, 1 577 )。氯膦酸酯類亦可就地由對 應之環型亞磷酸酯中合成（Silverburg，et al.，（1 996) /eii·，37:77 1 -774 )，後者可由氯磷雜環戊烷 或胺基磷酸酯中間體中製得。由焦磷酸酯或磷酸中所製之 氟磷酸酯中間體亦可充作環型前藥製備中之先質（
Watanabe et al., (19 9 8) Tetrahedron lett., 29:5763-66 )。 本發明之膦酸酯前藥亦可由游離酸中藉Mitsunobu反 應(Mitsunobu, (19 8 1) Synthesis, 1 ; Campbell, ( 1 9 9 2) J. (9rg. C/iem. 57:6331)製得，及由其它酸偶合試劑包括（ 但不限定於）碳化二亞胺（Alexander，et al, (1 994)
Collect. Czech. Chem. C o mmun. 5 9:1 8 5 3; Casara et al, ( 1 9 9 2) Bio or g. Med. Chem. Lett. 2:145; Ohashi et a 1, -141 - ⑧ (138) 1362934 ( 1 988) reiraAe心Ζ^ίί·，29:1 1 89 )及苯並三唑氧基參― (二甲胺基）鳞鹽（Campagne et al (1993) reira/iedron ie".，34:6743 )中製得。 令芳基鹵與亞磷酸酯衍生物接受Ni + 2催化反應可得 含芳基膦酸醋之化合物（Balthazar, et al (1980) J. 0厂客· Ckm. 45:54 25 )。膦酸酯亦可由氯鱗酸酯中、於鈀催化 劑之存在下、使用芳族三氟磺酸酯而製得（Petrakis et al ( 1 987 ) J· A m. C hem. S o c· 10 9:283 1； Lu et al ( 1 987) 726 )。另一方法中，芳基膦酸酯係由芳基磷酸 酯中、於陰離子性重排狀況下製得（Melvin (1981) Tetrahedron Lett.，22:3375; Casteel et al (1991) Synthesis * 69 1) 。1^-烷氧基芳基鹽與環型烷基膦酸酯之鹼金屬衍 ' 生物之反應可提供雜芳基- 2-膦酸酯連結者之一般合成 (Red.more ( 1970)人 Org. C/iem. 35:4114)。上述之這些 方法亦可擴展至其中W5基團爲雜環之化合物上。膦酸酯 # 之環型一1，3_丙基前藥亦由膦二酸類及經取代丙一 1，3 -二醇中、使用偶合劑諸如1，3 _二環己基碳化二亞胺（ DCC )於鹼（例如吡啶）之存在下合成。其它以碳化二亞 胺爲基底之偶合劑像1，3 -二異丙基碳化二亞胺或水溶性 試劑，1_ (3 —二甲胺基丙基）一 3-乙基碳化二亞胺氫 氯酸鹽（EDCI )亦可用以供合成環型膦酸酯前藥。 膦酸二酯S32.1轉換成對應膦酸單酯S32.2(反應圖 32，反應1 )之作用係藉一些方法達成。例如，其中R1 爲芳烷基團諸如苄基之酯 S32.1係如同 /. C/iem. -142- ⑧ (139) 1362934 (1995) 60:2946中所述地與三級有機鹼諸如二氮雜二環辛 烷（DABCO )或奎寧環起反應而轉換成單酯化物S32.2。 此反應係於惰性烴溶劑諸如甲苯或二甲苯中、於約110 °C 下進行。其中R1爲芳基團諸如苯基或烯基團諸如烯丙基 之二酯S32.1係藉將酯S32.1以鹼諸如水性氫氧化鈉之乙 腈液或氫氧化鋰之水性四氫呋喃液處理而完成。其中一個 R1基團爲芳烷基團諸如苄基且另一個爲烷基之膦酸二酯 φ S32.1係藉氫化作用，例如使用鈀/碳催化劑予以氫化而 轉換成其中R1爲烷基之單酯S32.2。其中兩個R1基團均 爲烯基諸如烯丙基之膦酸二酯係藉以氯參（三苯膦）铑（ 威金森氏試劑）於水性乙醇中、於迴流下、隨意地於二氮 ， 雜二環辛烷之存在下處理，例如藉使用人01. C/iem. - (1 973) 38:3224中所述供裂解羧酸烯丙酯所用之步驟而轉 換成其中R1爲烯基之單酯S32.2。 膦酸二酯S32.1或膦酸單酯S32.2轉換成對應膦酸 • S3 2.3 (反應圖32，反應2及3)之作用可如同/.C/iem.
Soc.，C/iem. Comm.，（1979) 739中所述地藉令二醋或單醋 與三甲基甲矽烷基溴起反應而完成。此反應係於惰性溶劑 諸如二氯甲烷中、隨意地於甲矽烷基化劑諸如雙（三甲基 甲矽烷基）三氟乙醯胺之存在下、於室溫下進行。其中 R1爲芳烷基團諸如苄基之膦酸單酯S 32.2係藉於鈀催化劑 上氫化，或藉以氯化氫於醚性溶劑諸如二噁烷中處理而轉 換成對應之膦酸S32.3。其中R1爲烯基諸如烯丙基之膦酸 單酯S32.2係藉與威金森氏試劑於水性有機溶劑諸如15 -143- (140) 1362934 %水性乙腈中或於水性乙醇中起反應，例如使用βΗν· Cfm. Acra. ( 1 985) 68:6 1 8中所述之步驟而轉換成膦酸 S32.3。其中R1爲苄基之膦酸酯S32.1之鈀催化性氫解作 用乃述於C/iem. ( 1 959) 24:434中。其中R1爲苯 基之膦酸酯S32.1之鈀催化性氫解作用則述於/· Am. C hem. S o c. ( 19 5 6) 78:23 3 6 中。 膦酸單酯S32.2轉換成膦酸二酯S32.1(其中新置入 φ 之R1基團爲烷基、芳烷基、鹵烷基諸如氯乙基、或芳烷 基）之方法可藉由一些反應達成，此些反應係令基質 S32.2與羥基化合物RhH於偶合劑之存在下起反應。第 二種膦酸酯基團通常異於首先置入之膦酸酯基團，亦即 ‘ R1其後置入R2，其中每一個R1及R2爲烷基、芳烷基' - 鹵烷基諸如氯乙基 '或芳烷基（反應圖32，反應4a)， 因而S.32.2轉換成S32.1a »適當之偶合劑爲彼些用以供製 備羧酸酯者，且包括碳化二亞胺諸如二環己基碳化二亞胺 % ，此事例中之反應最好於鹼性有機溶劑諸如吡啶中進行； 或（苯並三唑一 1 -基氧基）三吡咯啶鳞六氟磷酸鹽（ PYBOP，Sigma )，此事例中之反應係於極性溶劑諸如二 甲基甲醯胺中、於三級有機鹼諸如二異丙基乙胺中進行； 或 Aldrithiol-2 ( Aldrich )，此事例中之反應係於鹼性溶 劑諸如吡啶、於三芳基膦諸如三苯膦之存在下進行。另外 ’膦酸單酯S32.2轉換成二酯S32.1之方法可藉使用上述 之Mitsunobu反應達成。令基質與羥基化合物R1 〇H於偶 氮二羧酸二乙酯及三芳基膦諸如三苯膦之存在下起反應。 ⑧ -144- (141) (141)1362934 另外，膦酸單酯S32.2可藉與鹵化物R^r (其中R1基 團爲烯基或芳烷基）起反應而轉變成其中所置入之R1基 團爲烯基或芳烷基之膦酸二酯S 3 2.1。烷基化反應乃於極 性有機溶劑諸如二甲基甲醯胺或乙中、於鹼諸如碳酸铯之 存在下進行。另外，膦酸單酯可以二階段之步驟轉變成膦 酸二酯。第一階段係將滕酸單酯S3 2.2藉與亞硫醯氯或草 釀氣等依 Organic Phosphorus Compounds, G. Μ. Kosolapoff，L. Maeir，eds，Wiley, 1 976, p. 17 中所述之法 起反應而轉變成氯基類似物RP(〇) (OR1) Cl，再令所 得RP ( Ο ) ( OR1 ) Cl與羥基化合物Ι^〇Η於鹼諸如三乙 胺之存在下起反應，即得膦酸二酯S32.1。 膦酸R —連結_Ρ(0) (OH) 2係藉由上述供製備膦 酸二酯R —連結—P(〇) (OR1) 2 S32.1之方法轉換成膦 酸單酯RP ( 0 ) ( OR1 ) ( OH )(反應圖32，反應5 )， 惟僅使用一莫耳部分之化合物ί^ΟΗ或Rjr。膦酸二烷酯 可根據 Quast et al (19 7 4) Synthesis 490; Stowell et a 1 (1 990) Leii. 326 1;美國專利 5663 1 59 之方法 製得。 膦酸R —連結- P(O) (〇H)2S32.3係藉與羥基化 合物RiOH於偶合劑諸如 AIdrithiol-2( Aldrich)及三苯 膦之存在下進偶合反應而轉變成隣酸二酯R-連結-P(〇 )(OR1 ) 2 S32.1。此反應乃於鹼性溶劑諸如吼啶中進行 。另外，膦酸S32.3可藉使用（例如）二環己基碳化二亞 胺、於吡啶中、於約70 °C下進行偶合反應而轉變成其中 ⑧ -145- (142) 1362934 R1爲芳基之膦酸酯S32.1。另外，膦酸S32.3可藉烷基化 反應而轉變成其中R1爲烯基之膦酸酯S32.1。膦酸係與烯 基溴Rjr於極性有機溶劑諸如乙腈溶液中、於迴流溫度 下、於鹼諸如碳酸絶之存在下起反應以得膦酸酯S32.1。 反應圖3 2 〇 R-link—p-OR1 0R S32.1 0 R-link一Pn-〇R1 OH S32.2 R-link- -OR1 OR1 S32.1 R-link—Pv-〇R1 〇H S32.2 0 R-link一Pn-〇R1 OH S32.2 R-link—Px-〇R1 OH S32.2 4a
0 R-link—Pn-〇H 0H S32.3
0 R-link—Ps-〇H 〇H S32.3 0 R-link—P-OR' OR1 S32.1
O R-link—~~OR’ OR2 S32.1a
O R-link—f^-〇H OH S32.3
O
R-link —F^-~OR 〇H S32.2
R-link——F^-〇H OH S32.3 O R-link一Px-OR1 OR1 S32.1 膦酸酯胺基甲酸酯之製備 膦酸酯可有胺基甲酸酯鍵。胺基甲酸酯之製備乃述於
Comprehensive Organic Functional Group ⑧ -146- (143) 1362934
Transformations, A. R. Katritzky, ed., Pergamon, 1995, Vo 1. 6，p. 4 1 6ff 及於 Organic Functional Group Preparations, by S. R. Sandler 及 W. Karo, Academic Press, 1986, p_ 260ff中。胺基甲醯基團可根據技藝中已 知之方法，包括 Ellis, US 2002/ 0103378 A1 及 Hajima, US 60 18 04 9之教示藉由羥基團之反應形成。 反應圖33說明合成胺基甲酸酯鍵之各種方法。如同 φ 反應圖33所示，在產製胺基甲酸酯之一般反應中，醇 S33.1乃如同本文所述地轉換成其中Lv爲離基團諸如鹵 基、咪唑基、苯並三唑基等之活化衍生物S33.2。而後令 活化衍生物S33.2與胺S33.3起反應以得胺基甲酸酯產物 * · S33.4。反應圖33中之實例1—7說明完成一般反應之方 -. 法。實例8· 10則說明供製備胺基甲酸酯之其它方法。 反應圖33實例1說明使用醇S33.5之氯甲醯衍生物 以製備胺基甲酸酯之方法。此步驟中，令醇S33.5與光氣 # 於惰性溶劑諸如甲苯中、於約〇°C下起反應（如同Org. Syn. Coll. Vol. 3，167, 1965中所述），或令醇與一當量 之試劑諸如氯甲酸三氯甲氧酯起反應（如同 Org. Syn. Coll. Vol. 6, 715，1988中所述）以得氯甲酸酯S33.6。而 後令後者與胺組份S33.3於有機或無機鹼之存在下起反應 以得胺基甲酸酯S33.7。例如，令氯甲醯化合物S33.6與 胺S 3 3.3於水可相混性溶劑諸如四氫呋喃中、於水性氫氧 化鈉之存在下起反應（如同Org. Syn. Coll. Vol. 3，167, 1965中所述）以得胺基甲酸酯S33.7。另外，反應可於二 -147- (144) 1362934 氯甲烷中、於有機鹼諸如二異丙基乙胺或二甲胺基吡啶之 存在下進行。 反應圖33實例2說明氯甲酸酯化合物S33.6與咪唑 反應以得咪唑化物 S33.8。而後令咪唑化物產物與胺 S33.3起反應以得胺基甲酸酯S33.7。咪唑化物之製備係 於質子惰性溶劑諸如二氯甲烷中、於0°C下進行，而胺基 甲酸酯之製備係於類似溶劑中於室溫下、隨意地於鹼諸如 φ 二甲胺基吡啶之存在下進行（如同人Md. C/zem·，1 989, 32, 3 57中所述）。 反應圖33實例3說明氯甲酸酯S3 3.6與活化羥基化 合物R”OH反應以得混合之碳酸酯S33.10。此反應係於有 * 機溶劑諸如乙醚或二氯甲烷中、於鹼諸如二環己胺或三乙 - 胺之存在下進行。羥基化合物R"〇H擇自反應圖33中所 示之化合物群S33.19- S33.24，及類似化合物中。例如， 如果化合物R"〇H爲羥基苯並三唑S33.19，N —羥基琥珀 • 醯亞胺S33.20，或五氯酚S33.21，則混合碳酸酯S33.10 係藉令氯甲酸酯與羥基化合物於醚性溶劑中、於二環己胺 之存在下起反應而得（如同Can. /· C/iew.，1 982，60，976 中所述）。其中組份R"〇H爲五氟酚S33.22或2 -羥基吡 啶S33.23之類似反應係於醚性溶劑中、於三乙胺之存在 下進行（如同 *S;yw·，1986，303 及 C/iem. fier. 118，468, 1985中所述）。 反應圖33實例4說明使用烷氧羰基咪唑S33.8以製 備胺基甲酸酯。此步驟中，乃令醇S33.5與等莫耳量之羰 -148- (145) 1362934 基二咪唑S33.ll起反應以製得中間體S33.8。此反應係於 質子惰性溶劑諸如二氯甲烷或四氫呋喃中進行。而後令醯 氧基咪唑S33.8與等莫耳量之胺ΙΙ·ΝΗ2起反應以得胺基甲 酸酯S33.7。此反應乃於質子惰性溶劑諸如二氯甲烷中進 行（如同L"i·，42，200 1, 5227中所述）以得胺基甲 酸酯S33.7。 反應圖33實例5說明藉由中間體烷氧羰基苯並三唑 φ S33.13以製備胺基甲酸酯。此步驟中，乃令醇R0H於室 溫下與等莫耳量之苯並三唑羰基氯S 3 3.12起反應，以得 烷氧羰基產物S33.13。此反應係於有機溶劑諸如苯或甲苯 中、於三級有機胺諸如三乙胺之存在下進行（如同於 • 1 977，704中所述）。而後令產物與胺R’NH2 » .起反應以得胺基甲酸酯S33.7。此反應乃於甲苯或乙醇中 、於室溫至約80°C下進行（如同於1977, 704 中所述）。 # 反應圖33實例6說明胺基甲酸酯之製備，其中碳酸 酯（R”0) 2CO，S33.14，乃與醇S33.5起反應以得中間體 烷氧碳基中間體S33.15。而後令後者與胺R’NH2起反應 以得胺基甲酸酯S33.7。其中試劑S33.15由N-羥基琥珀 醯亞胺S33.20中所衍出之步驟乃述於7Vi. LeH., 1 992, 2781中；其中試劑S33.1S由2-羥基吡啶S33.23中所衍出 之步驟乃述於Ζ^ίί·，1991，425 1中；其中試劑S33.15 由4-硝基酚S33.24中所衍出之步驟乃述於 1993，103中。等莫耳量醇ROH與碳酸酯S33.14間之反 ⑧ •149- (146) (146)1362934 應係於惰性有機溶劑中、於室溫下進行。 反應圖33實例7說明由烷氧羰基疊氮S33.16中製備 胺基甲酸酯。此步驟中，乃令氯甲酸烷酯S33.6與疊氮化 物例如疊氮化鈉起反應以得烷氧羰基疊氮S33.16。而後令 後者與等莫耳量之胺反應以得胺基甲酸酯S33.7 。此反應乃於室溫下，於極性質子惰性溶劑諸如二甲亞碾 中進行（例如述於1982, 404中）。 反應圖33實例8說明藉由醇ROH與胺之氯甲醯衍生 物S33.17間之反應以製備胺基甲酸酯。此步驟中，乃如 同於 Synthetic Organic Chemistry, R. B. Wagner, H. D. Zook, Wiley, 1 953，ρ· 647中所述，令反應物於室溫下、 於質子惰性溶劑諸如乙腈中、於鹼諸如三乙胺之存在下結 合，以得胺基甲酸酯S33.7。 反應圖33實例9說明藉由醇ROH與異氰酸酯S33.18 間之反應以製備胺基甲酸酯。此步驟中，乃如同於 Synthetic Organic Chemistry, R. B. Wagner, H. D. Zook, Wiley, 1953, p. 645中所述，令反應物於室溫下、於質子 惰性溶劑諸如乙醚或二氯甲烷等溶劑中結合，以得胺基甲 酸酯S33.7。 反應圖33實例10說明藉由醇R〇h與胺R'NH2間之 反應以製備胺基甲酸酯。此步驟中，乃如同於Ckm. ieii. 197 2，37 3中所述’令反應物於室溫下、於質子惰性 溶劑諸如四氫呋喃中、於三級鹼諸如三乙胺，及硒之存在 下結合，以得胺基甲酸酯S33.7。 -150- (147) 1362934 反應圖33.胺基甲酸酯之製備 一般反應
ROH-ROCOLv R，2· » ROCONHR S33.1 S33.2 S33.3 S33.4 實例 (1) ROH--► S33.5 R'NH2 S33.3 ROCOCI ->- ROCONHR' S33.6 S33.7
(2) ROH- -卜 ROCOCI S33.5 S33.6
H
FT
O S33.8 R'NH2 S33.3 ROCONHR' 卜 S33.7 R"OH R’NH2 (3) ROH-ROCOCI -^ ROCOOR^- S33.5 S33.6 S33.9 S33.10 S33.3 ROCONHR' S33.7 (4) ROH S33.5
(5) ROH S33.5
O CN S33.11 -►
S33.12 o 呂R yN^N O S33.8 R'NH2 S33.3 -^ ROCONHR' S33.7
r.nh2 S33·3 - ROCONHR， S33.7 -151 - (6) (148) 1362934 ROH S33.5 (R"〇2)C=0 S33.14 ROCOR" R’Nh + ROCONHR1 S33.15 S33.3 S33.7 (7) R〇H -► ROCOCI -ROCON3 533.5 S33.6 S33.16 R'NH2 33.3 ROCONHR' -► 33.7 (8) R〇H R'NHCOCI ROCONHR· -^ 533.5 S33·17 S33.7
(9) ROH· S33.5 R'NCO S33^8 ROCONHR， S33.7 r_nh2 (10) ROH-^ ROCONHR丨 S33.5 S33.3 S33.7 0 OH R"0H = [I \ N-OH Cl、 Λ .Cl OH cK 、CI 0 T Cl S33.19 S33.20 S33.21
S33.22 S33.23 S33.24 經-烷酯基取代之雙胺基膦酸酯、單胺基膦酸酯、膦酸二 酯及膦酸單酯之製備 有一些方法可用以將膦酸轉換成胺基膦酸酯及膦酸酯 類。一群方法中，包括將膦酸轉換成分離之活化中間體諸 -152- (149) 1362934 如磷醯氯，亦或將膦酸就地活化以供與胺或羥基化合物起 反應。
膦酸轉換成磷醯氯之方法係藉與亞硫醯氯反應（例如 女卩同於 J Gen. Chem. USSR, 1983， 53， 480， Zh. Obschei Khim.，1958，28， 1063 或 J. Org. Chem. 1994，59，6144 中 所述）或與草醯氯反應（如同於Am. Chm. Soc.，1994, 116， 325 1 或 J. Org. Chem. 1994， 59， 6144 中所述)，或 藉與五氯化磷反應（如同於人Org. C/iem. 2001，66，329 或於人Md. Chm·, 1995，38，1372中所述）而達成。而 後令所得磷醯氯與胺或羥基化合物於鹼之存在下起反應以 得醯胺化物或酯產物。 將膦酸藉與羰基二咪唑起反應而轉換成活化咪唑基衍 生物（如同於·/· C/iem. Soc., CAem. Comm. (1991) 312 或
Nucleosides & Nucleotides (2000) 19: 1885 中戶斤述）。活 化之磺醯氧基衍生物係藉令滕酸與三氯甲基磺醯氯或與三 異丙基苯磺醯氯起反應而得（如同於7W. (1996) 7857 或 Bioorg. Med. Chem. Lett (1998) 8:663 中戶斤述)〇 而後令活化之磺醯氧基衍生物與胺或羥基化合物起反應以 得醯胺化物或酯。 另外，可令膦酸及胺或羥基反應物於二亞醯胺偶合劑 之存在下結合。藉於二環己基碳化二亞胺之存在下進行偶 合反應以製備膦酸醯胺化物及酯之方法乃述於（例如） J C hem. Soc., Chem. Comm. (19 91) 312 或 Coll. Czech.
Chem. Comm. (1987) 52:2792中。供活化之乙基二甲胺基 -153- (150) 1362934 丙基碳化二亞胺之使用及膦酸之偶合乃述於7Ή. Len. (200 1 ) 42:884 1 ^ Nucleosides & Nucleotides (2000) 19: 1 885 中。
有一些其它之偶合試劑業已說明供由膦酸中製備醯胺 化物及酯類。此些製劑包括Aid ri thiol-2 (Aldrich)，及 PYBOP 及 BOP(如同於人 Org. Chem. 1995，60, 5214 及 J. Med. C/iem. (1997) 40:3842 中所述），釆一2 —磺醯一3 -硝基 一 1，2,4 —三唑（MSNT )(如同於 J. Med. Chem. (1996) 39:4958中所述），二苯基磷醯疊氮（（如同於人 Med. C/iem. (1 984) 49:1 158 中所述），1- (2,4,6-三異 丙基苯擴酿—3 —硝基一 1，2,4 一三哩（TPSNT)(如同於 Bio or g. Med. Chem. Lett ( 1 998) 8:1013 中戶斤述）， '漠基參 (二甲胺基）鱗六氟磷酸鹽（BroP )(如同於Tet. Lett. (1996) 37:3997 中所述），2 -氯基 一 5，5 -二甲基-2—合 氧基—1，3,2 —二氧雜滕院（如同於 Nucleosides 19 95，14，871中所述），及氯磷酸二苯酯（ 如同於·/ Med· C/iem. ( 1 988) 3 1，1 305 中所述）。 膦酸可藉由Mit sun obu反應而轉換成醯胺化物及酯類 ，其中膦酸與胺或羥基反應物係於三芳基膦及偶氮二羧酸 二烷酯之存在下結合。其步驟乃述於Org . Leif., 2 00 1, 3, 643 或 J. Med. Chem., 1 997, 40, 3842 φ 。 膦酸酯亦可藉令膦酸與鹵基化合物於適當鹼之存在下 起反應而得。此方法乃述於（例如）Αηαί. C/iem. 1 9 87, 59， 1056 或 《/. C/zew. iSoc. Perhn /, 1993， 19, •154- ⑧ (151) 1362934 2303 或 Med. Chem, 1995， 38， 1 372 ^ Tet Lett., 2002, 43, 1161 中。 反應圖34-37說明將膦酸酯及膦酸轉換成經烷酯基取 代之雙胺基膦酸酯（反應圖34)，胺基膦酸酯（反應圖 35)，膦酸單酯（反應圖36)及滕酸單酯（反應圖37) 。反應圖38說明偕-二烷基胺基膦酸酯試劑之合成。 反應圖34說明將膦酸二酯S34.1轉換成雙胺基膦酸 φ 酯S34.5之方法。二酯S34.1(依前述之法製備）乃水解 成單酯S34.2或膦酸S34.6。供這些轉變作用所用之方法 乃述於上。單酯S34.2乃藉與胺基酯S34.9起反應而轉換 成單胺基膦酸酯S34.3，其中S34.9中之R2基團爲Η或烷 ‘ 基；R4b基團爲二價烷撐部分諸如CHCH3、CHCH2CH3、 . CH ( CH ( CH3 ) 2 ) ，CH(CH2Ph)等，或天然或改良胺 基酸中所存在之側鏈基團；且R5b基團爲C, 一 C12烷基諸 如甲基、乙基、丙基、異丙基或異丁基；C6— C2〇芳基諸 # 如苯基或經取代苯基；或C6 - C2c芳烷基諸如苄基或二苯 甲基。反應物係於偶合劑諸如碳化二亞胺例如二環己基碳 化二亞胺之存在下（如同於Am. C/iem. Soc., ( 1 957) 79:3575中所述），隨意地於活化劑諸如羥基苯並三唑之 存在下結合以得胺基膦酸酯產物S34.3。形成胺基膦酸酯 之反應係於偶合劑諸如 B0P(如同於 /_ Org. ( 1 995) 60:52 1 4 中所述）、Aldrithiol、PYBOP 及供製備 醯胺及酯類所用之類同偶合劑之存在下完成。另外，反應 物S34.2及S34.9可藉由Mitsunobu反應而轉變成單胺基 -155- (152) 1362934 勝酸酯S34.3。藉由Mitsunobu反應以製備成胺基膦酸酯 之方法乃述於入Afed. Chm，（ 1 995) 38:2742中。其係令 等莫耳量之反應物於惰性溶劑諸如四氫呋喃中、於三芳基 膦及偶氮二羧酸二烷酯之存在下結合。繼而令所得單胺基 膦酸酯S34.3轉變成單胺基膦酸S34.4。供水解反應所用 之狀況乃依R1基團之特性而定（如前所述）。而後令單 胺基膦酸S34.4與胺基酯S34.9起反應（如上所述）以得 φ 雙胺基膦酸酯S34.5，其中之胺基取代基乃相同或互異。 另外，膦酸S34.6可同時以兩種不同之胺基酯試劑（亦即 S3 4.9，且其中R1、R4b或R5b不相同）處理❶所得之雙胺 基膦酸酯產物S34.5混合物可繼而（例如）藉層析法予以 ， 分離。 ⑧
-156- (153)1362934 反應圖34 R-link· Ο -P-OR1 OR1 S34.1
Ο R-link—&- OR1· OH S34.2 R-link—F^-OH -OH S34.6 S34.9
34J
S34.S R-link- O II -F^—OR Lv S34.8
O
-- R-link—f3-OR1 R2NH(R4b)C02R5b /N-R2 S34.9 (A CO,R5b
S34.3 O R-link—Pn-〇H N-R2(R,( 5b C02R5b S34.4 0 R2 R-link—P-N. -h 1 (R4b)-C02R5b (Lv or OH) S34.11 〇 OR2 R-link—Px-Lv -- R-link—P-Nv 4b/C02RSb (Lv or OH) S34.9 N (R ) -- S34.7 (R4b) 'R S34.9 C02R5b S34.5 O R-link—PN—NH NH N(R4b)c〇2R5b (R，' 5b C02R5b S34.5 O R-link—f^-NH2 NH2 S34.10
Hal(R4b)C02R5b S34.12 ->r Ex6
此步驟之實例乃示於反應圖34、實例1中。此步驟 係令膦酸二苄酯S34.14與二氮雜二環辛烷（DABCO)於 甲苯中、於迴流下起反應（如同於〇l. Chm，1 995, 60，2946中所述）以得膦酸單苄酯S34. IS。而後令產物與 等莫耳量之丙胺酸乙酯S34.16及二環己基碳化二亞胺於 吡啶中起反應以得單胺基膦酸酯S34.17。繼而（例如）藉 於鈀催化劑上氫解以將苄基團移除而得單酸產物S34.18， 其根據 J. Med. Chem，（1997) 40 (23) :3842 可能不安定。 -157- (154) 1362934 胺酸乙 如同於 胺基膦 代亮胺 之產物 轉換成 行，此 :或以 可不同 步驟係 S34.21 C hem. 胺基甲 取代苯 衍生物 丙基苯 之反應 如同於 而後令此化合物S34.18於Mitsunobu反應中與亮 酯S34.19、三苯膦及偶氮二羧酸二乙酯起反應（ /. C/iewz·，1995，38，2742 中所述），即得雙 酸酯產物S34.20。 使用上示步驟，但使用不同之胺基酯S34.9取 酸乙酯S34.19或丙胺酸乙酯S34.16，即得相對應 S34.5 ° 另外，藉使用上述之偶合反應可將膦酸S34.6 雙胺基甲酸酯S34.5。此反應可以一階段之方式進 事例中之產物中所存在之氮一相關性取代基係相同 二階段之方式進行，此事例中之氮-相關性取代基 方法之實例乃示於反應圖34、實例2中。此 令膦酸S34.6於吡啶溶液中與過量之苯丙胺酸乙酯 及二環己基碳化二亞胺起反應（例如如同於·/. So c., C hem. Comm. , 1991，1063 中所述），即得雙 酸酯產物S34.22。 使用上述之步驟，但使用不同之胺基酯S3 4.9 丙胺酸乙酯，即得相對應之產物S34.5。 另一方法係將膦酸S34.6轉換成單或雙一活化 S34.7，其中Lv爲離基團諸如氯基、咪唑基、三異 磺醯氧基等。膦酸轉換成氯化物S34.7(Lv = Cl) 係藉與亞硫醯氯或草醯氯等起反應而達成（
Organic Phosphorus Compounds, G. M. Ko solapof f, L. (155) 1362934
Maeir，eds, Wiley, 1976, ρ· 17中所述）。膦酸轉換成單 咪唑化物（Lv=咪唑基）之反應乃述於·/_ Med. C/iem· 2 0 0 2, 45, 1 284 及於 J. C hem. S oc., C he m. Comm. , 1991, 312中。另外，膦酸乃藉與三異丙基苯磺醯氯起反應而活 化（如同於 2000, 10，1885 中 所述）。而後令活化產物與胺基酯S34.9於鹼之存在下起 反應以得雙胺基膦酸酯S34.5。此反應可以一階段之方式 φ 進行，此事例中之產物中所存在之氮取代基係相同；或以 二階段之方式進行（經由中間體S34.ll )，此事例中之氮 取代基可不同。 方法之實例乃示於反應圖34、實例3及5中。反應 * 圖34、實例3之步驟係令膦酸S34.6與十莫耳當量之亞硫 - 醯氯起反應（如同於 Z/i. Ohc/iei 1 95 8, 28，1063 中所述）以得二氯基化合物S34.23。而後令產物於迴流溫 度下、於極性質子惰性溶劑諸如乙腈中、及於鹼諸如三乙 # 胺之存在下、與絲胺酸丁酯S34.24起反應，即得雙胺基 膦酸酯產物S34.25。 使用上示之步驟，但使用不同之胺基酯S34.9取代絲 胺酸丁酯S34.24，即得相對應之產物S34.S。 反應圖34 '實例5之步驟係令膦酸S34.6如同入 Chem. Soc., Chm· Cowm.，1991，312 中戶斤述地與幾基二咪 唑起反應以得咪唑化物S34.S32。而後令此產物於乙腈溶 液中於室溫下、與一莫耳當量之丙胺酸乙酯S34.33起反 應以得單置換產物S34.S34。繼而令後者與羰基二咪唑起 ⑧ -159- (156) 1362934 反應以得活化之中間體S34.35，再將產物於相同狀況 N-甲基丙胺酸乙酯S34.3 3a起反應，即得雙胺基膦酸 物 S34.36 ° 使用上示之步驟，但使用不同之胺基酯S34.9取 胺酸乙酯S34.33或N-甲基丙胺酸乙酯S34.3 3a，即 對應之產物S34.5。 中間體單胺基膦酸酯S34.3亦可由單酯S34.2中 φ 令單酯與活化之衍生物S34.8 (其中Lv爲離基團諸 基、咪唑基等）使用上述之步驟起反應而得。而後令 S34.8與胺基酯S34.9於鹼諸如吡啶之存在下起反應 中間體單胺基膦酸酯S34.3。再將後者藉移除Ri基團 _ 產物與胺基酯S 34.9偶合（如上述）而轉換成雙胺基 - 酯產物S 3 4.5。 此步驟之實例（其中膦酸乃藉轉換成氯基衍 S34.26而活化）乃示於反應圖34、步驟4中。此步 # 令膦酸單苄酯S34.15於二氯甲烷中與亞硫醯氯起反 如同於7Ή. Leneri·，1994，35, 4097中所述）以得磷 S34.26。而後令此產物於乙腈溶液中、於室溫下、與 耳當量之3 -胺基-2 -甲基丙酸乙酯S34.27起反應以得 基膦酸酯產物S34.28。再將後者於乙酸乙酯中 '於 鈀/碳催化劑上氫化以得單酸產物S34.29。繼而令產 等莫耳當量之丙胺酸丁酯S 34.30、三苯膦、偶氮二羯 乙酯及三乙胺於四氫呋喃中進行Mitsunobu偶合反應 得雙胺基膦酸酯產物S34.31。 下與 酯產 代丙 得相 藉先 如鹵 產物 以得 並令 膦酸 生物 驟乃 應（ 醯氯 -莫 單胺 5 % 物以 酸二 ，即 -160- (157) 1362934 使用上示之步驟，但使用不同之胺基酯S34.9取代3 —胺基一2-甲基丙酸乙酯S34.27或丙胺酸丁酯S34.30, 即得相對應之產物S34.5。 活化之膦酸衍生物S34.7亦可經由二胺基化合物 S34.10而轉換成雙胺基膦酸酯產物S34.5。活化之膦酸衍 生物諸如磷醯氯類藉與氨反應而轉換成相對應胺基類似物 S34.10 之作用乃述於 Organic Phosphorus Compounds，G. _ M. Kosolapoff，L, Maeir，eds，Wiley, 1976 中。而後令雙 胺基化合物S34· 10於增溫下與鹵基酯S34.12 ( Hal =鹵 素，亦即F、Cl ' Br、I )於極性有機溶劑諸如二甲基甲 醯胺中、於鹼諸如4,4 一二甲胺基吡啶（DMAP )或碳酸 _ 鉀之存在下起反應以得雙胺基膦酸酯產物S34.5。另外， - S34.6可同時以兩種不同之胺基酯試劑（亦即S34.12，且 其中R4b或R5b不相同）處理。所得之雙胺基膦酸酯產物 S34.5混合物可繼而（例如）藉層析法予以分離。 # 此步驟之實例乃示於反應圖34、實例6中。其方法 係令二氯膦酸酯S34.23與氨起反應以得二醯胺S34.37。 反應係於水性、水性醇性或醇性溶液中、於迴流溫度下進 行。而後令所得二胺基化合物與二莫耳當量2-溴基-3-甲 基丁酸乙酯S34.38、於極性有機溶劑諸如N-甲基吡咯啶 酮中、於約150°C下、於鹼諸如碳酸鉀之存在下，及隨意 地於催化量之碘化鉀之存在下起反應，即得雙胺基膦酸酯 產物 S34.39。 使用上示之步驟，但使用不同之鹵基酯S34.12取代 ⑧ -161 - (158) 1362934 2 -溴基-3-甲基丁酸乙酯S34.38’即得相對應之產物S34.S 〇 反應圖34中所示之步驟亦可應用至雙胺基膦酸酯之 製備上（其中胺基酯部分乃置入不同之官能基團中）。反 應圖34、實例7說明由酪胺酸中所衍出之雙胺基膦酸酯 之製備。此步驟係令單咪唑化物S34.32與酪胺酸丙酯 S34.40起反應（如同實例5中所述）以得單胺基膦酸酯 • S34.41 〇令產物與羰基二咪唑起反應以得咪唑化物S34.42 ，再令此物料與另莫耳當量之酪胺酸丙酯起反應，即得雙 胺基膦酸酯產物S34.43。 使用上示之步驟，但使用不同之胺基酯S34.9取代酪 • 胺酸丙酯S34.40，即得相對應之產物S34.5。上示步驟中 - 兩個時期所用之胺基酯可相同或互異，故可製得具有相同 或互異取代基之雙胺基膦酸酯。 反應圖35說明單胺基膦酸酯之製法。 • 一步驟係將膦酸單酯S34.1如同反應圖34所示地轉 換成活化衍生物S34.8。而後令此化合物如上所述地與胺 基酯S34.9於鹼之存在下起反應，即得單胺基膦酸酯產物 S35.1° 步驟乃示於反應圖35、步驟1中。此方法係令膦酸 單苯酯S35.7與（例如）亞硫醯氯起反應（如同於人 Gen. Chem. USSR., 1983，32，367 中所述），以得氯基產 物S35.8。而後令產物如同反應圖34所述地與丙胺酸乙酯 S3起反應，即得胺基膦酸酯S35.10。 -162- ⑧ (159) 1362934 使用上示之步驟，但使用不同之胺基酯S34.9取代丙 胺酸乙酯S35.9，即得相對應之產物S35.1。 另外，將膦酸單酯S34.1如同反應圖34所述地與胺 基酯S34.9偶合以得胺基膦酸酯S35.1。如有需要，R1取 代基乃繼而藉初始裂解作用而改變以得膦酸S35.2。供此 轉變作用用之步驟乃依R1基團之特性而定，且如上所述 。而後將隣酸藉與羥基化合物R3〇H起反應（其中R3基 φ 團爲芳基、雜環、烷基、環烷基'幽烷基等）使用與反應 圖34中供將胺及膦酸偶合所用之相同偶合步驟（碳化二 亞胺、Aldrithiol-2' PYBOP、Mitsunobu 反應等）起反應 而轉變成胺基膦酸酯產物S35.3。 反應圖3 4實例1
0 R-link—fi-OBn OBn S34.14 0 R-link—《-OH OBn S34.15 H2NCH(Me)C02Et S34.16 - R-link —P、 OBn COOEt S34.17 R-link-|-^Me H2NCH(CH2Pr；)C02Et 0H COOEt S34.19 S34.18 R-link-
〇 H
Me P^C—(
NH COOEt COOEt S34.20 反應圖34實例2
Bn H2NCH(Bn)C02Et S34.21 -► Ο Relink—{^-〇H OH S34.6 0 )—COOEt
R-link—Pn-NH NH
Bn—( COOEt S34.22 -163- ⑧ (160)1362934 反應圖3 4實例3 0 R-link—fi-OH OH S34.6 R*Iink —P_Cl 〇 H2NCH(CH20H)C02Bu " S34.24
Cl S34.23 R-link-
OH 〇 CO〇Bu li t -P-NH NH HO C02Bu S34.25 反應圖34實例4 Ο R-link—ρχ-ΟΒη-OH S34.15 R-link· 0 H2NCH2CH(Me)C02Et 〇 ii S34.27 n -(3-OBn -^ R-link ——p—OBn
Cl S34.26
NH -C02Et
Me S34.28 R-link-
-OH NH
Me H2NCH(Me)C02Bu 〇 C02Bu 2 v y ^ 2 R-link —P-NH -C02Et S34.30
NH
Me S34.29 -C02Et S34.31 反應圖34實例5 〇 R-link—ρχ-ΟΗ OH S34.6 R-link-
Me O H2NCH(Me)C02Et 〇 )r-Q〇2^ -P-OH -R-link—P-NH S34.33 S34.32 OH S34.34 R-link-
Me 〇 \C〇2 Et it MeNHCH(Me)C02Et -P-NH --->： R-link
Me lm S34.35 S34.33a
Me- \ N- C( S34. 164- (161) 1362934 反應圖3 4實例6 R-link -Ρ\ — Cl Cl S34.23 〇 BrCH(P0C02Et R-link—p-NH2 -► R-link NH2 S34.38 S34.37 〇 ^C02Et
P、一NH
NH S34.39 C02Et 反應圖3 4實例7
此方法之實例乃示於反應圖35、實例2及3中。實 例2所示之順序中，膦酸單苄酯S35.11係藉使用上述之 一種方法與丙胺酸乙酯起反應而轉變成單胺基膦酸酯 S35.12。而後藉於乙酸乙酯溶液中、於5%鈀/碳催化劑 上進行催化性氫化以將苄基團移除而得胺基膦酸S35.13。 繼而令產物於二氯甲烷溶液中、於室溫下與等莫耳量之1 一（二甲胺基丙基）一 3 —乙基碳化二亞胺及三氟乙醇 -165- (162) 1362934 S35.14 起反應（例如如同於 7>i. ie".，2001，42，884 1 中 所述），即得胺基膦酸酯S35.15。 反應圖35'實例3中所示之順序中，單胺基膦酸 S35.13係於四氫呋喃溶液中 '於室溫下與等莫耳量之二環 己基碳化二亞胺及4 一羥基-N—甲基哌啶S35.16偶合， 即得胺基膦酸酯產物S35.17。 使用上示之步驟，但使用不同之單酸S35.2取代丙@ ^ 酸乙酯產物S35.12及使用不同之經基化合物r3〇h取代 三氟乙醇S35.14或4 -經基-N-甲基哌啶S35.16，即得相對 應之產物S35.3 ^ 另外’令活化之膦酸醋S34.8與氨起反應以得胺基膦 ' 酸酯S35.4。而後令產物如同反應圖34所述地與_基醋 - S35.5於鹼之存在下起反應以得胺基膦酸酯產物S3S.6。 如果適當則使用上述之步驟將R1基團的特性改變以得產 物S35.3。方法乃示於反應圖35、實例4中。此順序係令 •I 單苯基憐釀氯S35.18如反應圖34所述地與氨起反應以得 胺基產物S35.19。繼而將此物料於N -甲基吡咯啶酮溶液 中、於170°C下、與2 -溴基—3 —苯基丙酸丁酯S35.2〇 起反應，即得胺基膦酸酯產物S35.21。 使用這些步驟，但使用不同之鹵基酯S35.5取代丙胺 酸乙酯產物S35.12及使用不同之羥基化合物r3〇h取代2 —漠基一3 -苯基丙酸丁醋S35.20，即得相對應之產物 S35.6 ° 單胺基膦酸酯產物S35.3亦可由經雙重活化之膦酸酯 -166- (163) (163)
1362934 衍生物 S34.7中製得。此步驟之實例乃述於 1998，1，73中，令中間體S34.7與限量之胺基酯 反應以得單置換產物S34.ll。而後令後者與羥 R3OH於極性質子惰性溶劑諸如二甲基甲醯胺中 如二異丙基乙胺之存在下起反應，即得單胺基膦 S35.3 ° 方法乃示於反應圖35、實例5中。此方法 二氯S35.22於二氯甲烷溶液中、與一莫耳當量 基酪胺酸乙酯S35.23及二甲胺基吡啶起反應以 膦酸酯S35.24。而後令產物與酚S35.25於含碳 甲基甲醯胺中起反應，即得胺基膦酸酯產物S35. 使用這些步驟，但使用胺基酯S34.9及/或 物R3OH取代丙胺酸乙酯產物S35.12及使用不 化合物 R3〇H取代N —甲基酪胺酸乙酯 S35 S35·25 ，即得相對應之產物S35.3 。
Synlert.， S34.9 起 基化合物 、於驗諸 酸酯產物 係令磷醯 之N-甲 得單胺基 酸鉀之二 26 ° 羥基化合 同之羥基 .23或酚
-167- (164)1362934 反應圖3 5 Ο Ο Ο
S35.3 S34.8 S35.6 R-link——P—Lv-► 、Lv S34.9 0 R2 R-link_P-N\v(R4b) r3oh 0 R-link—R-〇r3 、N-R2 S34.7 5b co2r S34.11 co2r S35.3 5b 反應圖3 5實例1
R-link—Px-〇Ph-OH S35.7 ί? H2NCH(Me)C02Et n R-link一P-〇Ph -R-link—Ρχ-。Ph C| S35.9 NH Me—( C02Et S35.10 S35.8 -168- ⑧ (165)1362934 反應圖3 5實例2 〇 R-link—PN-〇Bn - OH S35.11 O R-link- Me- P-OBn -R-link— II 〜· -P\- OH NH NH ( Me- 人 C02Et C02Et S35.12 S35· CF3CH2〇H S35.14
O R-link—F3-OCH2CF3 NH Me—( C02Et S35.15 反應圖3 5實例3 Ο R-link一ί^-〇Η NH Me—'C02EtS35.13
R-link Me N-Me C02Et S35.17 反應圖35實例4 R-link- -OPh · 、 Cl S35.18 R-link O fi-OPh 、NH2 S35.19
BrCH(Bn)C02Bu -► R-link- S35.20
Bn- O II -p\ 一 OPh *NH / C02Bu S35.21 ⑧ (166) 1362934 反應圖3 5實例5
Ο R-link——f^— Cl S35.22
S35.23 HO O R-link—f^-CI N-Me
C02Et S35.24
PhOH S35.25
反應圖36說明經烷酯基取代之膦酸二酯之製法，其 中之一個酯基團內置入烷酯基取代基。 一個步驟係將依上文所述之法製得之膦酸單酯S34.1 使用上述之一種方法、與羥基酯S36.1(其中11415及R5b 基團乃如同反應圖34中所述）偶合。例如，將等莫耳量 之反應物於碳化二亞胺諸如二環己基碳化二亞胺之存在下 (如同於Au st. J. C hem·，1963, 609中所述）、隨意地於 二甲胺基吡啶之存在下（如同於7>f·, 1999，55，12997中 所述）偶合。反應乃於惰性溶劑中、於室溫下進行。 步驟乃示於反應圖36、實例1中。此方法係將膦酸 單苯酯S36.9於二氯甲烷溶液中於二環己基碳化二亞胺之 存在下與3_羥基—2 —甲基丙酸乙酯S36.10偶合，即得 膦酸混合二酯S36.ll。 -170- (167) 1362934 使用此步驟，但使用不同之羥基酯S33.1取代3 —羥 基一 2 —甲基丙酸乙酯S36.10，即得相對應之產物S33.2 〇 膦酸單酯S34.1轉換成混合二酯S3 6.2之反應亦可藉 由與羥基酯S3 6.1進行Mitsunobu偶合反應而達成（如同 於Org. Leiί.，2001，643中所述）。此方法係令反應物 S34.1及S36.1於極性溶劑諸如四氫咲喃中、於三芳基膦 φ 及偶氮二羧酸二烷酯之存在下結合以得混合二酯S36.2。 R1取代基可藉使用前述方法進行裂解而予變化，以得單 酸產物S36.3。繼而將產物（例如使用上述方法）與羥基 化合物R3OH偶合，即得二酯產物S36.4。 • 步驟乃示於反應圖36、實例2中。此方法係將膦酸 . 單烯丙酯S36.12於四氫呋喃溶液中、於三苯膦及偶氮二 '羧酸二乙酯之存在下與乳酸乙酯S3 6.13偶合，即得膦酸 混合二酯S36.14。令產物與參（三苯膦）铑化氯（威金森 Φ 催化劑）於乙腈中起反應（如前所述）以移除烯丙基團而 得單酸產物S36.15。而後令後者於吡啶溶液中、於室溫下 、於二環己基碳化二亞胺之存在下、與一莫耳當量3 -經 基吡啶S36.16偶合，即得混合二酯S36.17。 使用以上之步驟' 但使用不同之羥基酯S3 6.1及/或 不同之羥基化合物R3〇H取代乳酸乙酯S36.13或3-羥基 吡啶，即得相對應之產物S36.4。 混合二酯S 3 6.2亦可由單酯s 3 4.1中經由中間體活化 單醋S36.5獲得。此步驟係將單醋S34.1藉與（例如）五 -171 - ⑧ (168) (168)1362934 氯化磷（如同於·/· C/iem. 2001, 66，329中所述）， 或與亞硫醯氯或草醯氯（Lv = Cl)，或與三異丙基苯磺 醯氣之 Q比陡液（如同於 心·ϊ ά //wc/eoi/i/e·? 2000, 19，1 885中所述），或與羰基二咪唑（如同於·/. Merf. C/iem. 2002，45，1284中所述）起反應而轉換成活化化合 物S36.5。而後令所得之活化單酯與羥基酯S36.1起反應 (如上所述），即得混合二酯S36.2。 步驟乃示於反應圖36、實例3中。此順序係令膦酸 單苯酯S36.9於乙腈溶液中、於70t下、與十當量之亞硫 .醯氯起反應以得磷醯氯S36.19。而後令產物與4-胺基甲 醯一2—羥基丁酸乙酯S36.20於含三乙胺之二氯甲烷中起 反應，即得混合二酯S36.21。 使用上述之步驟、但使用不同之羥基酯S36.1取代4 —胺基甲醯一 2_羥基丁酸乙酯S36.20，即得相對應之產 物 S36.2。 混合膦酸二酯亦可藉其它供將R3〇基團置入中間體 S3 6.3 (其中羥基酯部分業已置入）中之路徑獲得。此步 驟係依前述之法將單酸中間體S36.3轉換成活化衍生物 S3 6.6 (其中Lv爲離基團諸如氯基、咪唑等）。而後令活 化之中間體與羥基化合物R3〇H於鹼之存在下起反應，即 得混合二酯產物S36.4。 方法乃示於反應圖3 6、實例4中。此順序係令膦酸 酯單酸S36.22與三氯甲磺醯氯於含可力丁之四氫呋喃中 起反應（如同於i. Med. C/zem. 1 995，38，4648中所述） -172- (169) 1362934 以得三氯甲磺醯氧基產物S36.23。而後令此化合物與3_ (嗎啉基甲基）酚S36.24於含三乙胺之二氯甲烷中起反 應，即得混合二酯產物S36.25。 使用上述之步驟、但使用不同之醇R3OH取代3 —( 嗎啉基甲基）酚S36.24，即得相對應之產物S36.4。 膦酸酯S36. 4亦可藉於單酯S34.1上進行烷基化反應 而得。單酸S34.1與鹵基酯S36.7間之反應係於極性溶劑 φ 中、於鹼諸如二異丙基乙胺之存在下進行（如同於
Ckm·，1 987，59，1056中所述）或於非極性溶劑諸如苯中 、於18 —冠醚一 6之存在下進行（如同於Syn. C〇mm.， 1995, 2 5, 3635 中所述）。 • 方法乃示於反應圖36、實例5中。此步驟係令單酸 ' S36.26與2 —溴基—3 -苯基丙酸乙酯S36.27及二異丙基 乙胺於二甲基甲醯胺中、於80 °C下起反應，即得混合二 酯產物S36.28 。 Φ 使用上述之步驟、但使用不同之鹵基酯S36.7取代2 —溴基一 3 —苯基丙酸乙酯S36.27，即得相對應之產物 S36.4 ° -173- ⑧ (170)1362934 反應圖3 6 HOR1 (1 equiv.) R-link- ，\ •OR1 mAbP S36·4 HO-R4b-COOR5b (K )
R-link—P、-〇H OH
C02R 5b
Hal-R4b-COOR5b S33.7 〇 HO-R4b-COOR5b R-link一R-〇R -> R-link- S34.1
、OH O II __ -p—OR 0-R4b-C00R5b R-link- S36.1 O —|i-OR1 Lv S36.5
S36.6 O R-link—P-〇H 0-R4b-C00R5b S36.3 O -p-OR3 0-R4b-C00R5b S36.4 反應圖3 6實例1 R-link—PN-〇Ph OH S36.9 H0CH2CH(Me)C02Et -► S36.10 R-link-
O -A、- OPh O
Me -C02Et S36.11 ⑧ 0 (171) 1362934 反應圖3 6實例2
>-R-link — Me- 3-OH Ο / C02Et S36.15 σ
OH S36.16 Ο ιι R-link—P'-O、 O Me—( 、N， CO〇Et S36.17 2
反應圖3 6實例3 R-link-
O -t^-OPh OH
SOCI 2 -i·- R-link- S36.18 S36.9 0 -p-OPh 1 Cl S36.19
Et02CCH(0H)CH2CH2C0NH2 S36.20
一 OPh C02Et H2N S36.21 175 - (172) 1362934 反應圖3 6實例4 0 R-link—Ρχ-ΟΗ- Ο
Me—^ C02Et S36.22 Ο R-link—|3-OS〇2〇Cl3 Ο
Me—( C02Et S36.23
C02Et S36.25 反應圖3 6實例5 Ο R-link——Ρν-ΟΗ OCH2CF3 S36.26
BrCH(Bn)C02Et ->~ S36.27
O R-link—Px-〇CH(Bn)C02Et OCH2CF3 S36.28 反應圖37說明膦酸二酯之製法，其中兩個酯取代基 均置入烷酯基團。 化合物係直接或間接地由膦酸S34.6中製備。其一係 將膦酸與羥基酯S37.2於前述反應圖34 - 36之狀況下， 諸如使用二環己基碳化二亞胺或類同試劑進行偶合反應， 或於Mitsunobu反應狀況下偶合，即得二酯產物S37.3, 其中二個酯取代基相同。 此法乃示於反應圖37、實例1中。此步驟係令膦酸 S34.6與三莫耳當量之乳酸丁酯S37.S於Aldrithio卜2及 -176- (173) 1362934 三苯膦之存在下、於吡啶中 '於約70°C下起反應，即得 二酯 S37.6。 使用上示步驟，但使用不同之羥基酯S3 7.2取代乳酸 丁酯S37.5，即得相對應之產物S37.3。 此外，二酯S37.3可藉將膦酸S34.6以鹵基酯S37.1 予以院基化而得。院基化反應係如同反應圖36中供製備 酯S36.4所述之法進行。 φ 此法乃示於反應圖37、實例2中。此步驟係令膦酸 S34.6與過量之3 -溴基一2 —甲基丙酸乙酯S37.7及二異 丙基乙胺於二甲基甲醯胺中、於約80 °C下起反應（如同 於 Anal. Chem.，1 987，59，1056 中所述），即得二酯 ' S37.8 ° - 使用上示之步驟，但使用不同之鹵基酯S37.1取代3 -溴基一 2 —甲基丙酸乙酯 S37.7，即得相對應之產物 S37.3 ° # 二酯S3 7· 3亦可藉將膦酸之活化衍生物S34.7與羥基 酯S37.2進行置換反應而得。置換反應係於極性溶劑中、 於適當鹼之存在下進行（如同反應圖36中所述）。置換 反應乃於過量羥基酯之存在下進行以得其中兩個酯取代基 相同之二酯產物S37.3，或接續以限量之不同羥基酯處理 以製得其中兩個酯取代基互異之二酯S37.3。 此法乃示於反應圖37、實例3及4中。如同實例3 中所示，令磷醯二氯S35.22與三莫耳當量之3—羥基—2 -(羥甲基）丙酸乙酯S37.9於含碳酸鉀之四氫呋喃中起 -177- ⑧ (174) 1362934 反應，即得二酯產物S37.10。 使用上示之步驟，但使用不同之羥基酯S37.2取代3 一羥基一2—（羥甲基）丙酸乙酯S37.9，即得相對應之產 物 S37.3。 反應圖37、實例4說明等莫耳量磷醯二氯S35.22與 2—甲基—3—羥基丙酸乙酯S37.11間之置換反應以得單 酯產物S37.12。反應係於乙腈中、於70°C下、於二異丙 Φ 基乙胺之存在下進行。而後令產物S37.12於相同狀況下 與一莫耳當量乳酸乙酯S37· 13起反應，即得二酯產物 S37.14 ° 使用上示之步驟，但接續與不同之羥基酯S37.2反應 ' 以取代 2—甲基一3_羥基丙酸乙酯S37.ll及乳酸乙酯 一 S 3 7 · 1 3 ，即得相對應之產物S 3 7.3 〇
-178- ⑧ (175)1362934 反應圖3 7 Ο Ο
反應圖3 7實例1 ί? H0CH(CH3)C02Bu R-link—《一 〇H -►- OH S37.5 i? R-link——0CH(CH3)C02Bu 0CH(CH3)C02Bu S37.6 反應圖3 7實例2 BrCH2CH(CH3)C02Et -►- OH S37.7 S34.6 R-link- i?
OH O R-link—P^—0CH2CH(CH3)C02Et 0CH2CH(CH3)C02Et S37.8 ⑧ (176) 1362934 反應圖3 7實例3 0 R-link—PN-CI Cl S35.22 (H0CH2)2CHC02Et S37.9 0 R-link—f=—0CH2CH(CH20H)C02Et 、0CH2CH(CH20H)C02Et S37.10 反應圖3 7實例4
〇 H0CH2CH(CH3)C02Et R-|ink-Prcl "^Τϊ S35.22
O R-link—P-〇CH2CH(CH3)C02Et Cl S37.12 HOCH(CH3)C02Et S37.13
O R-link—P-〇CH2CH(CH3)C02Et 0CH(CH3)C02Et S37.14 2,2 —二甲基一 2—胺乙基膦酸中間體可藉反應圖5中 之路徑製得。令2-甲基- 2-丙亞磺醯胺與丙酮縮合以 得亞磺醯亞胺 S38.ll (入 Org. Chm. 1999，64，12 )。 將甲基膦酸鋰二甲酯加至 S38.ll後可得 S38.12。將 S38.12進行甲醇分解作用可得胺S38.13。將胺以Cbz基 團保護，再將甲基團移除以得膦酸S38.14，其可使用稍早 所述之方法轉換成期望之S38.15 (反應圖38a)。化合物 S38.14之另一合成法亦示於反應圖38b中。根據文獻方法 (J. Org. Chem. 1992， 57, 58 1 3； Syn. Lett. 1997， 8, 893 )將市售之2 -胺基一 2_甲基一 1 一丙醇轉換成氮丙啶 S38.16。以亞磷酸酯將氮丙啶開啓以得 S38.17 ( -180- ⑧ (177) 1362934 1980，27，1 623 )。再將 S38.17 予以再 保護，即得S38.14。 反應圖3 8 h2n X^〇h 、HP(0)(0CH3)2 ，NR ~NiH RHN S38.16R = Cb R，s〇
S38.17
CbzHN
S38.14
BzO
實例及例示實施例 BzO 2 —去氧一 2 —氟基一3,5 —二—Ο —苯醯一 α 一 D —阿拉伯 呋喃糖苷基溴（2)
Tann et al., JOC 1985, 50, p.3644 Howell et al., JOC 1988, 53, p.85 將33%氫溴酸/乙酸（80毫升）加至1 ( 120克， 258毫莫耳）（由Davos或CMS chemicals所售）之二氯 甲烷（1升）溶液中。再將混合物於室溫下攪拌16小時 ，以冰水冷卻，再以碳酸氫鈉（150克/1.5升溶液）於1 _2小時期間徐緩中和。繼而將二氯甲烷相分離出及於減 壓下濃縮。令餘留物溶於乙酸乙酯中並以碳酸氫鈉清洗直 至酸不存在爲止。繼而將有機相於硫酸鎂上乾燥，過濾及 ⑧ -181 - (178) 1362934 於減壓下濃縮，即得黃色油狀之產物2(約115克）。
CI
2—去氧一2—氣基一3,5 —二一 Ο —苯酿一— D —阿拉伯 呋喃糖苷基一 9H— 6—氯基嘌呤（3) • Ma et al.，J. Med. Chem. 1997, 40, 2750
Marquez et al” J. Med· Chem. 1990, 33, 978 Hildebrand et al·，J. Org· Chem· 1992，57, 1808 Kazimierczuk et aK JACS 1984, 106, 6379 ' 將6-氯基嘌呤（52.6克）分三份加至氫化鈉（14克 ‘ ，60% )之乙腈（ 900毫升）懸浮液中。再將混合物於室 溫下攪拌1.5小時。而後將2 ( 258毫莫耳）之乙腈（300 毫升）溶液逐滴加入。繼而以乙酸（3.5毫升）令反應中 ® 止，過濾及於減壓下濃縮。令餘留物分界於二氯甲烷與水 間。再將有機相於硫酸鎂上乾燥，過濾及濃縮。而後將餘 留物以二氯甲烷而後乙醇（總體約1 : 2 )處理以沉澱出 黃色固狀之期望產物3(83克，由1中得65 % )。 OMe
-182- (179) 1362934 2 —去氧_2—氟基一 p— D —阿拉伯咲喃糖苔基—6—甲氧 基腺嘌呤（4) 將甲醇鈉（25重量％，76毫升）加至於〇°C下之3 (83克’ 167毫莫耳）之甲醇（1升）懸浮液中。再將混 合物於室溫下攪拌2小時。而後以乙酸（約Η毫升，pH =7)令反應中止。繼而將混合物於減壓下濃縮，再令所 得餘留物分界於己烷與水間（約500毫升己烷及300毫升 φ 水）。而後將水性層分離，將有機層與水（約300毫升） 再度混合一次。繼而將水的部份結合及於減壓下濃縮成約 100毫升。再將沉澱出之產物4藉過濾法收集（42克，88 % )。 OMe
2_去氧一2 —氟基一 5 —羧基一 P—D —阿拉伯呋喃糖苷基 一 甲氧基腺嘌呤（5)
Moss et al. J. Chem. Soc. 1963，pll49 將鉑/碳（10%，15克（20—30 %莫耳當量），水 漿液形式）及碳酸氫鈉（1.5克，17.94毫莫耳）之水（ 5〇0毫升）混合液於65°C下於氫下攪拌0.5小時。而後令 反應混合物冷卻’置於真空下，再以氮沖洗數次以完全移 除所有的氫。繼而將化合物4(5.1克，17.94毫莫耳）於 室溫下加入。再將反應混合物於65 °C下於氧（氣球）下 -183- (180) 1362934 攪拌直至藉LC— MS判定反應已完全爲止（通常24—72 小時）。而後將混合物冷卻至室溫並予過濾。將鉑/碳以 水徹底清洗。繼而將結合之濾液濃縮成約30毫升，藉於 〇°C下加入氫氯酸（4N )予以酸化（pH 4 )。再將沉澱出 之黑色固狀物藉過濾法收集。令粗製產物溶於最小量之甲 醇中，再通過矽膠墊中過濾（以甲醇洗提）。而後將濾液 濃縮及由水中結晶，即得灰白色固狀之化合物5 ( 2.5克
OMe 〇 (2’R，3’S，4’R，S’R) -6-甲氧基一9—[四氫 4—碘基 一3 —氟基一5—(二乙氧基膦醯）甲氧基一 2—呋喃基]嘌呤
Zemlicka et al·， J. Amer. Chem. Soc. 1972， 94, p3213 將二甲基甲醯胺縮二新戊醇（150毫升，538毫莫耳 )及甲磺酸（9.5毫升，146.6毫莫耳）加至5(22克， 73_77毫莫耳）之二甲基甲醯胺（400毫升）溶液中。再 將反應混合物於80-93 °C (內部溫度）下攪拌30分鐘， 而後冷卻至室溫並於減壓下濃縮。繼而令餘留物分界於乙 酸乙酯與水間。再將有機相分離出並以碳酸氫鈉其後鹽水 清洗，於硫酸鎂上乾燥，過濾及於減壓下濃縮。令餘留物 -184- ⑧ (181) 1362934 及（羥甲基）膦酸二乙酯（33毫升，225毫莫耳）溶於二 氯甲烷（250毫升）中，再冷卻至-40 °C。繼而將單溴化 碘（30.5克，1.1莫耳）之二氯甲烷（1〇〇毫升）溶液逐 滴加入。再將混合物於-20至-5 °C下攪拌6小時。而後以 碳酸氫鈉及硫代硫酸鈉令反應中止。將有機相分離出，將 水相以二氯甲烷萃取。再將結合之有機相以鹽水清洗，於 硫酸鎂上乾燥及於減壓下濃縮。而後將餘留物藉矽膠層析 φ 法予以純化，即得產物6 ( 6克，15.3% )。 製備6之另一步驟 將 （2.0克，6,7毫莫耳）之四氫呋喃（45毫升）溶 * 液於氮下以三苯膦（2.3克，8.7毫莫耳）處理。再將偶 - 氮二羧酸二異丙酯（1.8克，8.7毫莫耳）徐緩加入。而 後將反應混合物於室溫下攪拌1小時，繼而於減壓下濃縮 至乾。令餘留物溶於二氯甲烷（20毫升）中，而後以（ Φ 羥甲基）膦酸二乙酯（4.5克，27毫莫耳）處理。再將混 合物冷卻至-60 °C，繼而將單溴化碘（2克，9.6毫莫耳） 之二氯甲烷（10毫升）冷溶液加入。將反應混合物加溫 至-10°C並保持於10°c下1小時。再將反應混合物以二氯 甲烷稀釋，以飽和水性碳酸氫鈉而後水性硫代硫酸鈉清洗 。繼而將有機相分離出，於硫酸鎂上乾燥及於減壓下濃縮 至乾。再將反應混合物藉矽膠層析法（以25%乙酸乙酯 之二氯甲烷液而後轉換至3%甲醇之二氯甲烷液洗提）予 以純化，即得產物6 ( 0.9克，33% )。 -185- ⑧ (182) 1362934
EtO Μ OMe Ο 〈/ Et〇j\/〇丫0丫 Ν
(2’R，5’R) — 6 —甲氧基一9— [3—氟基一2,5 —二氫一5 — (二乙氧基膦醯）甲氧基一 2—呋喃基]嘌呤（7) 將次氯酸鈉（10-13%) (50毫升）逐滴加至化合 物6(6克，11.3毫莫耳）之乙酸（2.5毫升）溶液中。 而後將反應混合物攪拌0.5小時及於減壓下濃縮。繼而將 餘留物以乙酸乙酯處理而後過濾以移除固狀物。再將濾液 濃縮，而後將餘留物藉矽膠層析法予以純化，即得產物7 (4 克，88% )。
(21，5’R) — 9— (3—氟基一2,5~ 二氫一 5—膦醯甲氧 基一 2—呋喃基）腺嘌呤二鈉鹽（8) 將化合物7(2.3克，5.7毫莫耳）之甲醇（6毫升） 溶液與氫氧化銨（28— 30%) (60毫升）混合。再將所 得混合物於120°C下攪拌4小時，冷卻而後於減壓下濃縮 。繼而將餘留物於真空下乾燥12小時。令餘留物溶於二 甲基甲醯胺（40毫升）中，再將溴三甲基矽烷（3.5毫升 186- ⑧ (183) 1362934 )加入。繼而將混合物於室溫下攪拌16小時，而後於減 壓下濃縮。令餘留物溶於水性碳酸氫鈉（2.3克之100毫 升水液）中。再將溶液蒸發並令餘留物於C一 18 (4〇微米 )柱上（以水洗提）予以純化。而後將水性溶離份凍乾， 即得二鈉鹽8(1.22克，57%)。
單胺基膦酸酯製劑之實例（9) % 將二鈉鹽8(25毫克，0.066毫莫耳），（S) — Ala • — 〇 -環丁酯氫氯酸鹽（24毫克，2當量，0.133毫莫耳 )及酚（31毫克，0.333毫莫耳）於無水吡啶（1毫升） 中混合。再將三乙胺（111微升，0.799毫莫耳）加入， ^ 而後將所得混合物於6(TC下、於氮下攪拌。於另一個燒 瓶內，令2’-Aldrithiol (122毫克，0.466毫莫耳）及三苯 膦（103毫克，0.466毫莫耳）溶於無水吡啶( 〇·5毫升） 中，再將所得黃色溶液攪拌15 - 20分鐘。而後將此溶液 一次地加至8之溶液中。將結合之混合物於60 °C下、於 氮下攪拌16小時以得清澈黃色至淡棕色溶液。而後將混 合物於減壓下濃縮。令所得油狀物溶於二氯甲烷中，再藉 矽膠層析法（以0 _ 5 %甲醇之二氯甲液進行線性梯度洗 提）予以純化以得油狀物。令所得油狀物溶於乙腈及水中 -187- ⑧ (184) 1362934 ，再藉製備HPLC (線性梯度，5 - 95%乙腈之水液）予 以純化。而後將純溶離份結合及凍乾，即得白色粉狀之單 胺基膦酸酯9。
雙胺基膦酸酯製劑之實例（10) 將二鈉鹽8(12毫克，0.032毫莫耳），（S) _Ala —〇 -正丙酯氫氯酸鹽（32毫克，6當量，0.192毫莫耳 ' )無水吡啶（1毫升）中混合。再將三乙胺（53微升， • 0.384毫莫耳）加入，而後將所得混合物於60°C下、於氮 下攪伴。於另一個燒瓶內，令2’-Aldrithiol(59毫克， 0.224毫莫耳）及三苯膦（49毫克，0.224毫莫耳）溶於 # 無水毗啶（0.5毫升）中，再將所得黃色溶液攪拌15 — 20 分鐘。而後將此溶液一次地加至8之溶液中。將結合之混 合物於60°C下、於氮下攪拌16小時以得清澈黃色至淡棕 色溶液。而後將混合物於減壓下濃縮。令所得油狀物溶於 二氯甲烷中，再藉矽膠層析法（以0-5%甲醇之二氯甲 液進行線性梯度洗提）予以純化以得油狀物。令所得油狀 物溶於乙腈及水中，再藉製備HPLC (線性梯度，5 - 95 %乙腈之水液）予以純化。而後將純溶離份結合及凍乾， 即得白色粉狀之雙胺基膦酸酯10。 -188 - ⑧ (185) 1362934 單胺基滕酸酯製劑之實例（11)
將化合物8(1.5克，4毫莫耳）與丙胺酸乙酯氫氯酸 ^ 鹽（1.2]克，8毫莫耳）及酚（1.88克，20毫莫耳）混 合。再將無水吡啶（35毫升）其後三乙胺（6.7毫升，48 毫莫耳）加入。繼而將混合物於60°C下、於氮下攪拌15 —20分鐘。於另一燒瓶中，令2'-A]drithiol(7.3克）與 » 三苯膦（6 · 2克）於無水吡啶（5毫升）中混合，再將所 ' 得混合物攪拌1 〇 - 1 5分鐘以得清澈淡黃色溶液。而後將 此溶液加至上述混合物中並於60 °C下攪拌過夜。再將混 合物於減壓下濃縮以移除吡啶。令所得餘留物溶於乙酸乙 ® 酯中並以飽和碳酸氫鈉溶液（2x )而後飽和氯化鈉溶液清 洗。繼而將有機層於硫酸鈉上乾燥，過濾而後於減壓下濃 縮。令所得油狀物溶於二氯甲烷中，再負載至乾 CombiF】 ash柱（40克）上，同時於10分鐘期間以0—5 %甲醇之二氯甲烷液進行線性梯度洗提而後以5%甲醇之 二氯甲烷液洗提7 - 10分鐘。繼而將含期望產物之溶離份 結合及於減壓下濃縮以得泡沫狀物。令此泡沫狀物溶於乙 腈中再藉製備HPLC予以純化，即得11 ( 0.95克）。 令11 (950毫克）溶於小量乙腈中，再令其於室溫下 -189- (186) 1362934 靜置過夜。而後藉過濾法收集固狀物並以小量之乙腈清洗 。固狀物爲GS-327625。將濾液於真空下減量而後負載至 已於緩衝液A(2%乙醇之乙腈液）中均衡化之Chiralpak AS-H柱上。異構體A，12，乃隨著緩衝液a以10毫升/ 分鐘之速17分鐘而洗提出。其後緩衝液13(50%甲醇之 乙腈液）則用以將異構體13於8分鐘內由柱中洗提出。 移除所有溶劑並令其再溶於乙腈及水中。再將樣品凍乾（ Mass-348 毫克）。 實例1 0 2 舉例而非限制，本發明實施例乃以下列列表格式（表 Y)命名。這些實施例具有通式，MBF3，。 MBF3 ： Sc.Kl.K2 每一 MBF3之實施例均以經取代之核（Sc )來說明。 ® Sc乃述於下列表丨·1中。Sc亦以本文所存在之帶有至少 一個K1或K2(其中每一者均爲共價接合至Sc上的一個 點）之任何結構式說明。在表γ中所述之彼些實施例方 面’ Sc爲以一個數字所表示之核，而每一個取代基再依 順序以數字表示。表1」爲用以形成表γ實施例中之核的 —個表。每個核（Sc)均給予—個取自表中之編號標 不’而此標示係以1至2之數字最先出現在每一實施例中 。同樣地’表20.1至2〇 37列出所擇定取代基團（以編 號標示），且當然如所列地於K1— K2處接合至Sc上。 -190- ⑧ (187) 1362934 K1或K2已知並不代表原子，而係連接至母骨架Sc上的 點。因此，式MB F3化合物係根據下列表γ之化合物爲基 準而包括具有Sc基團之化合物。所有事例中，式MBF3 化合物均於核Sc上具有K1及K2，且相對應之基團K1 及K2乃如同於下表中所示。 因此，表Y中每個命名之實施例係以表1.1中標示核 之數字，其後標示每一個K1取代基團之數字，其後標示 φ 取代基K2之數字（如同於表20.2至20.36所示）來說明 。於圖解表格形式中，表Y之每個實施例均以具有條理 排列法之命稱出現：
Sc.Kl .K2 ， 每個Sc基團均顯示具有各種不同之取代基K1或K2 。每個列於表Y中之K1及K2基團爲列於表Y中之Sc核 之取代基。K1及K2已知並不代表基團或原子，而係單純 Φ 代表連接點。共價鍵結至核（Sc)上之位置在式MBF3中 係以K1及K2代表。表20.1至20.37中之K1及K2實施 例係以編號1至247表示。例如表1 . 1中有兩個參選者， 而這些Sc參選者編號爲1至2。每一者均標記爲Sc之識 別者（亦即1至2)。任何狀況下，表20.1至20.37之參 選者都是以一個數字開始，且獨立地擇自表20.1至20.37 ’因而每一者獨立地標記爲編號1至247。接合點之選擇 乃如同本文中所述。舉例但不限制，接合點乃擇自反應圖 及實例中所述者。 ⑧ (188)1362934
表1·1
-192- ⑧ (189)1362934 表 20.1
-193- (190)1362934 表 20.2
⑧ (191)1362934 表 20.3
-195- ⑧ (192) 1362934 表 20.4 CH3 Ο 20
CH,
O 、0 22
(193)1362934 表 20.5
H3C h3c
29 °
-197- (194)1362934 表 20.6
H3C
⑧ (195)1362934 表 20.7
R5 R5 0、
、0 O 40 'R4
R1 0 41
-199- (196)1362934 表 20.8
⑧ 1362934
201 - ⑧ (198)1362934 表 20.10
-202- 1362934
⑧ (200)1362934 表 20.12
⑧ 1362934
⑧ -205- 1362934
-206- ⑧ (203)1362934 表 20.15
⑧i (204)1362934 表 20.16
V Τ Ϊ t ⑧ -208- (205)1362934 表 20.17
105 -209 - ⑧ 1362934
-210 ⑧ (207)1362934 表 20.19 CHq 0>
N 110 o ch3 ,0、 'w3 ch3
o 112
111
CH
CH3
N
116 〇 -211 - ⑧ (208)1362934 II. 表 20.20
-212 ⑧ (209)1362934 III. 表 20.21
213- (D- (210)1362934 IV. 表 20.22 H3C\
-214- (211)1362934 V. 表 20.23
138 (212)1362934 VI. 表 20.24
R4
R5 141
142
R4
R】 0
143 R1 R1
R1
146 R1
⑧ (213)1362934 VII. 表 20.25
R4 148 149 150
151 152 153
!54 155 156
R3 157 158 159
-217 - (214)1362934 VIII. 表 20.26
218- ⑧ (215)1362934 IX. 表 20.27
172 %人R5 173 ο 〇
-219- ⑧ 179 178 (216)1362934 X. 表 20.28
⑧ (217)1362934 XI. 表 20.29
186 187
Ο
Ο
R1 189 188
⑧ 193 192 (218)1362934 XII. 表 20.30
Ο
0^ '0 ⑧ -222- 199 (219)1362934 XIII. 表 20_31
203
0
Η
204 205
207
-223- 206 (220)1362934 XIV. 表 20.32
CH3 Ο
208 0 ch3
209
212 Ο
-224- ⑧ (221)1362934 XV. 表 20.33
214 215
Ο
Ο
R4 Ο
R1 216
221 -225 - ⑧ 220 (222)1362934 XVI. 表 20.34
CH3 Ο
222 O CH3
223 224
Ο
、cr '0 226 Ο 《0八。人 -226- 227 (223)1362934 XVII. 表 20.35
⑧ (224)1362934 XVIII.表 20.36
R3 Ο 236
/〇\ Nr r4 Ι3 1 R 238 〇 、九\士 240
R1 239 241
242 243 -228- (225)1362934 表 20.37
-229- ⑧ (226)1362934 表Υ· 1.1.1 1.2.1 1.3.1 1.4.1 1.5.1 1.6.1 1.7.1 1.8.1 1.9.1 1.10.1 1.11.1 1.12.1 1.13.1 1.14.1 1.15.1 1.16.1 1.17.1 】_18.】 1.19.1 1.20.1 1.21.1 1.22.1 1.23.1 1.24.1 1.25.1 1.26.1 1.27.1 1.28.1 1.29.1 1.30.1 1.31.1 1.32.1 1.33.1 1.34.1 1.35.1 1.36.1 1.37.1 1.38.1 1.39.1
1.40.1 1.4M 1.42.1 1.43.1 1.44.1 1.45.1 1.46.1 】·47.】 1.48.1 1.49.1 1.50.1 1.51.1 1.52.1 1.53.1 1.54.1 1.55.1 1.56.1 1.57.1 1.58.1 1.59.1 1.60.1 1.61.1 1.62.1 1.63.1 1.64.1 1.65.1 Ι^1^1^1^1^1^1^1^1^1^1^1Μ1^1·1-1-1^1^ΙΜΙ1-1^1·1-1^Ϊ^Τ^Τ-1-1-ι^1^1-1^1^0123456789012345678 90 丨 234567890 6 7 8 9 ο 1 2 3 4 5 6 -— 8 9 0 12 3 4 5 6 7 8 9 ο 12 3 4 5 6 7 8 9 οοοο&οοο ο Q111111111 12 2 2 2 2 2 2 2 2 2 3 66667777777777888888888899999999991111111111111111111 11111111]]]] ·····--···*····**····♦··♦·········· ············ ^1 m 1 ] 1« 1 1 1 1 n 1# υ υ υ 11 1 1 J υ 1 1 1 1 1 Ϊ 1A 1 1 i If 1.131.1 1.196.1 1.14.2 1.79.2 1.144.2 1.209.2 1.132.1 1.197.1 1.15.2 1.80.2 1.145.2 1.210.2 1.133.1 1.198.1 1.16.2 1.81.2 1.146.2 1.211.2 1.134.1 1.199.1 1.17.2 1.82.2 1.147.2 1.212.2 1.135.1 1.200.1 1.18.2 1.83.2 1.148.2 1.213.2 1.136.1 1.201.1 1.19.2 1.84.2 1.149.2 1.214.2 1.137.1 1.202.1 1.20.2 1.85.2 1.150.2 1.215.2 1.138*1 1.203.1 1.21.2 1.86.2 1.151.2 1.216.2 1.139.1 1.204.1 1.22.2 1.87.2 1.152.2 1.217.2 1.140.1 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1.196." 1.16.12 1.83.12 1.150.12 1.197J1 1.17.12 1.84.12 1.15J.12 1.198.Π 1.18.12 1.85.12 1.152.12 1.199.11 1.19.12 1.86.12 1.153.12 1.200. Π 1.20.12 1.87.12 1.154.12 1.201.Π 1.2Π2 1.88.12 1.155.12 1.202.11 1.22.12 1.89.12 1.156.12 1.203.11 1.23.12 1.90.12 1.157.12 1.204.11 1.24.12 1.91.12 1.158.12 1.205.11 1.25.12 1.92.12 1.159.12 1.206.11 1.26.12 1.93.12 1.160.12 L207.ll 1.27.12 1.94.12 1.161.12 1.208.11 1.28.12 1.95.12 1.162.12 1.209.11 1.29.12 1.96.12 1.163.12 1.210.11 1.30.12 1.97.12 1.164.12 1.211.Π 1.31.12 1.98.12 1.165.12 1.212.11 1.32.12 1.99.12 ].166.12 L213.ll 1.33.12 1.100.12 1.167.12 1.214.11 1.34.12 1.101.12 1.168.12 1.215.11 1.35.12 1.102.12 1.169.12 L216.31 1.36.12 1.103.12 1,170.12 1.217.11 】.37.12 1.104.12 1·Π1_12 1,218.11 1.38.12 1.105.12 1.172.12 1.219.11 1.39.12 1.106.12 1.173.12 1.220. Π 1.40.12 1.107.】2 1.174.12 1.221.11 1.41.12 1.108.12 】.175.12 1.222.11 1.42.12 1.109.12 1.176.12 1.223:11 1.43.12 1.110.12 1.177.12 1.224.11 1.44.12 1.Π1.12 1.178.12 1.225.11 1.45.12 1.112.12 1.179.12 1.226.11 1.46.12 1.113.12 1.180.12 1.227.11 1.47.12 1.114.12 1.181.12 1.228.11 Κ48.12 1,115,12 1.182.12 1.229.11 1.49.12 1.Π6.12 1.183.12 1.230.11 1.50.12 1.117.12 1.184.12 1.231.11 1.51.12 1.118.12 1.185.12 1.232.11 1.52.12 1.119.12 1.186.12 1.233.11 1.53.12 】·]20·12 1.187.12 1.234.11 1.54.12 1.121.12 1.188.12 1.235.J1 1.55.12 1.122.12 1.189.12 1.236.11 1.56.12 1.123.12 1.190.12 1.237.11 1.57.12 1.124.12 1.191.12 1.238.11 1.58.12 1.125.12 1.192.12 1.239.11 1.59.12 1.126.12 1.193.12 1.240.11 1.60.12 1.127.12 1.194.12 1.241.Π 1.61.12 1.128.12 1：195.12 1.242.11 1.62.12 1.129.12 1.196.12 1.243.11 1.63.12 1.130.12 1.197.12 1.244.11 1.64.12 1.131.12 1.198.12 1.245.11 1.65.12 1.132.12 1.199.12 1.246.11 1.66.12 1.133.12 1.200.12 1.247.11 1.67.12 1.134.12 1.201.12 1.1.12 1.68.12 1.135.12 1.202.12 1.2.12 1.69.12 1.136.12 1.203.12 1.3.12 1.70.12 1.137.12 1.204.12 1.4.12 1.71.12 1.138.12 1.205.12 1.5.12 1.72.12 1.139.12 1.206.12 1.6.12 1.73.12 1.140.12 1.207.12 1.7.12 1.74.12 1.141.12 1.208.12 1.8.12 1.75.12 1.142.12 1.209.12 1.9.12 1.76.12 1.143.12 1.210.12 1.10.12 1.77.12 1.144.12 1.211.12 1.11.12 1.78.12 1.145.12 1.212.12 1.12.12 1.79.12 1.146.12 1.213.12 1.13.12 1.80.12 1.147.12 1.214.12 1.14.12 1.81.12 1.148.12 1.215.12 1.15.12 1.82.12 1.149.12 1.216.12 1.217.12 1.37.13 1.104.13 1.171.13 1.218.12 1.38.13 1.105.13 1.172.13 1.219J2 1.39.13 1.106.13 1.173.13 1.220.12 1.40.13 1.107.13 L174.13 1.221.12 1.41.13 1.108.13 1.175.13 1.222.12 1.42.13 1.109.13 1.176.13 1.223.12 1.43.13 1.110.13 [177.13 1.224.12 J.44.13 1.111.13 1.178.13 1.225.12 1.45.13 】.112.13 1.179.13 1.226.12 1.46.13 1.113.13 1.180.13 1.227.12 1.47.13 1.114.13 1.181.13 1.228.12 1.48.13 1.115.13 1.182.13 1.229.12 1.49.13 1.116.33 1.183.13 1.230.12 1.50.Ϊ3 1.117.13 1.184.13 1.231.12 1.51.13 1.118.13 1.185.13 1.232.12 1.52.13 1.119.13 1.186.13 1.233.12 1.53.13 1.120.13 1.187.13 1.234.12 1.54.13 1.121.13 1.188.13 1.235.12 1.55.13 1.122.13 1.189.13 1.236.12 1.56.13 1.123.13 1.190.13 1.237.12 1.57.13 1.124.13 1.191.13 1.238.12 1.58.13 1.125.13 1.192.13 1.239.12 1.59.13 1.126.13 1.193.13 1.240.12 1.60.13 1.127.13 1.194.13 1.241.12 1.61.13 1.128.13 1.195.13 1.242.32 1.62.13 1.129.13 1.196.13 1.243.12 1.63.13 1.130.13 1.197.13 1.244.12 1.64.13 1.131.13 1.198.13 1.245.12 1.65.13 1.132.13 1.199.13 1.246.12 1.66.13 1.133.13 1.200.13 1.247.12 1.67.13 1.134.13 1.201.13 1.1.13 1.68.13 1.135.13 1.202.13 1,2,13 1.69.13 1.136.13 1.203.13 1.3.13 1.70.13 1.137.13 1.204.13 1.4.13 1.71.13 1.138.13 1.205.13 1.5.13 1.72.13 1.139.13 1.206.13 1.6.13 1.73.13 1.140.13 1.207.13 1.7.13 1.74.13 1.141.13 1.208.13 1.8.13 1.75.13 1.142.13 1.209.13 1.9.13 1.76.13 1.143.13 1.210.13 1.10.13 1.77.13 1.144.13 1.211.13 1.11.13 1.78.13 1.145.13 1.212.13 1.12.13 1.79.13 1.146.13 1.213.13 1.13.13 1.80.13 1.147.13 1.214.13 1.14.J3 1.81.13 1.148.13 1.215.13 1.15.13 1.82.13 1.149.13 1.216.13 1.16J3 1.83.13 1.150.13 1.217.13 1.17.13 L84.13 1.151.13 1.218.13 1.18.13 1.85.13 1.152.13 1.219.13 1.19.13 1.86.13 1.153.13 1.220.13 1.20.13 1.87.13 1.154.13 1.221.13 1.21.13 1.88.13 1.155.13 1.222.13 1.22.13 1.89.13 1.156.13 1.223.13 1.23.13 1.90.13 1.157.13 1.224.13 1.24.13 1.91.13 1.158.13 1,225.13 1.25.13 1.92.13 1.159.13 1.226.13 1.26.13 1.93.13 1.160.13 1.227.13 1.27.13 1.94.13 1.161.13 1.228.13 1.28.13 1.95.13 1.162.13 1.229.13 1.29.13 1.96.13 1.163.13 1.230.13 1.30.13 1.97.13 1.164.13 1.231.13 1.31.13 1.98.13 1.165.13 1.232.13 1.32.13 1.99.13 1.166.13 1.233.13 1.33.13 1.100.13 U67.I3 1.234.13 1.34.13 1.101.13 1.168.13 1.235.13 1.35.13 ].102.13 1.169.13 1.236.13 1.36.13 1.103.13 1.J70.13 1.237.13
235- (232)1362934
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244- (241)1362934
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2.2.10 2.69.10 2.136.10 2.203.10 2.23.11 2.90.11 2.157.11 2.224.11 2.3.10 2.70,10 2.137.10 2.204.10 2.24.11 2.91.Π 2.158.11 2.225.11 2.4.10 2.71.ΙΟ 2.I3S.I0 2.205.10 2.25. Π 2.92.11 2.159.1) 2.226.1) 2.5.J0 2.72.10 2.139.10 2.206.10 2.26.11 2.93.11 2.160.11 2.227.11 2.6.10 2.73.10 2.140.10 2.207.10 2.27.11 2.94.11 2.16U1 2.228.Π 2.7.10 2.74.10 2.141.10 2.208.10 2.28.11 2.95.11 2.162.11 2.229.11 2.8.10 2.75.10 2A42.10 2.209.10 2.29.)1 2.96.11 2.163.11 2.230.11 2.9.10 2.76.10 2.143.10 2.210.10 2.30.11 2-97.11 2.164.11 2.231.11 2.10.10 2.77.10 2.144.10 2.211.10 2.31.11 2.98.11 2.165.11 2.232.11 2.11.10 2.78.10 2.145.10 2.212.10 2.32.11 2.99,11 2.166.11 2.233.11 2.J2.J0 2.79.10 2J46J0 2.2)3.10 2.33.11 2.100.11 2.167.11 2.234.Π 2.13.10 2.80.10 2.147.10 2.214.10 2.34.11 2.101.11 2.168.11 2.235.11 2.14.10 2.81.10 2.148.10 2.215.10 2.35.11 2.102.11 2.169.11 2.236.11 2.15.10 2.82.10 2.149.10 2.216.10 2.36.11 2.103.11 2.170.11 2.237.11 2.16.10 2.83.10 2.150.10 2.217.10 2.37.11 2.104.11 2.171.11 2.238.Π 2.17.10 2.84.10 2.151.10 2.218.10 2.38.11 2.105.11 2.172.11 2.239.11 2.18.10 2.85.10 2.152.10 2.219.10 2.39.Π 2.106.11 2.173.11 2.240.11 2.19.10 2.86.10 2.153.10 2.220.10 2.40.11 2.107.11 2.174.11 2.241.11 2.20.10 2.87.10 2.154.10 2.221.10 2.41.11 2.108.11 2.175.11 2.242.11 2.21.10 2.88.10 2.155.10 2.222.10 2.42.11 2.109.Π 2.176.Π 2.243.1 J 2.22.10 2.89.10 2.156.10 2,223.10 2.43.11 2.110.11 2.177.11 2.244.11 2.23.10 2.90.10 2.157.10 2.224.10 2.44.11 2.111.11 2.178.11 2.245.11 2.24.10 2.91.10 2.158.10 2.225.10 2.45.11 2.112.11 2.179.11 2.246.11 2.25.10 2.92.10 2.159.10 2.226.10 2.46. Π 2.113.Π 2.180.1 】 2.247.1】 2.26.10 2.93.10 2.160.10 2.227.10 2.47.11 2.114.11 2.181.11 2.1.12 2.27.10 2.94.10 2.161.10 2.228.10 2.48.11 2.115.11 2.182.11 2.2.12 2.28.10 2.95.10 2.162.10 2.229.10 2.49.11 2.116.11 2.183.11 2.3.12 2.29.10 2.96.】0 2.163.10 2.230.10 2.50.11 2.117.11 2.184.11 2.4.12 2.30.10 2.97.10 2.164.10 2.231.]〇 2.51.11 2.118.11 2.185.11 2.5.12 2.31.10 2.98.10 2.165.10 2.232.10 2.52.11 2.119.11 2.186.11 2.6.12 2.32.10 2.99.10 2.166.10 2.233.10 2.53.11 2.120.11 2.187.11 2.7.12 2.33.10 2.100.10 2.167.10 2.234.10 2.54.11 2.121.11 2.188.11 2.8.12 2.34.10 2,101,10 2.168.10 2.235.10 2.55.11 2.Ι22.Ι1 2.IS9.11 2.9.12 2.35.10 2.102.10 2.169.10 2.236.10 2.56.11 2.123.11 2.190.11 2.10.12 2.36.10 2.103.10 2.170.10 2.237.10 2.57.11 2.124.11 2.191.1】 2.11.12 2.37.10 2.104.10 2.171.10 2.238.10 2.58.11 2.125.11 2.192.11 2.12.12 2.38.10 2.105.10 2.172.10 2.239.Ϊ0 2.59.11 2.J26.1J 2.193.】1 2.13.12 2.39.10 2.106.10 2.173.10 2.240.10 2.60.11 2.127.11 2.194.11 2.14.12 2.40.10 2.107.10 2.174.10 2.241.10 2.61.11 2.128.11 2.195.11 2.15.12 2.43.10 2.108.10 2.175.10 2.242.10 2.62.11 2.129.11 2.196.11 2.16.12 2.42. JO 2.109.JO 2ΑΊ6Λ0 2.243.10 2.63.11 2.130.11 2.197.11 2.17.12 2.43.10 2.110.10 2.177.10 2.244.10 2.64.11 2.131.Π 2.198.11 2.18.12 2.44.10 2.111.10 2.178.10 2.245.10 2.65.11 2.132.11 2.199.11 2.19.12 2.45.10 2.112.10 2.179.10 2.246.10 2.66.11 2.133.11 ' 2.200.11 2.20.12 2.46.10 2.113.10 2.180.10 2.247.10 2.67.11 2.134.11 2.201.11 2.21.12 2.47.10 2.114.10 2.181.10 2.1.11 2.68.11 2.J35.II 2.202. Π 2.22.12 2.48.10 2.115.10 2.182.10 2.2.11 2.69.11 2.136.11 2.203. Π 2.23.12 2.49.10 2.116.10 2.183.10 2.3.11 2.70.11 2.137.11 2.204.11 2.24.12 2.50.10 2.Π7.10 2.184.10 2.4.11 2*71.11 2.138J1 2.205.11 2.25.12 2.51.10 2.118,10 2.185.10 2.5.11 2.72.11 2.339.J1 2.206. Π 2.26.12 2.52.10 2.119.10 2.186.10 2.6.11 2.73.11 2.140.11 2.207.11 2.27.12 2.53.10 2.120.10 2.187.10 2.7.11 2.74.11 2.141.11 2.208.11 2.28.12 2.54.10 2.121.10 2.188.10 2.8.11 2.75.11 2.142.1】 2.209.11 2.29.12 2.55.10 2.122.10 2.189.)0 2.9.]] 2.76.11 2.143.11 2.210.11 2.30.12 2.56.10 2.123.10 2.190.10 2.10.11 2.77.11 2.144.11 2.211.11 2.31.12 2.57.10 2.124.10 2.191.10 2.11.11 2.78.11 2.145.11 2.212.11 2.32.12 2.58.10 2.125.10 2.192.10 2.12.11 2.79.11 2.146.11 2.213.11 2.33.12 2.59.10 2.126.10 2.193.10 2.13.11 2.80.11 2.147.11 2.214.11 2.34.12 2.60.10 2.127.10 2.194.10 2.14.11 2.81.Π 2.148.11 2.215.11 2.35.12 2.61.10 2.128.10 2.195.10 2.15.11 2.82.11 2.149.11 2.216.11 2.36.12 2.62.10 2.129.10 2.196.10 2.16.11 2.83.11 2.150.11 2.217J1 2.37.12 2.63.10 2.130.10 2.197.10 2.17.11 2.84.11 2.151.11 2.218,11 2.38.12 2.64.10 2.131.10 2.198.10 2.18.11 2.85.11 2.152.11 2.219.11 2.39.12 2.65.10 2.132.10 2.199.10 2.19.11 2.86.11 2.153.11 2.220.11 2.40.12 2.66.10 2.133.10 2.200.10 2.20.11 2.87.11 2.154.11 2.221.11 2.41.12 2.67.10 2.134.10 2.201,10 2.21.11 2.88.11 2.155.J1 2.222.11 2.42.12 2.68.10 2.135.10 2.202.10 2.22.1】 2.89. Π 2.156.11 2.223.11 2.43.12
-348- (345)1362934
2.44.12 2.111.12 2.178.12 2.245.12 2.65.13 2.132.13 2.199.13 2.19.14 2.45.12 2.1J2.12 2.J79.J2 2.246.12 2.66.13 2.133.13 2.200.13 2.20.14 2.46.12 2.113.12 2.180.12 2.247.12 2.67.13 2.134.13 2.201.13 2.21.14 2.47.12 2.114.12 2.181.12 2.1.13 2.68.13 2.135.13 2.202.13 2.22.14 2.48.12 2.115.12 2.182.12 2.2.)3 2.69.13 2.136.13 2.203.13 2.23.14 2.49.12 2.116.12 2.183.12 2.3.)3 2.70.13 2.137.13 2.204.13 2.24.14 2.50.12 2.117.12 2.184.12 2.4.13 2.71.13 2.138.13 2.205.13 2.25.14 2.5】.12 2.118.)2 2J85.12 2.5.13 2.72.13 2.139.13 2.206.13 2.26.14 2.52.12 2.119.12 2.186.12 2.6.13 2.73.13 2.140.13 2.207.13 2.27.14 2.53.12 2.120.12 2.187.12 2.7.13 2.74.13 2.141.13 2.208.13 2.28.14 2.54.12 2.121.12 2.188J2 2.8.13 2.75.13 2.142.13 2.209.13 2.29.14 2.55.12 2.122.12 2.189.12 2.9.13 2.76.13 2.143.13 2.210.13 2.30.14 2.56.12 2.123.12 2.190.12 2.10.13 2.77.13 2.144.13 2.211.13 2.31.14 2.57.32 2.J24.12 2.19J.J2 2.Π.13 2.78.13 2.145.13 2.212.13 2.32.14 2.58.12 2.125.12 2.192.12 2.12.13 2.79.13 2.146.13 2.213.13 2.33.14 2.59.12 2.126.12 2.193.12 2.13.13 2.80.13 2.147.13 2.214.13 2.34.14 2.60.12 2.127.12 2.194.12 2.14.13 2.81.13 2.148.13 2.215.13 2.35.14 2.61.12 2.128.12 2.195.12 2.15.13 2.82.13 2.149.13 2.216.13 2.36.14 2.62.12 2.129.12 2.196.12 2.16.13 2.83.13 2.150.13 2.217J3 2.37.14 2.63.)2 2J30.12 2.397.12 2.17.13 2.84.13 2.151.13 2.218.13 2.38.14 2.64.12 2.131.12 2.198.12 2.18.13 2.85.13 2.152.13 2.219.13 2.39.14 2.65.12 2.132.12 2.199.12 2.19.13 2.86.13 2.153.13 2.220.13 2.40.14 2.66.12 2.133.12 2.200.12 2.20.13 2.87.13 2.154.13 2.22U3 2.41.14 2.67.12 2.134.12 2.201.12 2.21.13 2.88.13 2.155.13 2.222.13 2.42.14 2.68.12 2.135.12 2.202.12 2.22.13 2.89.13 2.156.13 2.223.13 2.43.14 2.69.12 2.136.12 2.203.12 2.23.13 2.90.13 2.157.13 2.224.13 2.44.14 2.70.12 2.137.12 2.204.12 2.24.13 2.91.13 2.158.13 2.225.13 2.45.14 2.71.12 2.138.12 2.205.12 2.25.13 2.92.13 2.159.13 2.226.13 2.46.14 2.72.12 2.139.12 2.206.12 2.26.13 2.93.13 2.160.13 2.227.13 2.47.14 2.73.12 2.140.12 2.207.12 2.27.13 2.94.13 2.161.13 2.228.13 2.48.14 2.74.12 2.141.12 2.208.12 2.28.13 2.95.13 2.162.13 2.229.13 2.49.14 2.75.12 2.142.12 2.209.12 2.29.13 2.96.13 2.163.13 2,230.13 2.50.14 2.76.12 2.143.12 2.210.12 2.30.13 2.97.13 2.164.13 2.231.13 2.51.14 2.77.12 2.144.12 2.211.12 2.31.13 2.98.13 2.165.13 2.232.13 2.52.14 2.78.12 2.145.12 2.212.12 2.32.13 2.99.13 2.166.13 2.233.13 2.53.14 2.79.12 2.146.12 2.213.12 2.33.13 2.100.13 2.167.13 2.234.13 2.54.14 2.80.12 2.147.12 2.214.12 2.34.13 2.101.13 2.168.13 2.235.13 2.55.14 2.81.12 2.148.12 2.215.12 2.35.13 2.102.13 2.169.13 2.236.13 2.56.14 2.82.12 2.149.12 2.216.12 2.36.13 2.103.J3 2.I70J3 2.237.13 2.57.14- 2.83.12 2.150.12 2.217.12 2.37.13 2.104.13 2.171.13 2.238.13 2.58.14 2.84.12 2.151.12 2.218.12 2.38.13 2.105.13 2.172.13 2.239.13 2.59.14 2.85.12 2.152.12 2.219.12 2.39.13 2.106.13 2.173.13 2.240.13 2.60.14 2.86.12 2.153.12 2.220.12 2.40.13 2.107.13 2.174.13 2.241.13 2.61.14 2.87.12 2.154.12 2.221.12 2.41.13 2.108.13 2.175.13 2.242.13 2.62.14 2.88.12 2.155.12 2.222.12 2.42.13 2.109.13 2.176.13 2.243J 3 2:63.14 2.89.12 2.156.12 2.223.12 2.43.13 2.110.13 2.177.13 2.244.13 2.64.14 2.90.12 2.157.12 2.224Ί2 2.44.13 2.111.13 2.178.13 2.245.13 2.65.14 2.91.12 2.158.12 2.225.12 2.45.13 2.112.13 2.179.13 2.246.13 2.66.14 2.92.12 2.159.12 2.226.12 2.46.13 2.113.13 2.180.13 2.247.13 2.67.14 2.93.12 2.160.12 2.227.12 2.47.13 2.114.13 2.181.13 2.1.14 2.68.14 2.94.12 2.161.12 2.228.12 2.48.13 2.115.13 2.182.13 2.2.14 2.69.14 2.95.12 2.162.12 2.229.12 2.49.13 2.116.13 2.183.13 2.3.14 2.70.14 2.96.12 2.163.12 2.230.12 2.50.13 2.117.13 2.184.13 2A14 2.71.14 2.97.12 2,164.12 2.231.12 2.51.13 2.118.13 2.185.13 2.5.14 2.72.14 2.98.12 2.165.12 2.232.12 2.52.13 2.119.13 2.186.13 2.6.14 2.73.14 2.99.12 2.166.12 2.233.12 2.53.13 2.120.13 2.187.13 2.7.14 2.74.14 2.300.12 2Λ61Λ2 2.234.32 2.54.33 2.121.13 2.188.13 2.8.14 2.75.14 2.101.12 2.168.12 2.235.12 2.55.13 2.122.13 2.189.13 2.9.14 2.76.14 2.102.12 2.169.12 2.236.12 2.56.13 2.123.13 2.190.13 2.10.14 2.77.14 2.103.12 2.170.12 2.237.12 2.57.13 2.124.13 2.191.13 2.11.14 2.78.14 2.104.12 2.171.12 2.238.12 2.58.13 2.125.13 2.192.13 2.12.14 2.79.14 2.105.12 2.172.J2 2.239.12 2.59.13 2.126.13 2.193.13 2.13.14 2.80.14 2.106.32 2.173.12 2.240J2 2.60.13 2.127,13 2.194.13 2.14.14 2.81.M 2.107.J2 2.174.12 2.241.12 2.6M3 2.128.13 2.195.13 2.15.14 2.82.14 2.108.12 2.175.12 2.242.12 2.62.13 2.129.13 2.196.13 2.16.14 2.83.14 2.109.12 2.176.12 2.243.12 2.63.13 2.130.13 2.197.13 2.17.14 2.84.14 2.Π0.12 2.177.12 2.244.12 2.64.13 2.131.13 2.198.13 2.18.14 2.85.14
-349- (346)1362934
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2.133.109 2,200.109 2.247.108 2.67.109 2.134.109 2.201.109 2.1.109 2.68.109 2.135.109 2.202.109 2.2.109 2.69.109 2.136.109 2.203.109 2.3.109 2.70.] 09 2.137.109 2.204.109
-393- (390)1362934
2.205.109 2.25. Π0 2.92.110 2.159.110 2.206.109 2.26.110 2.93.110 2.160.】】0 2.207.109 2.27.110 2.94.110 2.161.Π0 2.208.109 2.28.110 2.95.110 2.162.110 2.209.109 2.29.110 2.96.110 2.163.110 2.210.109 2.30.110 2.97.110 2.164.110 2.211.109 2.31.ΠΟ 2.98.110 2.165.Π0 2.212.109 2.32.110 2.99.110 2.166.1 】0 2.213.109 2.33.110 2.100.110 2.167.110 2.214.109 2.34.110 2.101.110 2.168.110 2.215.109 2.35.110 2.102.110 2.169.110 2.216.109 2.36.J10 2.103.110 2.170.110 2.2】7.】09 2.37.110 2.104.110 2.171.110 2.218.109 2.38.110 2.105.110 2.172.110 2.219.109 2.39.110 2.106.110 2.173.110 2.220.109 2.40.110 2.107.110 2.174.110 2.221.109 2.41.110 2.108.110 2.175.110 2.222.109 2.42.Π0 2.109.110 2.176.110 2.223.109 2.43.110 2.110.110 2.177.110 2.224.109 2.44.110 2.111.110 2.178.110 2.225.109 2.45.110 .2.112.110 2.179.110 2.226.109 2,46.110 2.113.110 2.180.110 2.227.109 2.47.110 2.114.110 2.181.110 2.228.309 2.48.1 JO 2.115.110 2.182.110 2.229.109 2.49.110 2.116.110 2.183.110 2.230.109 2.50.110 2.117.110 2.184.110 2.231.109 2.51.110 2.118.110 2.185.110 2:232.109 2.52.110 2.Π9.110 2.186.110 2.233.109 2.53.110 2.120.110 2.187.110 2.234.109 2.54.110 2.121.110 2.188.110 2.235.109 2.55.110 2.122.110 2.189.110 2.236,109 2.56.110. 2.123.110 2.190.110 2.237.109 2.57.110 2.124.Π0 2.19】.110 2.238.109 2.58.110 2.125.110 2.192.110 2.239.109 2.59.110 2.126.110 2.193.110 2.240.109 2.60.110 2.127.110 2.194.110 2.241.109 2.61.110 2.128.110 2.195.110 2.242.109 2.62.110 2.129.110 2.196.110 2.243.109 2.63.110 2.130.110 2.197.110 2.244.109 2.64.110 2.131.110 2.198.110 2.245.109 2.65.110 2.132.110 2A99.U0 2.246.109 2.66.110 2.133.110 2.200.110 2.247.109 2.67.110 2.134.110 2.201.110 2.1.110 2.68.110 2.135.110 2.202.110 2.2.110 2.69.110 2.136.110 2.203.110 2.3.110 2.70.110 2.137.110 2.204.110 2.4.110 2.71.110 2.138.110 2.205.110 2.5.110 2.72.110 2.139.110 2.206.110 2.6.110 2.73.110 2.140.110 2.207.110 2.7.110 2.74.110 2.141.110 2.208.110 2.8.110 2.75.110 2.142.110 2.209.110 2.9.110 2.76.110 2.143.110 2.210.Π0 2.10.110 2.77.110 2.144.110 2.211.110 2.11.110 2.78.110 2.145.110 2.212.110 2.12.110 2.79.110 2.146.110 2.213.110 2.13.110 2.80.110 2.147.Π0 2.214.110 2.14.110 2.81.110 2.148.110 2.215.110 2.15.110 2.82.110 2.149.110 2.216.110 2.16.Π0 2.83.110 2.150.110 2.217.110 2.17.110 2.84.1 ]〇 2.151.110 2.218.110 2.18.110 2.85.110 2.152.110 2.219.Π0 2.19.110 2.86.110 2.153.110 2.220.110 2.20.110 2.87.110 2.154.110 2.221.110 2.21.110 2.88.110 2.155.110 2.222.110 2.22.110 2.89.110 2.156.110 2.223.110 2.23.] 10 2.90.110 2.157.110 2.224.110 2.24,110 2.91.110 2.158.Π0 2.225.]】0 2.226.110 2.46.111 2.113.111 2.180.111 2.227.110 2.47. Π1 2-114.1】] 2.181.111 2.228.110 2.48.111 2.115.】】1 2.182.111 2.229.】10 2.49.111 2.116.111 2.183.111 2,230.)10 2.50.ΠΙ 2.117.111 2.184.]]] 2.231.110 2.51.Ill 2.118.111 2.185. "1 2.232.110 2.52.111 2.119.111 2.186.1 Π 2.233.110 2.53.111 2.120.Π1 2.187.111 2.234.110 2.54.111 2.121.111 2.188.111 2.235.110 2.55.111 2.122.Π1 2.)89.111 2.236.110 2.56.111 2.123.111 2.190.111 2.237.110 2.57.11] 2.124.Π1 2.191.川 2.238.110 2.58.111 2.125.111 2.192.111 2.239.110 2.59.111 2.126.111 2.193.111 2.240.110 2.60.111 2.127.111 2.194.111 2.241.110 2.61.111 2」28.111 2.195.111 2.242.110 2.62.111 2.129.111 2.196.111 2.243.110 2.63.111 2.130.111 2.197.111 2.244.110 2.64.111 2.131.Ill 2.198.111 2.245.110 2.65.111 2.132.111 2.199.1 Π 2.246.110 2.66.111 2.133.111 2.200.111 2.247.110 2.67.111 2.134.111 2.201.111 2.1.111 2.68.111 2.135.111 2.202.111 2.2.111 2.69.111 2.136.111 2.203.Γ11 2.3.111 2.70.1 】1 2.137.111 2.204.111 2.4.111 2.71.111 2.138.111 2.205.111 2.5.111 2.72.111 2.139.11J 2.206.111 2.6.J11 2.73.111 2.140.111 2.207.111 2.7.111 2.74.1 Π 2.141.Ill 2.208.1 】1 2.8.111 2.75.111 2.142.111 2.209.111 2.9.111 2.76.111 2.143.111 2.210.111 2.10.111 2.77.111 2.144.11.1 2.211.111 2.11.111 2.78.111 2.145.111 2.212.111 2*12.111 2.79.111 2.146.111 2.213.111 2.13.111 2.80.111 2.147.111 2.214.111 2.14.111 2.81.111 2.148.111 2.215.111 2.15.111 2.82.111 2.149.111 2.216.111 2.16.111 2.83.111 2.150.111 2.217.111 2.17.111 2.84.1Π 2.151.111 2.218.111 2.18.111 2.85.111 2.152.111' 2.219.1 Π 2.19.111 2.86.111 2.153.111 2.220. Ill 2.20.111 2.87.111 2.154.111 2.221.111 2.21.111 2.88.111 2.155.111 2.222.111 2.22.111 2.89.111 2.156.111 2.223.111 2.23.111 2.90.111 2.157.111 2.224.111 2.24.111 2.91.Ill 2.158.111 2.225.111 2.25.111 2.92.111 2.159.111 2.226.111 2.26.111 2.93.111 2.160.111 2.227.111 2.27.111 2.94.111 2.161.111 2.228.111 2.28.111 2.95.111 2.162.1Π 2.229.111 2.29.111 2.96.1 】1 2.163.111 2.230.111 2.30.111 2.97.1 Π 2.164.111 2.231.111 2.31.111 2.98.111 2.165.111 2.232.111 2.32.1】】 2.99.111 2.166.Π1 2.233.111 2.33.111 2.100.111 2.167.111 2.234.111 2.34.111 2.101.1" 2.168.111 2.235.1 Π 2.35.111 2.102.111 2.169.111 2.236.111 2.36.111 2.103.111 2.170.111 2.237.111 2.37.111 2.104.111 2.171.111 2.238.111 2.38.111 2.105.11] 2.172.111 2.239.111 2.39.111 2.106.1 Π 2.173.111 2.240.111 2.40.111 2.107.111 2.174.111 2.241.111 2.41.1 ]1 2.108J11 2.175.111 2.242.111 2.42.11】 2.109.1 ]1 2.176.111 2.243.1 " 2.43.11】 2.110.111 2.177.1Π 2.244.Π1 2.44.111 2.111.111 2.178.111 2.245.111 2.45.111 2.112.1Π 2.179.111 2.246.111 ⑧ (391)1362934
2.247.1 Π 2.67.1 J2 2.134.112 2.201.112 2.1.112 2.68.112 2.135.112 2.202.112 2.2.112 2.69. η 2 2.136.112 2.203.112 2.3.112 2.70.112 2.137.112 2.204.112 2.4.112 2.71.112 2.138.112 2.205.112 2.5.112 2.72.112 2.139·"2 2.206.112 2.6.112 2.73.112 2.140.112 2.207.112 2.7.112 2.74.112 2.141.112 2.208.112 2.8.112 2.75.112 2.142.112 2.209.112 2.9.112 2.76.112 2.143.112 2.210.112 2.10.1J2 2.77.112 2.144.112 2.211.112 2.Π.112 2.78. Π 2 2.J45.112 2.212.112 2.12.112 2.79.112 2.146.112 2.213.Π2 2.13.112 2.80.112 2.147.Π2 2.214.112 2.14.112 2.81.112 2.148.112 2.215.112 2.15.Π2 2.82,112 2.149.112 2.216.112 2.16.112 2.83.112 2.150.112 2.217.112 2.17.112 2.84.112 2.151.112 2.218.112 2.18.112 2.85.112 2.152.112 2.219.112 2.19.112 2.86.112 2.153.112 2.220.112 2.20.112 2.87.112 2.154.112 2.221.112 2.21.112 2.88.112 2.155.112 2.222.1 】2 2.22.112 2.89.112 2.156.】12 2.223.112 2.23.112 2.90.112 2.157.Π2 2.224.112 2.24.112 2.91.112 2.158.112 2.225.112 2.25.112 2.92.112 2.159.112 2.226.112 2.26.112 2.93.112 2.160.112 2.227.112 2.27. Π 2 2.94.112 2.161.112 2.228.112 2.28.112 2.95.112 2.162.112 2.229.112 2.29.112 2.96.112 2.163.112 2.230. Π 2 2.30.112 2.97. Π 2 2.164.112 2.231.112 2.31.112 2.98.112 2.165.112 2.232.112 2.32.112 2.99.112 2J66.112 2.233.112 2.33.112 2.100.112 2.167.112 2.234.112. 2.34.112 2.101.112 2.168.112 2.235.112 2.35:1 】2 2.102.112 2.169.112 2.236.112 2.36.112 2.103.112 2.170.112 2.237.112 2.37.112 2.104.112 2.171.112 2.238.112 2.38.112 2.105.112 2.172.112 2.239.112 2.39.112 2.106.112 2.173.112 2.240.112 2.40.112 2.107.112 2.174.112 2.24】.112 2.41.112 2.108.112 2.175.112 2.242.112 2.42.112 2.109.112 2.176.112 2.243.112 2.43.112 2.110.112 2.177.112 2.244.112 2*44.112 2.111.112 1178.112 2.245.112 2.45.112 2.112.112 2.179.112 2.246.112 2.46. Π 2 2.113.112 2.180.Π2 2.247.112 2.47.112 2.114.112 2.181.112 2.1.113 2.48.112 2.115.112 2.182.112 2.2.113 2.49.112 2.116.112 2.183.112 2.3.113 2.50. Π 2 2.117.112 2.184.112 2.4.113 2.51.112 2.118.112 2.185.112 2.5.113 2.52.112 2.119.112 2.186.112 2.6.113 2.53.112 2.120.112 2.187.112 2.7.113 2.54.112 2.121.112 2.188.112 2.8.113 2.55.112 2.122.Π2 2.189.112 2.9.113 2.56.112 2.123.112 2.190.112 2.10.113 2.57.112 2.124.112 2.19].Π2 2.11.113 2.58.112 2.125.Π2 2.192.Π2 2.12.113 2.59.112 2.126.1)2 2.193.112 2.13.113 2.60.112 2.127.112 2.194.】12 2.14.113 2.61.112 2.128.112 2.195.112 2.15.113 2.62.112 2.129.112 2.196.112 2.16.113 2.63.112 2.130.112 2.197.112 2.17.113 2.64.112 2.131.112 2.198.112 2.18.113 2.65.112 2.132.Π2 2.199.112 2.Ι9.Π3 2.66.112 2.133.112 2.200.112 2.20.113 2.21.113 2.88. Π 3 2.155.113 2.222.113 2.22.113 2.89.113 2.156.113 2.223.113 2.23.113 2.90. Π 3 2.157.Π3 2.224.113 2.24.113 2-91.113 2.158.113 2.225.113 2.25.113 2.92.113 2.159.Π3 2.226.113 2.26.113 2.93.113 2.160.113 2.227-113 2.27.113 2.94.113 2.)61.1)3 2.228.Π3 2.28. !13 2.95.113 2.162.113 2.229.113 2.29.113 2.96.113 2.163.113 2.230.113 2.30.113 2.97.113 2.164.113 2.231.113 2.31.113 2.98.113 2.165.113 2.232.113 2.32.113 2.99.113 2.166.113 2.233.113 2.33.Π3 2.100.113 2.167.113 2.234.113 2.34.113 2.101.113 2.168.Π3 2.235.113 2.35. Π 3 2.102.113 2.169.113 2.236.113 2.36.113 2.103.113 2.170.113 2.237.113 2.37.113 2.104.113 2.171.113 2.238.113 2.38.113 2.105.113 2.172.113 2.239.1 J3 2.39.113 2.106.113 2.173.113 2.240.113 2.40.113 2.107.113 2.174.113 2.241:113 2.41.113 2.108.113 2.175.113 2.242.113 2.42.113 2.109.113 2.176.113 2.243.113 2.43.113 2.110.J13 2.177.113 2.244.113 2.44.113 2.111.113 2.178.113 2.245.113 2.45. Π 3 2.112.Π3 2.179.113 2.246.113 2.46.113 2.113.113 2.180.113 2.247.113 2.47.113 2.114.113 2.181.113 2.1.114 2.48.113 2.115.113 2.182.113 2.2.114 2.49.113 2.116.113 2.183.113 2.3.114 2.50.113 2.117.113 2.184.113 2.4.114 2.51.113 2.118.113 2.185.113 2.5. J14 2.52.113 2.119.113 2.186.113 2.6.114 2.53.Π3 2.120.113 2.187.113 2.7.114 2.54.113 2.Ϊ2Ι.113 2.188.113 2.8.114 2.55.113 2.122.113 2.189.Π3 2.9.114 2.56.113 2.123.113 2.190.113 2.10.114 2.57.113 2.124.113 2.191.113 2.11.114 2.58.113 2.125.113 2.192.113 2.12.114 2.59.113 2.126.113 2.193.113 2.13.114 2.60.113 2.127.113 2.194.113 2.14.114 2.61.113 2.128.113 2.195.113 2.15.114 2.62.113 2.129.113 2.196.113 2.16.114 2.63.] 13 2.130.113 2.197.113 2.17.114 2.64.113 2.131.113 2.198.113 2.1S.114 2.65.113 2.132.113 2.199.113 2.19.114 2.66.113 2.133.113 2.200.113 2.20.114 2.67.113 2.134.Π3 2.201.113 2.21.114 2.68.113 2.135.113 2.202.113 2.22.114 2.69.113 2.136.113 2.203.113 2.23.114 2.70.113 2.137.】13 2.204.113 2.24.114 2.71.113 2.138.113 2.205.113 2.25.114 2.72.113 2.139.J 13 2.206.113 2.26.114 2.73.113 2.140.113 2.207.113 2.27.114 2.74.113 2.141.113 2.208.113 2.28.114 2.75.113 2.142.] 13 2.209.113 2.29.114 2.76.113 2.143.113 2.210.113 2.30.114 2.77.113 2.144.113 2.211.113 2.31.114 2.78.113 2.145.113 2.212.113 2.32.114 2.79.113 2.146.113 2.213.Π3 2.33.114 2.80.113 2.147.113 2.214.1 ]3 2.34.114 2.81.113 2.148.113 2.215.113 2.35.114 2.82.113 2.149.113 2.216.113 2.36.114 2.83.113 2.J50.113 2.217.113 2.37.114 2.84.113 2.151.113 2.218.113 2.38.114 2.85.113 2.152.113 2.219.113 2.39.114 2.86.113 2.153.113 2.220.113 2.40.114 2.87.113 2.154.113 2.221.113 2.41.114
-395- (392)1362934
2.42.114 2.109-114 2.176.114 2.243.114 2.63.115 2.130.115 2.197.Π5 2.17.116 2.43.114 2.110.114 2.177.114 2.244.114 2.64.115 2.131.Π5 2.198.115 2.18.Π6 2.44.] 14 2.1Π.114 2.178.114 2.245.114 2.65.115 2.132.115 2.199.115 2.19.116 2.45.114 2.112.114 2.179.114 2.246.Π4 2.66.115 2.133.115 2.200.115 2.20.116 2.46.114 2.113.114 2.180.Π4 2.247.114 2.67.115 2.134.115 2.201.115 2.21.116 2.47,114 2.114.114 2.181.114 2.1.115 2.68.115 2.135.115 2.202.115 2.22.116 2.48.114 2.115.114 2.182.114 2.2.115 2.69.115 2.136.115 2.203.115 2.23.116 2.49.114 2.116.114 2.183.114 2.3.115 2.70.115 2.137.115 2.204.115 2.24.116 2.50.114 2.117.114 2.184.114 2.4.115 2.71.115 2.138.115 2.205.115 2.25.116 2.51.114 2.1J8.114 2.185.114 2.5.115 2.72.115 2.139.Π5 2.206.115 2.26.116 2.52.114 2.119.114 2.186.114 2.6.115 2.73.115 2.140.115 2.207.115 2.27.116 2.53.1 J4 2.120.114 2.187.114 2.7.115 2.74.115 2.141.115 2.208.115 2.28.116 2.54.114 2.121.114 2.188.114 2.8.115 2.75.115 2.142.115 2.209.115 2.29.116 2.55.114 2.122.114 2.189.Π4 2.9.115 2.76.115 2.143.】15 2.2J0.115 2.30. 2.56.114 2.123.114 2.190.114 2.10.1J5 2.77.115 2.144.115 2.211.115 2.31.116 2.57.114 2.124.114 2.191.114 2.11.115 2.78.115 2.145.115 2.212.115 2.32.116 2.58.114 2.125.114 2.192.114 2.12.115 2.79.115 2.146.115 2.213.115 2.33.116 2.59.114 2.126.114 2.193.114 2.13.Π5 2.80.115 2.147.115 2.214.115 2.34.116 2.60.114 2.127.114 2.194.114 2.14.115 2.81.115 2.148.115 2.215.115 2.35.116 2.61.114 2.128.114 2.195.114 2.15.115 2.82.115 2.149.115 2.216.115 2.36.116 2.62. Π 4 2.129.114 2.196.114 '2.16.115 2.83*115 2.150.115 2.217.115 237.116 2.63.114 2.130.114 2.197.114 2.17.115 2.84.115 2.151.115 2.218.115 2.38.116 2.64.114 2.131.114 2.198.114 2.18.115 2.85.115 2.152.115 2.219,115 2.39.116 2.65.114 2.132.114 2.199.Π4 2.19.115 2.86.115 2.153.115 2:220.115 2.40.116 2.66.114 2.133.114 2.200.114 2.20.115 2,87.115 2.154.115 2.221.115 2.41.116 2.67.114 2.134.114 2.201.114 •2.21.Π5 2.88.115 2.155.115 2.222.115 2.42.11-6 2.6S.I14 2.135.114 2.202.114 2.22. II5 2.89.115 2.156.115 2.223. J15 2.43.116 2.69.114 2.136.114 2.203.114 . 2.23.115 2.90.115 2.157.115 2.224.115 2.44.116 2.70.114 2,137.114 2.204.114 2.24.115 2.91.315 2.158.Π5 2.225.115 2.45.116 2.71.114 2.138.114 .2.205.114 2.25.115 2.92.115 2.159.115 2.226.115 2.46.116 2.72.114 2.139.114 •2.206.114 2.26.115 2.93.115 2.160.115 2.227.115 2.47.116 2.73.114 2.140.114 2.207.Π4 2.27.115 2.94.115 2.161.115 2.228.115 2.48.116 2.74.114 2.141.114 2.208.114 2.28.115 2.95.115 2.162.115 2.229.115 2.49. Π 6 2.75.114 2.142.114 2,209.114 2.29.115 2.96.115 2.163.115 2.230.115 2.50. Π 6 2.76.114 2.143.114 2.210.114 2.30.115 2.97.115 2.164.115 2.231.115 2.51.116 2.77.114 2.144.114 2.211.114 2.31.Π5 2.98.115 2.165.115 2.232.115 2.52. Π 6 2.78.114 2.145.114 2.212.114 2.32.115 2.99.115 2.166.115 2.233.115 2.53.116 2.79.114 2.146·】14 2.213.114 2.33.115 2,100.115 2.167.115 2.234.115 2.54.116 2.80.114 2.147.114 2.214.114 2.34.115 2.101.115 2.168.115 2.235.115 2.55.116 2.SL114 2.I48.M4 2.215.Π4 2.35.115 2A02.U5 2.169.1 】5 2.236J15 2.56.116 2.82.114 2.149.114 2.216.114 2.36.115 2.103.115 2.170.115 2.237.115 2.57.116 2.83.114 2.150.114 2.217.114 2.37.115 2.104.115 2.171.115 2.238.115 2.58.116 2.84.114 2.151.114 2.218.114 2.38.115 2.105.115 2.172.115 2.239.115 2.59.116 2.85.114 2.152.114 2.219.114 2.39.115 2.106.115 2.173.115 2.240.115 2.60.116 2.86.114 2.153.114 2.220.114 2.40.115 2.107.115 2.174.115 2.241.115 2.61.116 2.87.114 2.154.114 2.221.114 2.41.115 2.108.115 2.175.115 2.242.115 2.62.116 2.88.114 2.155.114 2.222.114 2.42.115 2.109.115 2.176.115 2.243.115 2.63.116 2.89.114 2.156.114 2.223.114 2.43.115 2.110.115 2.177.115 2.244.115 2.64.116 2.90.114 2.157.114 2.224.114 2.44.115 2.111.115 2.178.115 2.245:115 2.65.116 2.91.114 2.158.114 2.225. Π 4 2.45.115 2,112.115 2.179.115 2.246.1 ]5 2.66.116 2.92.114 2,159.114 2.226.114 2.46.115 2.113.115 2.180.115 2.247.115 2.67.116 2.93.114 2.160.114 2.227.114 2.47.115 2.114.115 2.181.115 2.1.116 2.68.116 2.94.114 2.161.114 2.228.114 2.48.115 2.115.115 2AS2.U5 2.2.116 2.69.U6 2.95.114 2.162.114 2.229.114 2.49.115 2.116.115 2.183.115 2.3.116 2.70.116 2.96.114 2.163.114 2.230.114 2.50.115 2.117.115 2.184.115 2.4.116 2.71.116 2.97.114 2.164.114 2.231.114 2.51.115 2.Π8.115 2.185.115 2.5.116 2.72.116 2.98.114 2.165.114 2.232.114 2.52.115 2.119.115 2.186.115 2.6.116 2.73.116 2.99.114 2.166.114 2.233.114 2.53.115 2.120,115 2.187.115 2.7.116 2.74. J16 2.100.114 2.167.114 2.234.114 2.54.115 2.121.115 2.188.115 2.8.116 2.75.116 2.101.114 2.168.114 2.235.114 2.55.115 2.122.115 2.189.115 2.9.116 2.76.116 2.102.114 2.169.114 2.236.114 2.56.115 2.123.115 2.190.115 2.10.116 2.77.116 2.103.114 2.170.114 2.237.114 2.57.115 2.124.115 2.191.115 2.11.116 2.78.116 2.104.114 2.171.114 2.238.114 2.58.Π5 2.125.115 2.192.115 2.12.116 2.79.116 2.105.114 2.172.114 2.239.114 2.59,115 2.126.115 2.193.Π5 2.13.116 2.80.116 2.106.114 2.173.H4 2.240.114 2.60.Π5 2.127.115 2.194.115 2.14.116 2.81.116 2.107.114 2.174.114 2.241.114 2.61.115 2.128.115 2.195.115 2.15.116 2.82.116 2.108.114 2.175.114 2.242.114 2.62. Π 5 2.129.115 2.196.115 2.16.116 2.83.116
-396- (393)1362934 2.84.116 2.151.116 2.218.116 2.38.117 2.105.117 2.172.117 2.239.1 】7 2.59.1 2.Β5.136 2.152.116 2.219.Π6 2.39.117 2.106.117 2.173.117 2.240.1)7 2.60.1 2.86.116 2.153.116 2.220.116 2.40.117 2.107.117 2.174.117 2.241.117 2.61.1 2.87.116 2.154.116 2.221.116 2.41.117 2.108.117 2.175.117 2.242.117 2.62.1 2.88.116 2.155.116 2.222.116 2.42.117 2.109.Π7 2.176.Π7 2.243.] Π 2.63.1 2.89.116 2.156.116 2.223.116 2.43.117 2.110.117 2.177.117 2.244.117 2.64.1 2.90.116 2.157.116 2.224.116 2.44.117 2.111.117 2.178.117 2.245.117 2.65.1 2.9K116 2.158.116 2.225.116 2.45.117 2.112.117 2.179.117 2.246.117 2.66.1 2.92.116 2.159.116 2.226.116 2.46.117 2.113.117 2.180.117 2.247.117 2.67.1 2.93.116 2.160.116 2.227.116 2.47.117 2.114.117 2.181.117 2.1.118 2.68.1 2.94.116 2.161.116 2.228.116 2.48.117 2.115.117 2.182.117 2.2.118 2.69.1 2.95.116 2.162.116 2.229.116 2.49.117 2.116.117 2.183.117 2.3.118 2.70.1 2.96.116 2.163.116 2.230.116 2.50.117 2.117.117 2.184.117 2.4.118 2.71.1 2.97.116 2.164.Π6 2.231.116 2.51.117 2.118.117 2.185.117 2.5.118 2.72.1 2.98.116 2.165.116 2.232.116 2.52.117 2.119.117 2AS6.U7 2.6.Π8 2.73.1 2.99.116 2.166.116 2.233.116 2.53.117 2.120.117 2.187.117 2.7.118 2.74.1 2.100.116 2.167.116 2.234.116 2.54.117 2.121.117 2.188.117 2.8.118 2.75.1 2.101.116 2.168.116 2.235.116 2.55.117 2.122.117 2.189.117 2.9.118 2.76.1 2.102.116 2.169.116 2.236.116 2.56.117 2.123.117 2.190.117 2.10.118 2.77.1 2.103.116 2.170.Ϊ16 2.237.116 2.57·】Π 2.124.Π7 2.191.117 2.11J18 2.78.1 2.104.116 2.171.116 2.238.116 2.58.117 2.125.117 2.192.117 2.12.118 2.79.1 2.105-116 2.172.116 2.239.116 2.59.117 2.126.117 2.193.117 2.13.118 2.80.1 2.106.116 2.173.116 2.240.116 2.60.117 . 2-127.117 2.194.117 2.14.118 2.S1.1 2.107.116 2.174.116 2.241.116 2.61.117 2.128.117 2.195.117 2.15.118 2.82.1 2.108.116 2.175.116 2.242. Π 6 2.62.117 2.129.117 2.196.117 2.16.118 2.83.1 2.109.116 2.176.116 2.243.116 2.63.117 2.130.117 2.197.117 2.17.118 2.84.1 2.110.116 2.177.116 2.244.116 2.64.117 2.131.117 2.198.117 2.18.118 2.85.1 2.1.11.Π6 2.178.Π6 2.245.116 2.65.117 2.132.117 2.199.117 2.19.118 2.86.1 2.112.116 2.179.116 2.246.116 2.66.117 2.133.117 2.200.117 2.20.118 2.87.1 2.Π3.Π6 2.180.116 2.247,116 2.67.117 2.134.117 2.201.117 2.21.118 2.88.1 2.114.116 2.181.116 2.1.117 2.68.117 2.135.117 2.202.Π7 2.22. Π 8 2.89.1 2.115.116 2.182.116 2.2.117 2.69.117 2.136.117 2.203.117 2.23.118 2.90.1 2.116.116 2.183.116 2.3.117 2.70.117 2.137.117 2.204.117 2.24.118 2.91.1 2.117.116 2.184.116 2.4.117 2.71.117 2.138.117 2.205.117 2.25.118 2.92.1 2.118.116 2.185.116 2.5.117 2.72.117 2.139.117 2.206.117 2.26.118 2.93.1 2.Π9Μ6 2.186.116 2.6.Π7 2.73.]】7 2.J40.I17 2.207.117 2.27.118 2.94.1 2.120.Π6 2.187.116 2.7.117 2.74.117 • 2.141.117 2.208.117 2.28.118 2.95.1 2.121.116 2.188.116 2.8.117 2.75.117 2.142.117 2.209.Π7 2.29.118 . 2.96.1 2.122.116 2.189.116 2.9.117 2.76.117 2.143.117 2.210.117 2.30.118 2.97.1 2.123.116 2.190.116 2.10.117 2.77.117 2.144.117 2.211.117 2.31.118 2.98.1 2.124.116 2.191.116 2.11.117 2.78.117 2.145.117 2.212.117 2.32.118 2.99.1 2.125.116 2.192.116 2.12.117 2.79.117 2.146.117 2.213.117 2.33.118 2.100· 2.126.Π6 2.193.116 2.13.117 2.80.117 2.147.117 2.214.117 2.34.118 2.101. 2.127J16 2.194.116 2.14.117 2.81.117 2.148.117 2.215.117 2.35.118 2.102. 2.128.116 2.195.116 2.15.117 2.82.117 2.149.117 2.216.117 2.36.118 2.103. 2.129.116 2.196.116 2.16.117 2.83.117 2.150.117 2.217.117 2.37.118 2.104· 2.130.116 2.197.116 2.Ι7.1Ι7 2.84.117 2.151.117 2.218J 17 2.3S.US 2.105. 2.131.116 2.198.116 2.18.117 2.85.117 2.152.117 2.219.117 2.39.118 2.106. 2.132.116 2.199.116 2.19.117 2.86.117 2.153.117 2.220.117 2.40. Π 8 2.107. 2.133.116 2.200.116 2.20.117 2.87.117 2.154.117 2.221.117 2.41:118 2.108. 2.134.116 2.201.116 2.21.117 2.88.117 2.155.117 2.222.117 2.42.118 2.109. 2.135.Π6 2.202.116 2.22. η 7 2.89. Π 7 2.156.117 2.223.117 2.43.118 2.110. 2.136.116 2.203.116 2.23.117 2.90.117 2.157.117 2.224.117 2.44.118 2.111· 2.137.116 2.204.116 2.24.117 2.91.117 2.158.117 2.225.117 2.45.118 2.112. 2.138.116 2.205.116 2.25.117 2.92.117 2.159-117 2.226.117 2.46.118 2.113. 2.139.116 2.206.116 2.26.117 2.93.117 2.160.117 2.227.117 2.47.118 2.114. 2.140.116 2.207.116 2.27.117 2-94.117 2.161.117 2.228.117 2.48.118 2.115. 2.141.116 2.208.116 2.28.117 2.95.117 2.162.117 2.229.117 2.49.118 2.116. 2.142.116 2.209.116 2.29.117 2.96.117 2.163.117 2.230.117 2.50.118 2.117. 2.143.116 2.210.116 2.30.117 2.97.117 2.164.117 2.231.117 2.51.118 2.118. 2.144.116 2.211.Π6 2.31.117 2.98.117 2.165.117 2.232.117 2.52.118 2.119. 2.145.Π6 2.212.116 2.32.117 2.99.117 2.166.117 2.233.117 2.53.118 2.120. 2.146.Π6 2.213.116 2.33.1Π 2.100.117 2.167.117 2.234.117 2.54.118 2.121. 2.147.116 2.214.116 2.34.117 2.101.117 2.168.117 2.235.117 2.55.118 2.122. 2.148.116 2.215.116 2.35.117 2,102.117 2.169.117 2.236.1 】7 2.56.118 2.123. 2.149.116 2.2)6.116 2.36.117 2.103.117 2.170.117 2.237.117 2.57.118 2.124. 2.150.116 2.217.Π6 2.37.117 2.104.117 2.171.Π7 2.238.117 2.58.118 2.125. 6 β ΟΟ Β οο 8 Β 8 8 S 8 DD Β 8 8 8 Do Do Do 8 8 S 8 8 8 οο 88888888888888008888888888888888888888888811111111111111111111111111 -397- (394)1362934 2.126.1 2.127.1 2.128.1 2.129.1 2.130.1 2.131.1 2.132.1 2.133.1 2.134.1 2.135.1 2.136.1 2.137.1 2.138.1 2J39.1 2.140.1 2.141.1 2.142.1 2.143.) 2.144.1 2.145.1 2.146.1 2.147.1 2.148·】 2.149.1 2.150.1 2.151.1 2.152.1 2.153.1 2.154.1 2.155.1 2.156.1 2.157.1 2.158.1 2.159.1 2.160.1 2.161.1 2.162.1 2.163.) 2.164.1 2.165.1 2.166.1 2.167.1 2.168.1 2.169.1 2.170.1 2.171.1 2.172.1 2.173.1 2.174.1 2.175.1 2.176.1 2.177.1 2.178.1 2.179.1 2.180.1 2.181.1 2.182.1 2.183.1 2.184.1 2.155.1 2.186.1 2.187.1 2.188.1 2.189.1 2.190.1 2.191.1 2.192.1 2.13.Π9 2.14.119 2.15.119 2.16.119 2.17.119 2.18.119 2.19.119 2.20.119 2.21.119 2.22.119 2.23.119 2.24.119 2.25.119 2.26.119 2.27.119 2.28.119 2.29.119 2.30.119 2.31.119 2.32.119 2.33.119 2.34.119 2.35.119 2.36.119 2.37.119 - 2.38.119 2.39.119 2.40.119 2.41.119 2.42.119 2.43.119 2.44.119 2.45.119 2.46.119 2.47.119 2.48.119 2.49.119 2.50.119 2.51.119 2.52.119 2.53.119 2.54.119 2.55.119 2.56.119 2.57.119 2.58.119 2.59.119 2.60.119 2.61.119 2.62.119 2.63.119 2.64.119 2.65.119 2.66.119 2.67.119 2.68.119 2.69.119 2.70.119 2.71.119 2.72.119 2.73.119 2.74.119 2.75.119 2.76.119 2.77.119 2.78.119 2.79.119 2.193.118 2.194.118 2.195.118 2.196.118 2.197.118 2.198.118 2.199.118
2.200.1 JS 2.201.118 2,202.118 2.203.118 2.204.118 2.205.118 2.206. Π 8 2.207. Π 8 2.208.118
2.209.118 2.2J0.11S 2.211.118
2.212.1 IS 2.213.118 2.214.118 2.215.118
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2.240.200 2.60.201 2.127.201 2.194.201 2.241.200 2.61.201 2.128.201 2.195.201 2.242.200 2.62.20】 2.129.201 2.196.201 2.243.200 2.63.201 2.130.201 2.197.201 2.244.200 2.64.201 2.131.201 2.198.201 2.245.200 2.65.201 2.132.201 2.199.201 2.246.200 2.66.201 2.133.201 2.200.201 2.247.200 2.67.201 2.134.201 2.201.201 2.1.201 2.68.201 2.135.201 2.202.201 2.2.201 2.69.201 2.136.201 2.203.201 2.3.201 2.70.201 2.137.20] 2.204.201 2.4.201 2.71.201 2.138.201 2.205.201 2.5.201 2.72.20] 2.139.201 2.206.201 2.6.201 2.73.201 2.140.201 2.207.201 2.7.201 2.74.201 2.141.201 2.208.201 2.8.201 2.75.201 2.142.201 2.209.201 2.9.201 2.76.20】 2.143.201 2.210.201 2.10.201 2.77.20】 2J44.20J 2.211.20】 2.11.201 2.78.201 2.145.201 2.212.201 2.12.201 2.79.201 2.146.201 2.213.201 2.13.201 2.80.201 2.147.201 2.214.201 2.14.201 2.81.201 2.148.201 2.215.201 2.15.201 2.82.201 2.149.201 2.216.201 2.16.20】 2.83.201 2.150.201 2.217.201 2.17.201 2.84.201 2.151.201 2.218.201 2.18.201 2.85.201 2.152.201 2.219.201 2.19.201 2.86.201 2.153.201. 2.220.201 2.20.201 2.87.201 2.154.201 2.221.201 2.21.201 2.88.201 2.155.201 2.222.201 2.22.201 2.89.201 2.156:201 2.223.201 2.23.201 2.90.201 2.157.201 2.224.201 2.24.201 2.91.201 2.158.201 2.225.201 2.25.201 2.92.201 2.159.201 2.226.201 2.26.201 2.93.201 2.160.201 2.227.201 2.27.201 2.94.20】 2.161.20】 2.228.201 2.28.201 2.95.201 2.162.201 2.229.201 2.29.201 2.96.201 2.163.201 2.230.201 2.30.20】 2.97.201 2.164.201 2.231.201 2.31.201 2.98.201 2.165.201 2.232.201 2.32.201 2.99.201 2.166.201 2.233.201 2.33.201 2.100.203 2.167.201 2.234.201 2.34.201 2.101.201 2.168.201 2.235.201 2.35.201 2.102.201 2.169.201 2.236.201 2.36.201 2.103.201 2.170.201 2.237.201 2.37.201 2.104.201 2.171.201 2.238.201 2.38.201 2.105.201 2.172.201 2.239.201 2.39.201 2.106.201 2.173.201 2.240.201 2.40.201 2.107.20】 2.174.201 2.241.201 2.41.201 2.108.201 2.175.201 2.242.201 2.42.201 2.109.201 2.176.201 2.243.201 2.43.201 2.110.201 2.177.201 2.244.201 2.44.201 2.111.201 2.178.201 2.245.201 2.45.201 2.112.201 2.179.201 2.246.201 2.46.201 2.113.201 2.180.201 2.247.201 2.47.201 2.114.201 2.181.201 2.1.202 2.48.20】 2.1 )5.201 2.182.201 2.2.202 2.49.201 2.116.201 2.183.201 2.3.202 2.50.201 2.117.201 2.184.20】 2.4.202 2.51.201 2.118.201 2.185.201 2.5.202 2.52.201 2.119.201 2.186.201 2.6.202 2.53.201 2.120.201 2.187.201 2.7.202 2.54.20] 2.121.201 2.188.201 2.8.202 2.55.201 2.122.201 2.189.201 2.9.202 2.56.201 2.123.201 2.190.201 2.10.202 2.57.201 2.124.201 2.19】.201 2.11.202 2.58.201 2.125.201 2.192.201 2.12.202 2.59.201 2.126.201 2.193.201 2.13.202 2.14.202 2.81.202 2.148.202 2.215.202 2.15.202 2.82.202 2.149.202 2.216.202 2.16.202 2.83.202 2.150.202 2.217.202 2.17.202 2.84.202 2,151.202 2.218.202 2.18.202 2.85.202 2.152.202 2.219.202 2.19.202 2.86.202 2.153.202 2.220.202 2.20.202 2.87.202 2.154.202 2.221.202 2.21.202 2.88.202 2.155.202 2.222.202 2.22.202 2.89.202 2.156.202 2.223.202 2.23.202 2.90.202 2.157.202 2.224.202 2.24.202 2.91.202 2.158.202 2.225.202 2.25.202 2.92.202 2.159.202 2.226.202 2.26.202 2.93.202 2.160.202 2.227.202 2.27.202 2.94.202 2.161.202 2.228.202 2.28.202 2.95.202 2.162.202 2.229.202 2.29.202 2.96.202 2.163.202 2.230.202 2.30.202 2.97.202 2.164.202 2.231.202 2.31.202 2.98.202 2.165.202 2.232.202 2.32.202 2.99.202 2.166.202 2.233.202 2.33.202 2.100.202 2.167.202 2.234.202 2.34.202 2.101.202 2.168.202 2.235.202 2.35.202 2.102.202 2.169.202 2.236.202 2.36.202 2.103.202 2.170.202 2.237.202 2.37.202 2.104.202 2.171.202 2.238.202 2.38.202 2.105.202 2.172.202 2.239.202 2.39.202 2.106.202 2.173.202 2.240.202 2.40.202 2· 107.202 2.174.202 2.241.202 2.41.202 2.108.202 2.175.202 2.242.202 2.42.202 2.109.202 2.176.202 2.243.202 2.43.202 2.110.202 2.177.202 2.244.202 2.44.202 2. Π 1.202 2.178.202 2.245.202 2.45.202 2.112.202 2.179.202 2.246.202 2.46.202 2.113.202 2.180.202 2.247.202 2.47.202 2.114.202 2.181.202 2.1.203 2.4S.202 2.115.202 2.182.202 2.2.203 2.49.202 2.116.202 2.183.202 2.3.203 2.50.202 2.117.202 2.184.202 2.4.203 2.51.202 2.118.202 2.185.202 2.5.203 2.52.202 2.119.202 2.186.202 2.6.203 2.53.202 2.120.202 2.187.202 2.7.203 2.54.202 2J21.202 2.J 88.202 2.8.203 2.55.202 2.122.202 2.189.202 2,9,203 2.56.202 2.123.202 2.190.202 2.10.203 2.57.202 2.124.202 2.191:202 2.11.203 2.58.202 2.125.202 2.192.202 2.12.203 2.59.202 2.126.202 2.193.202 2.13.203 2.60.202 2.127.202 2.194.202 2.14.203 2.61.202 2.128.202 2.195.202 2.15.203 2.62.202 2.129.202 2.196.202 2.16.203 2.63.202 2 J 30.202 2.197.202 2.17.203 2.64.202 2.131.202 2.198.202 2.18.203 2.65.202 2.132.202 2.199.202 2.19.203 2.66.202 2.133.202 2.200.202 2.20.203, 2.67.202 2.134.202 2.201.202 2.21.203 2.68.202 2.135.202 2.202.202 2.22.203 2.69.202 2.136.202 2.203.202 2.23.203 2.70.202 2.137.202 2.204.202 2.24.203 2.71.202 2.138.202 2.205.202 2.25.203 2.72.202 2.139.202 2.206.202 2.26.203 2.73.202 2.140.202 2.207.202 2.27.203 2.74.202 2.141.202 2.208.202 2.28.203 2.75.202 2.142.202 2.209.202 2.29.203 2.76.202 2.143.202 2.210.202 2.30.203 2.77.202 2.144.202 2,2 Π.202 2.31.203 2.78.202 2.145.202 2.212.202 2.32.203 2.79.202 2.146.202 2.213.202 2.33.203 2.80.202 2.147.202 2.214.202 2.34.203
-436- (433)1362934
2.35.203 2.102.203 2.169.203 2.236.203 2.36.203 2.103.203 2.170.203 2.237.203 2.37.203 2.104.203 2.171.203 2.238.203 2.38.203 2.105.203 2.172.203 2.239*203 2.39.203 2.106.203 2.173.203 2.240.203 2.40.203 2.107.203 2.174.203 2.241.203 2.41.203 2.108.203 2.175.203 2.242.203 2.42.203 2.109.203 2.176.203 2.243.203 2.43.203 2.110.203 2.177.203 2.244.203 2.44.203 2.111.203 2.178.203 2.245.203 2.45.203 2.112.203 2.179.203 2.246.203 2.46.203 2.113.203 2J80.203 2.247.203 2.47.203 2.114.203 2.181.203 2.1.204 2.48.203 2.115.203 2.182.203 2.2.204 2.49.203 2.116.203 2.183.203 2.3.204 2.50.203 2.117.203 2.184.203 2.4.204 2.51.203 2.118.203 2.185.203 2.5.204 2.52.203 2.119.203 2.186.203 2.6.204 2.53.203 2.120.203 2.187.203 2.7.204 2.54.203 2.121.203 2.188.203 2.8.204 2.55.203 2.122.203 2.189.203 2.9.204 2.56.203 2.123.203 2.190.203 2.10.204 2.57.203 2.124.203 2.191.203 2.11.204 2.58.203 2.125.203 2.192.203 2.12.204 2.59.203 2.126.203 2.193.203 2.13.204 2.60.203 2.127.203 2.194.203 2.14.204 2.61.203 2.128.203 2.195.203 2.15.204 2.62.203 2.129.203 2.196.203 2.16.204 2.63.203 2.130.203 2.197.203 2.17-204 2.64.203 2.131.203 2.198.203 2.18.204 2.65.203 2.132.203 2.199.203 2.19.204 2.66.203 2.133.203 2.200.203 2.20.204 2.67,203 2.134.203 2.201.203 2.21.204 2.68.203 2.135.203 2.202.203 2.22.204 2.69.203 2.136.203 2.203.203 2.23.204 2.70.203 2.137.203 2.204.203 2.24.204 2.71.203 2.138.203 2.205.203 2.25.204 2.72.203 2.139.203 2,206·203 2.26.204 2.73.203 2J40.203 2.207.203 2.27.204 2.74.203 2.141.203 2.208.203 2.28.204 2.75.203 2J42.203 2.209.203 2.29.204 2.76.203 2.143.203 2.210.203 2.30.204 2.77.203 2.144.203 2.211.203 2.31.204 2.78.203 2.145.203 2.212.203 2.32.204 2.79.203 2.146.203 2.213.203 2.33.204 2.80.203 2.147.203 2.214.203 2.34.204 2.81.203 2.148.203 2.215.203 2.35.204 2.82.203 2.149.203 2.216.203 2.36.204 2.83.203 2.150.203 2.217.203 2.37.204 2.84.203 2.151.203 2.218.203 2.38.204 2.85.203 2.152.203 2.219.203 2.39.204 2.86.203 2.153.203 2.220.203 2.40.204 2.87.203 2_ 154.203 2.221.203 2.41.204 2.88.203 2.155.203 2.222.203 2.42.204 2.89.203 2.156.203 2.223.203 2.43.204 2.90.203 2.J57.203 2.224.203 2.44.204 2.91.203 2.158.203 2.225.203 2.45.204 2.92.203 2.159.203 2.226.203 2.46.204 2.93,203 2.160.203 2.227.203 2.47.204 2.94.203 2.161.203 2.228.203 2.48.204 2.95.203 2.162.203 2.229.203 2.49.204 2.96.203 2.163.203 2.230.203 2.50.204 2.97.203 2.164.203 2.231.203 2.51.204 2.98.203 2.165.203 2.232.203 2.52.204 2.99.203 2.166.203 2.233.203 2.53.204 2.100.203 2.167.203 2.234.203 2.54.204 2.101.203 2.168.203 2.235.203 2.55.204 2.56.204 2.123.204 2.190.204 2.10.205 2.57.204 2.124.204 2.191.204 2.11.205 2.58.204 2.125.204 2.192.204 2.12.205 2.59.204 2.126.204 2.193.204 2.13.205 2.60.204 2.127.204 2.194.204 2.14.205 2.61.204 2.128.204 2.195.204 2.15.205 2.62.204 2.129.204 2.196.204 2.16.205 2.63.204 2.130.204 2.197.204 2.17.205 2.64.204 2.131.204 2.198.204 2.18.205 2.65.204 2.132.204 2.199.204 2.19.205 2.66.204 2.】33.204 2.200.204 2.20.205 2.67.204 2.134.204 2.201.204 2.21.205 2.68.204 2.135.204 2.202.204 2.22.205 2.69.204 2.136.204 2.203.204 2.23.205 2.70.204 2.137.204 2.204.204 2.24.205 2.71.204 2.138.204 2.205.204 2.25.205 2.72.204 2.139.204 2.206.204 2.26.205 2.73.204 2.140.204 2.207.204 2.27.205 2.74.204 2.141.204 2.208.204 2.28.205 2.75.204 2.142.204 2.209.204 2.29.205 2.76.204 2.143.204 2.210.204 2.30.205 2.77.204 2.144.204 2.211.204 2.31.205 2.78.204 2.145.204 2.212.204 2.32.205 2.79.204 2.146.204 2.213.204 2.33.205 2.80.204 2.147.204 2.214.204 2.34.205 2.83.204 2.148.204 2.215.204 2.35.205 2.82.204 2.149.204 2.216.204 2.36.205 2.83.204 2.150.204 2.217.204 2.37.205 2.84.204 2.151.204 2.218.204 2.38.205 2.85.204 2.152.204 2.219.204 2.39.205 2.86.204 2.153.204 2.220.204 2.40,205 2.87.204 2.154.204 2.221.204 2.41.205 2.88.204 2.155.204 2.222.204 2.42.205 2.89.204 2.156.204 2.223.204 2.43.205 2.90.204 2.157.204 2*224.204 2.44.205 2.91.204 2.158.204 2.225.204 2.45.205 2.92.204 2.159.204 2.226.204 2.46.205 2.93.204 2.160.204 2.227.204 2.47.205 2.94.204 2.161.204 2.228.204 2.48.205 2.95.204 2.162.204 2.229.204 2.49.205 2.96.204 2.163.204 2.230.204 2.50.205 2.97.204 2.164.204 2.231.204 2.51.205 2.98.204 2.165.204 2.232.204 2.52.205 2.99.204 2.166.204 2.233.204 2.53.205 2.100.204 2.167.204 2.234.204 2.54.205 2.101.204 2.168.204 2.235.204 2.55.205 2.102.204 2.169.204 2.236.204 2.56.205 2.103.204 2.170.204 2.237.204 2.57.205 2.104.204 2.171.204 2.238.204 2.58.205 2.105.204 2.172.204 2.239.204 2.59.205 2.106.204 2.173.204 2.240.204 2.60.205 2.107.204 2.174.204 2.241.204 2.61.205 2.108.204 2.175.204 2.242.204 2.62.205 2.109.204 2.176.204 2.243.204 2.63.205 2.110.204 2.177.204 2.244.204 2.64.205 2.111.204 2.178.204 2:245.204 2.65.205 2.112.204 2.179.204 2.246.204 2.66.205 2.113.204 2.180.204 2.247.204 2.67.205 2.114.204 2.181.204 2.1.205 2.68.205 2.115.204 2.182.204 2.2.205 2.69.205 2.116.204 2.183.204 2.3.205 2.70.205 2.117.204 2.184.204 2.4.205 2.71.205 2.118.204 2.185.204 2.5.205 2.72.205 2.119.204 2.186.204 2.6.205 2.73.205 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-437- (434)1362934
2.77.205 2.144.205 2.2 Π.205 2.31.206 2.78.205 2.145.205 2.212.205 2.32.206 2.79.205 2.146.205 2.213.205 2.33.206 2,80.205 2.147.205 2.214.205 2.34.206 2.81.205 2.148.205 2.215.205 2.35.206 2.82.205 2.149.205 2.216.205 2-36.206 2.83.205 2.150.205 2.217.205 2.37.206 2.84.205 2.151.205 2.218.205 2.38.206 2.85.205 2.152.205 2.219.205 2.39.206 2.86.205 2.153.205 2.220.205 2.40.206 2.87.205 2.154.205 2.221.205 2,41,206 2.88.205 2.155.205 2.222.205 2.42.206 2.89.205 2.156.205 2.223.205 2.43.206 2.90.205 2.157.205 2.224.205 2.44.206 2.91.205 2.158.205 2.225.205 2.45.206 2.92.205 2.159.205 2.226.205 2.46.206 2.93.205 2.160.205 2.227.205 2.47.206 2.94.205 2.161.205 2.228.205 2.48.206 2.95.205 2.162.205 2.229.205 2.49.206 2.96.205 2.163.205 2.230.205 2.50.206 2.97.205 2.164.205 2.231.205 2.51.206 2.98.205 2.165.205 2.232.205 2.52.206 2.99.205 2.166.205 2.233.205 2.53.206 2.100.205 2.167.205 2.234.205 2.54.206 2.101.205 2.168.205 2.235.205 2.55.206 2.102.205 2.169.205 2.236.205 2.56.206 2.103.205 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J 63.210 2.210.209 2.30.210 2.97.210 2.164.210 2.211.209 2.31.210 2.98.210 2.165.210 2.212.209 2.32.210 2.99.210 2.166.210 2.213,209 2.33.210 2.100.210 2.167.210 2,214,209 2.34.210 2.101.210 2.168.210 2.215.209 2.35.210 2.102.210 2.169.210 2.216.209 2.36.210 2.103.210 2.170.210 2.217.209 2.37.210 2.104.210 2.171.210 2.218.209 2.38.210 2.105.210 2.172.210 2.219.209 2.39.210 2.106.210 2.173.210 2.220.209 2.40.210 2.107.210 2.174.210 2.221.209 2.41.210 2.108.210 2.175.210 2.222.209 2.42.210 2.109.210 2.176.210 2.223.209 2.43.210 2.110.210 2.177.210 2.224.209 2.44.210 2.111.210 2.178.210 2.225.209 2.45.210 2.112.210 2.179.210 2.226.209 2.46.210 2.113.210 2.】80.210 2.227.209 2.47.210 2.114.210 2.181.210 2.182.210 2.2.211 2.69.211 2.136.211 2.183.210 2.3.21 i 2.70.211 2.137.21J 2.184.210 2.4.21】 2.71.211 2.138.211 2.185.210 2.5.211 2.72.211 2.139.211 2.186.210 2.6.211 2.73.211 2.140.2 Π 2.187.210 2.7.211 2.74.211 2.141.211 2.188.210 2.8.211 2.75.211 2.142.211 2.189.210 2.9.211 2.76.211 2.143.211 2.190.210 2.10.211 2.77.211 2.144.211 2.19I.2I0 2.11.211 2.78.211 2.145.211 2.192.210 2.12.211 2.79.211 2.146.211 2.193.210 2.13.211 2.80.211 2.147.211 2.194.210 2.14.211 2.81.211 2.148.211 2.195.210 2.15.2Π 2.82.211 2.149.211 2.196.210 2.16.211 2.83.211 2.150.211 2.197.210 2.17.211 2.84.211 2.151.211 2.198.210 2.18.2Π 2.85.211 2.152.211 2.199.2 JO 2.19.2】] 2.86.211 2.153.211 2.200.210 2.20.211 2.87.211 2.154.211 2.201.210 2.21.211 2.88.211 2.155.211 2.202.210 222.211 2.89.2Π 2.] 56.213 2.203.210 2.23.21] 2.90.211 2.157.211 2.204.210 2.24.211 2.91.211 ' 2.158.211 2.205.210 2.25.211 2.92.2Π 2.159.211 2.206.210 2.26.211 2.93.211 2.160.211 2.207.210 2.27.211 2.94.211 2.161.211 2.208.210 2.28.211 2.95.211 2.162.211 2.209.210 2.29.2】1 2.96.211 2.163.211 2.210.210 2.30.211 2.97.211 2.164.211 2.211.210 2.31.211 2.98-.211 2.165.211 2.212.210 2.32.211 2.99.211 2.166.211 2.213.210 2.33.211 2.100.211 2.167.211 2.214.210 2.34.211 2.101.211 2.168.211 2.215.210 2.35.211 2.102.211 2.169.211 2.216.210 2.36.211 2. J 03.211 2.170.211 2.217.210 2.37.211 2.104.2 Π 2.171.211 2.218.210 2.38.211 2.105.2Π 2.172.211 2.219.210 2.39.211 2.】06.211 2.173.211 2.220.210 2.40.211 2.107.211 2.174.211 2.221.210 2.41.211 2.108.211 2.175.211 2.222.210 2.42.211 2.109.211 2.176.211 2.223.210 2.43.211 2.110.211 2.177.211 2.224.210 2.44.211 2.111.211 2.178.211 2.225.210 2.45.211 2.112.211 2.179.211 2.226.210 2.46.211 2.113.211 2.180.21】 2.227.210 2.47.211 2.114.211 2.181:211 2.228.210 2.48.211 2.115.211 2.182.211 2.229.210 2.49.211 2.116.211 2.183.211 2.230.210 2.50.2Π 2.117.2Π 2.184.211 2.231.210 2.51.211 2.118.211 2.185*211 2.232.210 2.52.211 2.119.211 2.186.211 2.233.210 2.53.2Π 2.120.2Π. 2J87.211 2.234.210 2.54.211 2.121.211 2.188.211 2.235.210 2.55.211 2.122.211 2.189.211 2.236.210 2.56.211 2.123.211 2.1 卯,211 2.237.210 2.57.211 2.124.211 2.191.211 2.238.210 2.58.211 2.125.211 2.192.211 2.239.210 2.59.211 2.126.211 2.193.211 2.240.210 2.60.211 2.127.211 2.194.211 2.241.210 2.61.2Π 2J28.211 2.195.211 2.242.210 2.62.2Π 2.129.211 2.196.211 2.243.210 2.63.211 2.130.211 2.197.211 2.244.210 2.64.211 2.131.211 2.198.2 Π 2.245.210 2.65.211 2.132.211 2.199.211 2.246.210 2*66.211 2.133,211 2.200.211 2_247.210 2.67.211 2.134.211 2.201.211 2.1.211 2.68.2】1 2.135.211 2.202.211 •440- (437)1362934
2.203.211 2.23.212 2.90.212 2.157.212 2.204.211 2.24.212 2.91.212 2.158.212 2.205.211 2.25.212 2.92.212 2.159.212 2.206.211 2.26.212 2.93.212 2.160.2] 2 2.207.211 2.27.212 2.94.212 2.161.212 2.208.2 Π 2.28.212 2.95.212 2.162.212 2.209.211 2.29.212 2.96.212 2.163.212 2.210.211 2.30.212 2.97.212 2.164.212 2.211.211 2.31.212 2.98.212 2.165.212 2.212.211 2.32.212 2.99.212 2.166.212 2.213.211 2.33.212 2.100.212 2.167.212 2.214.211 2.34.212 2.101.212 2.168.212 2.215.211 2.35.212 2.102.212 2.169,212 2.216.211 2.36.212 2.103.212 2.170.212 2.217.211 2.37.212 2.104.212 2.171.212 2.218.211 2.38.212 2.105.212 2.172.212 2.219.2 Π 2.39.212 2.106.212 2.173.212 2.220.211 2.40.212 2.107.212 2.174.212 2.221.211 2.41.212 2.108.212 2.175.212 2.222.211 2.42.212 2.109.212 2.176.212 2.223.211 2.43.212 2.110.212 2.177.212 2.224.2】1 2.44.212 2.111.212 2.178.212 2.225.211 2.45.212 2.112.212 2.179.212 2.226.211 2.46.212 2.113.212 2.180.212 2.227.211 2.47.212 2.114.212 2.181.212 2.228.211 2.48.212 2.115.212 2.182.212 2.229.211 2.49.212 2.116.212 2.183.212 2.230.211 2.50.212 2.117.212 2.184.212 2.231.211 2.51.212 2.118.212 2.185.212 2.232.211 2.52.212 2.119.212 2.186.212 2.233.211 2.53.212 2.120.212 2.187.212 2.234.211 2.54.212 2.121.212 2.188.212 2.235.211 2.55.212 2.122.212 2.1S9.212 2.236.211 2.56.212 2.123.212 2.190.212 2.237.211 2.57.212 2.124.212 2.191.212 2.238.211 2.58.212 2.125.212 2.192.212 2.239.211 2.59.212 2.126.212 2.193.212 2.240.21! 2.60.212 2.127.212 2.194.212 2.241.211 2.61.212 2.128.212 2.195.212 2.242.211 2.62.232 2.129.212 2.196.212 2.243.211 2.63.212 2.130.212 2.197.212 2.244.211 2.64.212 2.131.212 2.198.212 2.245.211 2.65.212 2.132.212 2.199,212 2.246.2 Π 2.66.212 2.133.212 2.200.212 2.247.211 2.67.212 2.134.212 2.201.212 2.1.212 2.68.212 2.135.212 2.202.212 2.2.212 2.69.212 2.136.212 2.203.212 2.3.212 2.70.212 2.137.212 2.204.212 2.4.212 2.71.212 2.138.212 2.205.212 2.5.212 2.72.212 2.139,212 2.206.212 2.6.212 2.73.212 2.140.212 2.207.212 2.7.212 2.74.212 2.141.212 2.208.212 2.8.212 2.75.212 2.142.212 2.209.2J2 2.9.212 2.76.212 2.143.212 2.210.212 2.10.212 2.77.212 2.144.212 2.211.212 2.11.212 2.78.212 2.145.212 2.212.212 2.12.212 2.79.212 2.146.212 2.213.212 2.13.212 2.80.212 2.147.212 2.214.212 2.14.212 2.81.212 2.148.212 2.215.212 2.15.212 2.82.212 2.149.212 2.216.212 2.16.212 2.83.212 2.150.212 2.217.212 2.17.212 2.84.212 2.151.212 2.218.212 2.18.212 2.85.212 2.152,212 2.219.212 2.19.212 2.86.212 2.153.212 2.220.212 2.20.212 2.87.212 2.154.212 2.221.212 2.21.212 2.88.212 2.155,212 2.222.212 2.22.212 2.89.212 2.156.212 2.223.212 2.224.212 2Α4.213 2.111.213 2.178.213 2.225.212 2.45.213 2.112.213 2.179.213 2.226.212 2.46.213 2.113.213 2.180.213 2.227.212 2.47.213 2.114.213 2.181.213 2.228.212 2.48.213 2.115.213 2.182.213 2.229.212 2.49.213 2.116.213 2.183.213 2.230.212 2.50.213 2.Π7.213 2.184.213 2.231.212 2.51.213 2.118.213 2.185.213 2.232.212 2.52.213 2.Π9.213 2.186.213 2.233.212 2.53.213 2.120.213 2.187.213 2.234.212 2.54.213 2.121.213 2.188.213 2.235.212 2.55.213 2.122.213 2.189.213 2.236.212 2.56.213 2.123.213 2.190.213 2.237.212 2.57.213 2.124.213 2.191.213 2.238.212 2.58.213 2.125.213 2.192.213 2.239.212 2.59.213 2J26.213 2.193.213 2.240.212 2.60.213 2.127.213 2.194.213 2.241.212 2.61.213 2.128.213 2.195.213 2.242.212 2.62.213 2.129.213 2.196.213 2.243.212 2.63.213 2.130.213 2.197.213 2.244.212 2.64.213 2.131.213 2.198.213 2.245.212 2.65.213 2.132.213 2.199.213 2.246.212 2.66.213 2.133.213 2.200.213 2.247.212 2.67.213 2.134.213 2.201.213 2.1.213 2.68.213 2.135.213 2.202.213 2.2.213 2.69.213 2.136.213 2.203.213 2.3.213 2.70.213 2.137.213 2.204.213 2.4.213 2.71.213 2.138.213 2.205.213 2.5.213 2.72.213 2.139.213 2.206.213 2*6.213 2.73.213 2.140.213 2.207,213 2.7.213 2.74.213 2.141.213 2.208.213 2.8.213 2.75.213 2.142.213 2.209.213 2.9.213 2.76.213 2.143.213 2.210.213 2.10.213 2.77.213 2.144.213 2.211.213 2.11.213 2.78.213 2.145.213 2.212.213 2.12.213 2.79.213 2.146.213 2.213.213 2.13.213 2.80.213 2.147.213 2.214.213 2.14.213 2.81.213 2.148.213 2.215.213 2.15.213 2.82.213 2.149.213 2.216.213 2.16.213 2.83.213 2.150.213 2.217.2】3 2.17.213 2.84.213 2.151.213 2.218.213 2.18.213 2.85.213 2.152.213 2.219.213 2.19.213 2.86.213 2.153.213 2.220.213 2.20.213 2.87.213 2.154.213 2.221.213 2.21.213 2.88.213 2.155.213 2.222.213 2.22.213 2.89.213 2.156.213 2.223.213 2.23.213 2.90.213 2.157.213 2.224.213 2.24.213 2.91.213 2.158.213 2.225.213 2.25.213 2.92.213 2.159.213 2.226.213 2.26.213 2.93.213 2.160.213 2.227.213 2.27.213 2.94.213 2.161.213 2.228.213 2.28.213 2.95.213 2.162.213 2.229.213 2.29.2 ϊ 3 2.96.213 2.163.213 2.230.213 2.30.213 2.97.213 2.164.213 2.231.213 2.31.213 2.98.213 2.165.213 2.232.213 2.32.213 2.99.213 2.166.213 2.233.213 2.33.213 2.100.213 2.167.213 2.234.213 2.34.213 2.101.213 2.168.213 2.235.213 2.35.213 2.102.213 2.169.213 2.236.213 2.36.213 2.103.213 2.170.213 2.237.213 2.37.213 2.104.213 2.171.213 2.238.213 2.38.213 2.105.213 2.172.213 2.239.213 2.39.213 2.106.213 2.173.213 2.240.213 2.40.213 2.107.213 2.174.213 2.241.213 2.41.213 2.108.213 2.】75·2】3 2.242.213 2.42.213 2.J09.213 2.176.213 2.243.213 2.43.213 2.110.213 2.177.213 2.244.213
-441 - (438)1362934
2.245.213 2.65.214 2.132.214 2.199.214 2.246.213 2.66.214 2.133.214 2.200.214 2.247.213 2.67.214 2.134.214 2.201.214 2.1.214 2.68.214 2.135,214 2.202.214 2.2.214 2.69.214 2.136.214 2.203.214 2.3.214 2.70.214 2.137.214 2.204.214 2.4.214 2.71.214 2.138.214 2.205.214 2.5.214 2.72.214 2.139.214 2.206.214 2.6.214 2.73.214 2.140.214 2.207.214 2.7,214 2.74.214 2.141.214 2.208.214 2.8.214 2.75.214 2.142.214 2.209.214 2.9.214 2.76.214 2.143.214 2.210.214 2.10.214 2.77.214 2.144.2M 2.211.214 2.11.214 2.78.214 2.145.214 2.212.214 2.12.214 2.79.214 2.146.214 2.213.214 2.13.214 2.80.214 2.147.214 2.214.214 2.14.214 2.81.214 2.148.214 2.215.214 2.15.214 2.82.214 2.149.214 2.216.214 2.16.214 2.83.214 2.150.214 2.217.214 2.17.214 2.84.214 2.151.214 2.218.214 2.18.214 2.85.214 2.152.214 2.219.214 2.19.214 2.86.214 2.153.214 2.220.2 Η 2.20.214 2.87.214 2.154.214 2.221.214 2.21.214 2.88.214 2.155.214 2.222.214 2.22.214 2.89.214 2.156.214 2.223.214 2.23.214 2.90.214 2.157.214 2.224.214 2.24.214 2.91.214 2.158.214 2.225.214 2.25.214 2.92,214 2.159.214 2.226.214 2.26.214 2.93.214 2.160.214 2.227.2Η 2.27.214 2.94.214 2.161.214 2.228.214 2.28.214 2.95.214 2.162.214 2.229.214 2.29.214 2.96.214 2.163.214 2.230.214 2.30.214 2.97.214 2.164.214 2.231.214 2.31.214 2.98.214 .2.165.214 2.232.214 2.32.214 2.99.214 2.166.214 2.233.214 2:33.214 2.100.214 2.167.214 2.234.214 2.34.214 2.101.214 2.168.214 2.235.214 2.35.214 2.102.234 2.169.214 2.236.214 2.36.214 2.103.214 2.170.214 2.237.214 2.37.214 2.104.214 2.171.214 2.238.214 2.38.214 2.105.214 2.172.214 2.239.214 2.39.214 2.106.214 2.173.214 2.240.214 2.40.214 2.107.214 2.174.214 2.241.214 2.41.214 2.108.214 2.175.214 2.242.214 2.42.214 2.I09.2J4 2.176.214 2.243.234 2.43.214 2.110.214 2.177.214 2.244.214 2.44.214 2.111.214 2.178.214 2.245.214 2.45.214 2.112.214 2.179.214 2.246.214 2.46.214 2.113.214 2.180.214 2.247.214 2.47.214 2.114.214 2.181.214 2.1.215 2.48.214 2.115.214 2.182.214 2.2.215 2.49.214 2.116.214 2.183.214 2.3.215 2.50.214 2.117.214 2.184.214 2.4.215 2.51.214 2.1Ϊ8.214 2.185.214 2.5.215 2.52.214 2.119.214 2.186.214 2.6.215 2.53.214 2.120.214 2.187.214 2.7.215 2.54.214 2.121.214 2.188.214 2.8.215 2.55.214 2.122.214 2.189.214 2.9.215 2.56.214 2.123.214 2.190.214 2.10.215 2.57.214 2.124.214 2.191.214 2.11.215 2.58.214 2.125.214 2.192.214 2.12.215 2.59.214 2.126.214 2.193.214 2.13.215 2.60.214 2.127.214 2.194.214 2.14.215 2.61.214 2.128.214 2.195.214 2.15.215 2.62.214 2.)29.214 2.196.2] 4 2.16.215 2.63.214 2.130.214 2.197.214 2J7.215 2.64.214 2.131.214 2.198.214 2.18.215 2.19.215 2.86.215 2.153.215 2.220.215 2.20.215 2.87.215 2.154.215 2.221.215 2.21.215 2.88.215 2.155.215 2.222.215 2.22.215 2.89.215 2.156.215 2.223.215 2.23.215 2.90.215 2.157.215 2.224.215 2.24.215 2.91.215 2.158.215 2.225.215 2.25.215 2.92.215 2.159.215 2.226.215 2.26.215 2.93.215 2.160.215 2.227.215 2.27.215 2.94.215 2.161.215 2.228.215 2.28.215 2.95.215 2.162.215 2.229.215 2.29.215 2.96.215 2.163.2J5 2.230.215 2.30.215 2.97.215 2.164.215 2.231.215 2.31.215 2.98.215 2.165.215 2.232.215 2.32.215 2.99.215 2.166.215 2.233.215 2.33.215 2.100.215 2.167.215 2.234.215 2.34.215 2.101.215 2.168.215 2.235.215 2.35.215 2.102.215 2.169.215 2.236.215 2.36.215 2.103.215 2.170.215 2.237.215 2.37.215 2.104.215 2.171.215 2.238.215 2.38.215 2.105.215 2.172.215 2.239.215 2.39.215 2.106.215 2.173.215 2.240.215 2.40.215 2.] 07.215 2J 74.215 2.241.215 2.41.215 2.108.215 2.175.215 2.242.215 2.42.215 2.109.215 2.176.215 2.243.215 2.43.215 2.110.215 2.177.215 2.244.215 2.44.215 2.111.215 2.178.215 2.245.215 2.45.215 2.112.215 2.179:215 2.246.215 2.46.215 2.113.215 2.180.215 2.247.215 2.47.215 2.114.215 2.181.215 2.1.216 2.48.215 2.115.215 2.182.215 2.2.216 2.49.215 2.116.215 2.183.215 2.3.216 2.50.215 2.117.215 2.184.215 2.4.216 2.51.215 2.118.215 2.185.215 2.5.216 2.52.215 2.119.215 2.186.215 2.6.216 2.53.215 2.120.215 2.187.215 2.7.216 2.54.215 2.121.215 2.188.215 2.8.216 2.55.215 2.122.215 2.189.215 2.9.216 2.56.215 2.123.215 2.190.215 2.10.216 2.57.215 2.124.215 2.191.215 2.11.216 2.58.215 2.125.215 2.192.215 2.12.216 2.59.215 2.126.215 2.193.215 2.13.216 2.60.215 2.127.215 2.194.215 2.14.216 2.61.215 2.328.215 2,195.215 2.15.216 2.62.215 2.129.215 2.196:215 2.16.216 2.63.215 2.130.215 2.】97.2】5 2·17.2】6 2.64.215 2.131.215 2.198.215 2.18.216 2.65.215 2.132.215 2.199.215 2.19.216 2,66.215 2.133.215 2.200.215 2.20.216 2.67.215 2.134.215 2.201.215 2.21.216 2.68.215 2.135.215 2.202.215 2.22.216 2.69.215 2.136.215 2.203.215 2.23.216 2.70.2] 5 2.137.215 2.204.215 2.24.216 2.71.215 2.138.215 2.205.215 2.25.216 2.72.215 2.139.215 2.206.215 2.26.216 2.73.215 2.140.215 2.207.215 2.27.216 2.74.215 2.141.215 2.208.215 2.28.216 2.75.215 2.142.215 2.209.215 2.29.216 2.76.215 2.143.215 2.210.215 2.30.216 2.77.215 2.144.215 2.211.215 2.31.216 2.78.215 2.145.215 2.212.215 2.32.216 2.79.215 2.146.215 2.213.215 2.33.216 2.80.215 2.147.215 2.214.215 2.34.216 2.81.215 2.148.215 2.215.215 2.35.216 2.82.215 2.149.215 2.2J6.215 2.36.216 2.83.215 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-456- 1362934
(453) 2.134.246 2.20].246 2.21.247 2.88.247 2.155.247 2.222.247 2.135.246 2.202.246 2.22.247 2.89.247 2.156.247 2.223.247 2.136.246 2.203.246 2.23.247 2.90.247 2.157.247 2.224.247 2.137.246 2.204.246 2.24.247 2.91.247 2.158.247 2.225.247 2.138.246 2.205.246 2.25_247 2.92.247 2.159.247 2.226.247 2.139.246 2.206.246 2.26.247 2.93.247 2.160.247 2.227.247 2.140.246 2.207.246 2.27.247 2.94.247 2.161.247 2.228.247 2.141.246 2.208.246 2.28.247 2.95.247 2.162.247 2.229.247 2.142.246 2.209.246 2.29.247 2.96.247 2.163.247 2.230.247 2.143.246 2.210.246 2.30.247 2.97.247 2.164.247 2.231.247 2.144.246 2.211.246 2.31.247 2.98.247 2.165.247 2.232.247 2.145.246 2.212.246 2.32.247 2.99.247 2.166.247 2.233.247 2J46.246 2.213.246 2.33.247 2.100.247 2.167.247 2.234.247 2.147.246 2.214.246 2.34.247 2.101.247 2.168.247 2.235.247 2.148.246 2.215.246 2.35.247 2.102.247 2.169.247 2.236.247 2.] 49.246 2.216.246 2.36.247 2.103,247 2.170.247 2.237.247 2.150.246 2.217.246 2.37.247 2.104.247 2.171.247 2.238.247 2.151.246 2.218.246 2.38.247 2.105.247 2-172.247 2.239.247 2.152.246 2.219.246 2.39.247 2.106.247 2.173.247 2.240.247 2.153.246 2.220.246 2.40.247 2.107.247 2.174.247 2.241,247 2.154.246 2.221.246 2.41.247 2.108.247 2.175.247 2.242.247 2.155.246 2.222.246 2.42.247 2.109.247 2.176.247 2.243.247 2.156.246 2.223.246 2.43.247 2.110.247 2.177.247 2.244.247 2.157.246 2.224.246 2.44:247 2.111.247 2.178.247 2.245.247 2.158.246 2.225.246 2.45.247 2.112.247 2.179.247 2.246.247 2.159.246 2.226.246 2.46.247 2.113.247 2.180.247 2.247.247 2.160.246 2.227.246 2.47.247 2.114.247 2.181.247 2.161.246 2.228.246 2.48.247 2.115.247 2.182.247 2.162.246 2.229.246 2.49.247 2.116.247 2.183.247 2.163.246 2.230.246 2.50.247 2.117.247 2.184.247 2.164.246 2.231.246 2.51.247 2.118.247 2.185.247 2.165.246 2.232.246 2.52.247 2.119.247 2.186.247 2.166.246 2.233.246 2.53.247 2.120.247 2.187.247 2.167.246 2.234.246 2.54.247 2.121.247 2.188.247 2':1'68.246 2.235.246 2.55.247 2.122.247 2.189.247 2.169.246 2.236.246 2.56.247 2.123.247 2.190.247 2.170.246 2.237.246 2.57.247 2.124.247 2.191.247 2.171.246 2.238.246 2.58.247 2.125.247 2.192.247 2.172.246 2.239.246 2.59.247 2.126.247 2.193.247 2.173.246 2.240.246 2.60.247 2.127.247 2.194.247 2.174.246 2.241.246 2.61.247 2.128.247 2.195.247 2.175.246 2.242.246 2.62.247 2.129.247 2.196.247 2.176.246 2.243.246 2.63.247 2.130.247 2.197.247 2.177.246 2.244.246 2.64.247 2.131.247 2.198.247 2.178.246 2.245.246 2.65.247 2.132.247 2.199.247 2.179.246 2.246.246 2.66.247 2.133.247 2.200.247 2.180.246 2.247.246 2.67.247 2.134.247 2.201.247 2.181.246 2.1.247 2.68.247 2.135.247 2.202.247 2.182.246 2.2.247 2.69.247 2.136.247 2.203.247 2.183.246 2.3.247 2.70.247 2.137.247 2.204.247 2.184.246 2.4.247 2.71.247 2.138.247 2.205.247 2.185.246 2.5.247 2.72.247 2.139.247 2.206.247 2.186,246 2.6.247 2.73.247 2.140.247 2.207.247 2.187.246 2.7.247 2.74.247 2.141.247 2.208.247 2.188.246 2.8.247 2.75.247 2.142.247 2.209.247 2.189.246 2.9.247 2.76.247 2.143.247 2.210.247 2.190*246 2.10.247 2.77.247 2.144.247 2.211.247 2.191.246 2.11.247 2.78.247 2.145.247 2.212.247 2.192.246 2.12.247 2.79.247 2.146.247 2.213.247 2.193.246 2,13.247 2.80.247 2.147.247 2.214.247 2.194.246 2.14.247 2.81.247 2.148.247 2.215.247 2.195.246 2.15.247 2.82.247 2.149.247 2.216.247 2.196.246 2.16.247 2.83.247 2.150.247 2.217.247 2.197.246 2.17.247 2.84.247 2.151.247 2.218.247 2.198.246 2.18.247 2.85.247 2.152.247 2.219.247 2.199.246 2.19.247 2.86.247 2.153.247 2.220.247 2.200.246 2.20.247 2.87.247 2. J 54.247 2,221,247 ⑧ (454) 1362934 例示實施例
實例 R 1 R2 酯 分子量 55 Ala OPh 環戊酯 546.5 54 Ala OCH2CF3 Et 5 12.36 53 Ala OPh 3 -呋喃-4 H 548.47 52 Ala OPh c B u t 532.47 50 Phe(B) OPh Et 5 82.5 3 56 Phe(A) OPh Et 5 82.5 3 57 Ala(B) OPh Et 506.43 5 1 Phe OPh sBu(S) 610.58 58 Phe OPh c B u 608.57 49 Phe OCH2CF3 iBu 616.5 1 59 Ala( A) OPh Et 506.43 48 Phe OPh sBu(R) 6 10.58 60 Ala(B) OPh CH2cPr 532.47 6 1 Ala( A) OPh CH2cPr 532.47 62 Phe(B) OPh η B u 610.58 63 Phe(A) OPh η B u 6 10.58 47 Phe OPh CH2cPr 608.57 46 Phe OPh CH2CBU 622.59 45 Ala OPh 3-戊酯 548.5 1 64 ABA(B) OPh Et 520.46 -458- (455)1362934
65 AB A(A) OPh Et 520.46 44 Ala OPh C H 2 c B u 546.5 43 Met OPh Et 566.55 42 Pro OPh Bn 594.54 66 Phe(B) OPh iBu 610.58 67 Phe(A) OPh iBu 610.58 4 1 Phe OPh iPr 596.56 40 Phe OPh η P r 596.56 79 Ala OPh CH2cPr 532.47 68 Phe OPh Et 582.53 69 Ala OPh Et 506.43 70 ABA OPh 正戊酯 562.54 39 Phe Phe nPr 709.71 38 Phe Phe Et 681.66 37 Ala Ala Et 529.47 7 1 CHA OPh Me 574.55 36 Gly OPh iPr 506.43 35 ABA OPh η B u 548.5 1 34 Phe OPh 烯丙酯 594.54 33 A1 a OPh 正戊酯 548.5 1 32 Gly OPh iBu 520.46 72 ABA OPh iBu 548.51 73 Ala OPh η B u 534.48 3 1 CHA CHA Me 665.7 30 Phe Phe 烯丙酯 705.68 29 ABA ABA 正戊酯 641.68 -459- (456)1362934
28 Gly Gly iBu 557.52 27 Gly Gly iPr 529.47 26 Phe OPh iBu 610.58 25 Ala OPh nPr 520.46 24 Phe OPh nBu 610.58 23 ABA OPh η P r 534.48 22 ABA OPh Et 520.46 2 1 Ala Ala Bn 653.61 20 Phe Phe nBu 737.77 19 ABA ABA nPr 585.57 18 ABA ABA Et 557.52 17 Ala Ala nPr 557.52 74 Ala OPh iPr 520.46 75 Ala OPh Bn 568.5 16 Ala Ala nBu 585.57 15 Ala Ala iBu 585.57 14 ABA ABA nBu 613.63 13 ABA ABA iPr 585.57 12 Ala OPh iBu 534.48 77 ABA OPh Me 506.43 78 ABA OPh iPr 534.48 11 ABA ABA iBu 613.63 -460- (457) 1362934 實例1 1 1 H NMR ( CDC13 ) 5 8.39 ( s > 1H ) <5 8. 12 ( s ， 1H ) δ 6.82 (m，lH) <5 5.96-5.81 (m，4H) <5 4.03 - 3.79 ( m > 10H ) ¢5 3.49 ( s - 1H ) <5 3.2 ( m > 2H ) δ 1.96 - 1.69 ( m > 1 OH ) 5 1.26 ( m > 4H ) d 0.91 ( m > 12H ) 31P NMR ( CDC13) 20.37 (s，IP) MS ( M + l ) 614 φ 實例1 2 ]H NMR ( CDCb ) δ 8.39 ( s > 1H ) 5 8. 13 ( s > 1H ) δ 1.21 - 7.11 (m，5H ) δ 6.82 ( s > 1 H ) <5 5.97 - 5.77 ( m ，4H) δ 4.14 - 3.79 ( m > 6H) <5 3.64 ( t > 1H ) δ 2.00 - ' 1.88 ( bm ， 4H) <5 1.3 1 ( dd > 3H ) <5 0.91 ( m > 6H )。
- 31P NMR ( CDCb ) δ 20.12 ( s > 0.5P) <5 19.76 ( s > 0.5P )MS ( M +1 ) 5 35
實例13 *H NMR ( CDCI3 ) :68.39(s，lH) ，8.13(s，lH) ，6.81 ( m，1H) ，5.95 ( m，1H) ，5.81 ( s，1H)， 4.98 (m，2H) > 3.90 ( m > 2H ) ，3.37(m，lH) > 3.19 (m > 1H ) ，1.71 (m，4H) > 1.25 (m> 12H) ，0.90( m，6H ) 質譜（m/e) : (M + H) + 586.3 實例14 -461 - (458) 1362934 】H NMR(CDC13) ： (58.38 (s，1H) > 8. 12 ( s > 1H ) ，6.80 ( m，1H) ，5.93 ( m，1H) ，5.79 ( s，1H)， 4.02 ( m > 6H) > 3.42 ( m > 1H ) > 3.2 1 ( m > 1H ) - 1.65 (m，4H) ，1.35(m，8H) ，0.92(m，12H) 質譜（m/e) : (M + H) + 6 14.3 實例1 5
1H NMR ( CDC13 ) : <5 8.38 ( s > 1H ) ，8.12 ( s，1H) ，6.80 ( m，1H) ，5.93 ( m，2H) ，5.80 ( s，1H)， 3.91 (m，6H) ，3_42(m，1H) ，3.30(m，1H) > 1.9 1 (m，2H) ，l_40(m，6H) ，0.90(m，12H) 質譜（m/e) : (M + H) + 5 86.3 實例16 'H NMR ( CDCI3 ) : <58.37 (s，1H) ，8.17(s，1H) ，6_80 ( m，1H) ，6.18 ( s，1H) ，5.93 ( m，1H)， 5.79 ( s，1H) ，4.02 ( m，6H) ，3.46 ( m，1H) ，3.37 (m > 1H ) > 1.61 ( m > 4H ) ，1.32(m，10H) ，0.92( m，6 H ) 質譜（m/e) : (M + H) + 614.3 實例17
1H NMR ( CD3OD ) : δ 8.29 ( s > 1H ) ，8.25 ( s，1H )> 6.84 ( m > 1H ) ，6.00(s，lH) ，5.96(m，lH)，
-462- (459) 1362934 4.04 ( m，8H) > 1.66 ( m > 4H ) ，1.38 ( m，6H) > 0.98 (m，6 H ) 質譜（m/e) : (M + H) + 5 5 8.3 實例18
1H NMR ( CD3〇D ) ： δ 8.29 ( s > 1H ) ，8.25 ( s，1H )，6.84(m，lH) ，5.99(s，lH) ，5_96(m，lH)，
4.04 ( m，8H) ，1.67 ( m，4H) ，1.23 ( m，6H) ，0.95 (m，6 H ) 質譜（m/e) : (M + H) + 5 5 8.3 實例1 9
1H NMR ( CD3OD ) ： 5 8.29 ( s，1 H ) ，8_25 ( s，1H )，6.84(m，lH) ，5.99(s，lH) ，5.96(m，lH)， 4.03 (m，8H) > 1.66 ( m > 8H ) > 0.93 ( m > 12H ) 質譜（m/e): (M + H) + 5 86.3 實例20
NMR ( CD3OD ) ： δ 8.25 ( s - 1H ) > 8. 17 ( s > 1H )，7.21 (m，10H) > 6.80 ( m > 1H ) ，5.91 (s，1H) ，5.72 ( m，1H) ，4.04 ( m，6H) ，3.50 ( m，2H)， 2.90 ( m > 4H) ，1.47(m，8H) > 0.92 ( m > 6H ) 質譜（m/e) : (M + H) + 7 3 8.4 -463- (460) 1362934 實例2 1
'H NMR ( CD3〇D ) ： 5 8.24 ( s，2H) ，7.33 ( m，10H )，6_81(m，lH) ，5.88(s，lH) ，5.84(m，lH)， 5.12 (m，4H) > 3.94 ( m > 4H ) > 1.35 ( m > 6H ) 質譜（m/e) : (M + H) + 654.3 實例22
]H NMR ( CDCh ) <5 8.3 8 ( d > 1H ) 5 8 · 1 2 ( d ， 1 H ) <5 7.3 1 - 7.10 ( m > 5H ) <56.81 (m，lH) δ 5.98 - 5.7 5 ( m -4H ) <5 4.23 - 3.92 ( m > 7H ) 5 3.65 ( m > 1H ) 5 1.63
(n3H ) δ 1.26 ( m > 4H ) 6 1.05 - 0.78 ( m > 3H) 31P NMR δ 2 1.01 ( s ， 0.6P ) δ 20.12 ( s - 0.4P ) MS ( M+l ) 52 1 實例23 1H NMR ( CDCI3 ) ： 58.14 (d> 1H) <5 8 · 1 3 ( d，1H ) 5 7.30-7.10( m，5H) 6 6.82( m，lH) ¢5 5.99-5.77 ( m，3H) 54.22-3.92 (m>6H) <53.61 (m> 1H) 5 1.65 (m， 4H) 5 1.26-0.71 (m> 6H) 31P NMR(CDC13) δ 20.99 ( s，0.6P ) δ 20.08 ( s，0.4P) MS ( M+l) 535 實例24 1 H NMR ( CDCI3 ) : (5 8.39 ( d > 1 H ) 5 8.08 ( d > 1 H ) <5 7.28 - 6.74 ( m - 10H ) 5 5.90 ( m，4H) δ 4.37 ( m -
-464- (461)1362934 1H ) (5 4.05 ( m > 5H ) δ 3.56 ( m > 2H ) )(5 1 .55 ( m > 2H ) <5 1.22 ( m > 3H ) δ 3 1 P NMR ( CDC13 ) δ 20.95 ( s > 0.5P ) < )MS ( M+1 ) 6 11
ά 2.99 ( m，2H 0.88 ( m，3H ) 20.01 ( s，0.5P
實例25 lU NMR ( CDCI3 ) : δ 8.38 ( d > 1H ) (5 7.31-7.11 (m> 5H) <5 6.8 2 ( s > 1 H ) m ， 4H ) δ 4.22 - 3.63 ( m > 6H ) 5 2.1 1.65 ( m > 2H ) <5 1 .30 ( m > 4H ) (50.88 NMR ( CDCI3 ) δ 20.75 ( s ， 0.5P ) δ 1« MS ( M+ 1 ) 52 1 5 8.11 ( s，1 H ) δ 5.96 - 5.76 ( 7 ( bm ， 2H) δ (m，3H ) 。3 1 P 5.82 ( s > 0.5P)
實例26 1H NMR ( CDCI3 ) δ 8.40 ( d > 1 H ) δ I 7.27 - 6.74 ( m > 10H ) δ 5.93 - 5.30 ( m >1H) (54.14-3.77 (m-4H) ¢5 3.58 ( (m，2H) (5 1.90 ( m ' 3H ) <5 1.2 6 ( m > ，6H ) 。31P NMR ( CDC13 ) δ 20.97 ( s (s > 0.5P ) MS (M+l) 611 • 09 ( d，1 H) δ ，4H ) δ 4.39 ( m m，2H ) <5 2.95 1 H ) δ 0.85 ( m ，0.5P ) δ 20.04 實例27 1H NMR ( CD3OD ) ： 8.3 1 ( s > 1H ) ，6.84 ( m，1H ) ，6.02 ( s， 1H ) ，5 · ，8.25 ( s，1H ) 98 ( m， 1H )， -465- ⑧ (462) 1362934 4.98 (m，2H) ，4.01(m，2H) ，3_66(m，4H) > 1.23 (m，1 2H ) 質譜（m/e) : (M + H) + 530.2 實例28 1H NMR ( CD3〇D ) ： 8.3 1 ( s > 1H ) ，8.25 ( s，1H) ，6.84 ( m，1H) ，6.01 ( s，1H) ，5.98 ( m，1H)，
4.03 (m，2H) ，3.86(m，4H) ，3.68(m，4H) ，1.92 (m，2H ) ，0,93 ( m，1 2H ) 質譜（m/e) : (M + H) + 55 8.3 實例29 】H NMR ( CD3OD) : 8.29 ( s，1H) ，8.25 ( s，1H) ，6.84 ( m，1H) ，5.99 ( s，1H) ，5_97 ( m，1H)， 4.01 ( m，8H) ，1.66 ( m，8H) ，1_32 ( m，8H) > 0.96
質譜（m/e): (M + H) + 642.4 實例30 1H NMR ( CD3OD ) ： 8.25 ( s > 1H ) ，8.16(s，1H) ，7.24 ( m，10H) ，6.80 ( m，1H ) ，5.90 ( s，1H )， 5.71 (m，lH) > 5.25 ( m > 4H ) ，4.57(m，2H) > 4.5 1 (m，2H) ，4.05(m，2H) ，3.46(m，2H) > 2.92 ( m ，6H ) (463)1362934 質譜（m/e) : (M + H) + 706.4 實例3 1 'H NMR ( CD3〇D ) ： 8.32 ( s > 1H ) ，8.25 ( s，1H) > 6.84 ( m > 1H ) ，6.00 ( s，1H) ，5.97 ( m，1H)， 3.93 ( m，4H) ，3.71 ( s，3H) ，3.60 ( s，3H) > 1.5 1 (m ， 26H)
質譜（m/e) : (M + H) + 666.5 實例32 1H NMR ( CDCI3 ) : (58.39(s，1H) <5 8. 1 7 ( d > 1H ) δ 7.32 - 6.82 ( m > 5H) 56.82 (s， 1H ) 5 5.98 - 5.81 ( m > 3H ) 54.27-3.64 (m，6H) 5 1.94 (m，lH) 50.90 (m ， 6H ) 。 31P NMR ( CDC13 ) δ 2 1.50 ( s > 0.5P ) δ 2 1.37 ( s > 0.5P ) MS ( M +1 ) 52 1 實例33 *H NMR ( CDCI3 ) δ 8.39 ( s > 1H ) 58.13 (s， 1H) <5 7.27 - 7.14 ( m > 5H ) δ 6.85 ( s > 1H ) <5 5.9 7 - 5.7 7 ( m ，4H) (5 4.18— 4.05 (m，7H) (5 1.60 (m，3H) 5 1.29 (m， 7H ) δ 0.90 ( m > 3H ) 3 1P NMR ( CDC13 ) δ 20.69 (s，0.6P ) δ 19.77 ( s > 0.4P ) MS ( M+l) 549 實例34
-467- (464) 1362934 ]H NMR ( CDC13 ) (5 8.39 ( d > 1H ) (5 8.07 ( d > 1H ) δ
7.27-6.74 (m ， 1 OH ) δ 5.91 ( m > 2H ) <5 5.69 ( m ， 2H )<55.27 (m'2H) 54.55 (m>2H) (54.30(m>lH) <5
3.69 ( m > 1H) δ 2.95 ( m > 1H) δ 5.05 ( m > 2H ) 31P NMR ( CDCI3 ) δ 20.94 ( s > 0.5P ) <5 19.94 ( s > 0.5P ) MS ( M+ 1 ) 595 φ 實例3 5 1H NMR ( CDCh ) δ 8.39 ( d > 1H ) <58.11 ( d > 1H ) δ 7.28 - 7. 10 ( m > 5H ) 5 6.82 ( s ' 1H ) δ 5.98 - 5.76 ( m ，3H) (54.18-3.56 (m，4H) 5 3.59 ( m - 1H ) 5 1.74 1 - 0.70 ( m > 12H) 。31P NMR ( CDC13 ) <5 2 1.00 ( s > ' 0.6P ) δ 20.09 ( s > 0.4P ) MS ( M +1 ) 549 實例36
1 H NMR ( CDCI3 ) (5 8.3 9 ( d > 1H ) (5 8 · 1 2 ( d ， 1 H ) δ 7.29 ( m ， 2Η) δ 7.15 ( m > 3H) δ 6.82 ( s > 1H) δ 5.94 (dd > 1 H ) 5 5.80 ( s > 3H ) <55.02(m， 1H ) δ 4.23-
3.58 (m，6H) δ 2.18 ( s > 3H ) <5 1.23 ( m > 6H ) °31P NMR ( CDCI3 ) δ 21.54 ( s > 0.5P ) δ 21.43 ( s > 0.5P)。 MS ( M + 1 ) 507 實例37 H NMR ( CD3OD ) : 8.30 ( s，1H) ，8_25 ( s，1H) -468- (465)1362934 ，6.84 ( m，1 Η ) ，6.00 ( s，1H ) ，5 4.06 ( m，8H) ，1.31 ( m，12H ) 質譜（m/e) : (M + H) + 530.3 .9 5 ( m > 1 H )，
實例38 1H NMR ( CD3〇D ) : 8.25 ( s，1H ) ，7.24 ( m，10H ) ，6.84 ( m，1H )， 5.75 ( m > 1H ) > 4.08 ( m > 6H ) > 3.60 (m，4H) ，1.21(m，6H) 質譜（m/e) : (M + H) + 682.4 ，8. 16 ( s，1H ) 5.91 ( s，1H )， (m，2H ) > 2.90
實例39 】H NMR (CD3OD) : 8.25 ( s，1H) ，7.22 ( m，10H ) ，6.8 1 ( m，1H )， 5.72 ( m，1H) ，4.02 ( m，6H) ，3.63 (m，4H) > 1.58 ( m > 4H ) ，0.87(m， 質譜（m/e) : (M + H) + 7 10.4 ，8 · 1 6 ( s，1 H ) 5.90 ( s，1H )， (m，2H ) > 2.90 6H ) 實例40 1H NMR ( CD3〇D ) : 8.25 ( m，2H) ，6.95 ( m，1H ) ，6.82 ( m，1H ) ，5 5.72 (m，1H) ，3.95 (m，4H) ，3.63 (m > 1H ) ，2.81 ( m，1H ) ，1 .55 ( m ，3H ) ，7.22 ( m，8H ) .90 ( m > 2H )， (m > 1H ) > 3.07 ，2H ) ，0.86 ( m -469- (466)1362934 質譜（m/e) : (Μ + Η) + 597·4 實例41 lH NMR ( CD3〇D ) ： 8.25 ( m > 2H )， ，6.96 ( m，1H ) ，6.81 ( m， 1H ) ，5. 5.73 ( m，1H) ，4.05 ( m，2H) > 3.60
(m，lH) > 2.81 ( m > 1H ) ，1.13(m， 質譜（m/e) : (M + H) + 597.5 7.20 ( m，9H ) 97 ( m，2H )， m，1H ) ，3.02 6H ) 實例42 !H NMR ( CD3OD ) ： 8.25 ( m > 2H ) )，6.83(m，lH) ，5.92(m，2H) ，5 4.25 (m，4H) ，3.20(m，1H) > 1.90( 質譜（m/e) : (M + H) + 5 95.6 ，7.33 ( m，1 OH • 1 5 ( m，2H )， m，4H )
實例43 1H NMR ( CD3OD ) ： 8.25 ( m > 2H )， ，6_83 ( m，1 H ) ，5.98 ( m，2H ) ，4. 2.50 ( m > 4H) ，2.01(m，3H) ，1.22( 質譜（m/e) : (M + H) + 567.3 7.15 ( m，5H ) 10 ( m，5H )， m，3H ) 實例44 1H NMR ( CD3OD ) ： 8.25 ( m > 2H )， ，6.83 ( m，1H ) ，5.98 ( m，2H ) ，4. 7_ 15 ( m，5H ) 10 ( m，5H )， -470- (467) 1362934 2.57(m，lH) - 1.80 ( m > 6H ) ，1.25(m，3H) 質譜（m/e) : (M + H) + 547.7 實例45 5H ) H )， > 0.88 *H NMR ( CD3〇D ) : 8.25 ( m，2H) ，7.17 ( m ，6.85 ( m，1H) ，5.99 ( m，2H) ，4.66 ( m，1 4.12 ( m > 3H ) ，1.56(m，4H) > 1.2 8 ( m > 3H )
質譜（m/e) : (M + H) + 549.3 實例46 1H NMR ( CD3OD ) : 8.25 ( m，2H) ，7.12 ( m )，6.83(m，lH) ，5.99(m，2H) > 5.72 ( m > 1 4.10 (m，4H) ，3.65(m，1H) ，3.02(m，1H) (m，lH) ，2.50(m，lH) ，1.89(m，6H) 質譜（m/e) : (M + H) + 623.4 實例47 1H NMR ( CD3OD ) : 8.25 ( m，2H) ，7.15 ( m )> 6.82 ( m > 1H ) > 5.99 ( m > 2H ) ，5.73(m，l 3.99 ( m > 4H) > 3.65 ( m > 1H ) ，3.05(m，lH) (m > 1 H ) ，1.02(m，lH) > 0.5 1 ( m - 2H ) ，0· ，2H ) 質譜（m/e) : (M + H) + 609.3 ，1 OH H )， ，2.79 ，1 OH H )， ，2.85 20 ( m -471 - (468) 1362934 實例48 1H NMR ( CD3〇D ) : 8.25 ( m，2H) > 7.20 ( m > 9H ) ，6.96(m，lH) ，6.81(m，lH) ，5.97(m，2H)， 5.73 (m，1H) > 4.7 1 ( m > 1H ) ，4.05(m，2H) ，3.60 (m，lH) ，3_02(m，lH) ，2.81(m，lH) > 1.49 ( m ，2H) ，1.07(m，3H) ，0_82(m，3H)
質譜（m/e) : (M + H) + 6 1 1,2 實例49 'H NMR ( CD3OD ) : 8.20 ( m，2H) ，7.25 ( m，6H) ，6.82(m，lH) ，5.95(m，2H) ，5.68(m，lH)， 3.93 (m，6H) ，3.50(m，lH) ，3.20(m，lH) > 2.81 (m > 1 H ) ，1.90(m，lH) ，0.95(m，6H) 質譜（m/e) : (M + H) + 6 1 7.3 實例50
1H NMR ( CD3OD ) ： 8.23 ( m > 2H ) ，7.18(m，10H )，6.96(m，lH) > 6.81 ( m > 1H ) ，5.94(m，2H)， 5.72 ( m > 1H) ，4_81(m，lH) ，4.05(m，2H) > 3.60 (m，lH) ，3.02(m，lH) > 2.8 1 ( m > 1H ) ，2.25(m ，2H) ，1 · 8 1 ( m，4H ) 質譜（m/e) : (M + H) + 609.3 472- (469) (469)1362934 實例51 1H NMR ( CD3OD ) ： 8.25 ( m > 2H ) ，7.20 ( m，9H) ，6.96 ( m，1H) ，6.81 ( m，1H) ，5.97 ( m，2H)， 5.73 (m，lH) ，4.71(m，lH) ，4_05(m，2H) > 3.60 (m，lH) ，3.02(m，lH) ，2_81(m，lH) ，1.49(m ，2H) ，1.07(m，3H) ，0.82(m，3H) 質譜（m/e) : (M + H) + 6 1 1.4 實例5 2
1H NMR ( CD3OD ) ： (5 8.29 ( m > 1H ) ，8.25 ( m，1H )，7_:2 0(m，5H) ，6.85(m，lH) ，5.97(m，2H)， 4.85(m，lH) ，4.15(m，2H) ，3.95(m，lH) > 2.28 (m，2H) ，1.99 ( m，2H) ，1.77 ( m，2H) > 1.26 ( m ，3H ) 質譜（m/e) : (M + H) + 5 3 3.3 實例53
'H NMR ( CD3OD ) : <5 8_29 ( m，1H ) ，8.25 ( m，1H )，7_20(m，5H) ，6.85(m，lH) ，5.98(m，2H)， 5. 1 8 ( m > 1 H ) ，4.03(m，7H) ，2.15(m，lH) ，1.95 (m，lH) ，l_26(m，3H) 質譜（m/e) : (M + H) + 549.2 實例54
-473- (470) 1362934
H NMR ( CD3〇D ) : 5 8.24 ( m，2Η) ，6.85 ( m，1H )’ 6.01 (m，2 H ) ，4.43 (m，2 H ) ，4.09(m，5H)， 1.38 ( m，3H ) ，1.23 ( m，3H ) 質譜（m/e) : (M + H) + 5 1 3.2 實例55 於磷處之非對映異構體混合物之1H NMR ( 300MHz， • CD3OD 參考溶劑 3.30ppm ) ： δ ( ppm ) = 8.22 - 8.27 ( m ' ，2H) > 7.09 - 7.34 ( m > 5H ) ，6.84(brs，lH) * 5.93 -6.02 ( m > 2H ) ，5.00-5.14 (m，lH) > 4.01 - 4.26 ( m，2H) ，3.89-3.94 (m，1H) ，1.50-1.88 (m，8H) " ，1.23(br t，3H，J=6.8)。於磷處之非對映異構體混 - 合物之 31p NMR( 121MHz ’ 1H 解親）：6 (ppm)= 23.56 ， 22.27 (〜60 : 40 比）» 上述所有文獻及引用之專利乃明確地倂入本文中以供 Φ 於其引用的位置參考。上文所引用文獻中所特別引用之文 - 節或頁數乃倂入本文中以供專一性地參考。本發明業已詳 盡地說明以足以令熟知技藝者進行及使用下列實施例之主 題。明顯地，下列實施例之方法及組成物可在本發明範圍 及精髓內進行一些改良° 下文實例中，所提供變數之下標及上標符號是有所區 別的。例如R,不同於Rl。 -474-

Claims (1)

1362934
附件3A :第094125503號申請專利範圍修正本 民國101年1月19曰修正
十、申請專利範圍 1 . 一種如下式所示之化合物
其中h與R2係選自下表：
Ri r2 酯 Ala OPh c P e nt Ala OCH2CF3 Et Ala OPh 3 -呋喃-4 H Ala OPh c B ut Phe(B) OPh Et Phe(A) OPh Et Ala(B) OPh Et Phe OPh sBu(S) Phe OPh cBu Phe OCH2CF3 iBu A 1 a ( A) OPh Et Phe OPh sBu(R) 1362934 Ala(B) OPh CH2cPr Ala(A) OPh CH2cPr Phe(B) OPh nB u Phe(A) OPh nB u Phe OPh CH2cPr Phe OPh C H 2 c B u Ala OPh 3 -p ent ABA(B) OPh Et ABA(A) OPh Et Ala OPh CH2CBU Met OPh Et Pro OPh Bn Phe(B) OPh iBu Phe(A) OPh iBu Phe OPh iPr Phe OPh nPr Ala OPh CH2cPr Phe OPh Et Ala OPh Et ’ ABA OPh nPent Phe Phe nPr Phe Phe Et Ala Ala Et CHA OPh Me -2-
s 1362934
Gly OPh iPr ΑΒΑ OPh nBu P he OPh allyl Ala OPh nP ent Gly OPh iBu ABA OPh iBu Ala OPh nBu CHA CHA Me P h e Phe allyl ABA ABA nPent Gly Gly iBu Gly Gly iPr P h e OPh iBu Ala OPh nPr Phe OPh nBu ABA OPh nPr ABA OPh Et Ala Ala Bn Phe Phe nBu ABA ABA nP r ABA ABA Et Ala Λ1 a nP r Ala OPh iPr Ala OPh Bn -3- 1362934 Ala Ala nBu Ala Ala iBu ΑΒΑ ΑΒΑ nBu ΑΒΑ ΑΒΑ iPr Ala OPh iBu ΑΒΑ OPh Me ΑΒΑ OPh iPr ΑΒΑ ΑΒΑ iBu
其中Ala代表L —丙胺酸’ Phe代表L -苯丙胺酸， Met代表L -甲硫胺酸’ ΑΒΑ代表（S) —2 —胺基丁酸， Pro代表L -脯胺酸，CHA代表2 —胺基一3— (S)環己 基丙酸’ Gly代表甘胺酸； Ri或R2胺基酸羧基係經酯化如酯欄中所示，其中 cPent爲環戊酯；Et爲乙酯，3 —呋喃—4H爲（R)四氫 呋喃—3 —酯’ cBut爲環丁酯，sBu(S)爲（S)二級丁 酯 ’ sBu ( R)爲（R)二級 丁酯，iBll 爲異 丁酯，cH2CPr 爲甲基環丙酯’ nBu爲正丁醋；CH2cBu爲甲基環丁醋；3 —pent爲3-戊酯；nPent爲正戊酯；iPr爲異丙酯；nPr 爲正丙酯：ally丨爲烯丙酯；Me爲甲酯；Bn爲苄酯：且 其中括弧內之A或B代表於磷處之一個立體異構體 ’最低極性之異構體以（A)表示，較具極性之異構體以 (B )表示。 或其藥學上可接受之鹽或溶劑化物》 -4- S 1362934 2 ·如申請專利範圍第1項之化合物，具有以下所示 式XX :
4_ 一種藥學組成物，包含藥學賦形劑及抗病毒有效 量之申請專利範圍第1至3項中任一項之化合物。 5·如申請專利範圍第4項之藥學組成物，其另包含 第二活性成分。 6. —種組合，包含申請專利範圍第1至3項中任一 項之化合物及—或多種抗病毒活性成分。 7. 如申請專利範圍第6項之組合，其中該等抗病毒 活性成分之—或多者係選自尼可韋（Nicavir )、 Aldesleukin 德 口卜咐（Gacj〇iinium texaphyrin)、恩福 1362934 韋地（Enfuvirtide )、西米皮莫氫氯酸鹽（S e m ap i m o d hydrochloride ) ' 依夫他濱（Elvucitabine )、藍藻抗病 毒蛋白 N ( Cyanovirin N )、偶氮甲薩胺 （ Azodicarbonamide)、替諾福韋雙異丙醯氧基甲酯富馬酸 鹽(Tenofovir disoproxil fumarate ) 、Anticort、Reverset 、仙皮定(Sampidine) 、Immunitin、Inactivin、Racivir 、硫酸纖維素、狄皮扶林（Dapivirine)、拉米夫定/齊 多夫定/阿巴卡韋硫酸鹽 （Lamivudine/Zidovudine/ abacavir sulfate)、伊妥韋林（Etravirine)、阿達吉白 素 a(Adargileukin alfa)、格里米諾（Glyminox)、十 二基硫酸鈉、恩奎韋洛（Ancriviroc) 、0-(2 -經丙基）-β-環糊精、達魯那韋（Darunavir)、馬拉韋洛（Maraviroc )、Dermavir、擴酸化檸檬黃素（sulfonated Hesperidin )、V-I 免疫藥 （V-I Immunitor )、里普韋林 （ Rilpivirine )、代謝物 X ( Metabo 1 ite X ) ' MIV-150/ 角 叉菜膠（MIV-150/Carraguard)、替諾福韋雙異.丙醯氧基 甲醋富馬酸鹽/恩曲他濱/依發韋侖（Tenofovir disoproxil fumarate/emtricitabine/efavirenz )、胸腺核蛋 白（Thymus nuclear protein) 、GS-913 7 (Elvitegravir)、 及乙酸酞酸纖維素（cellulose acetate phthalate)。 8.如申請專利範圍第6項之組合，其中該等抗病毒 活性成分之一係選自 阿巴卡韋硫酸鹽（Abacavir sulfate); 阿巴卡韋硫酸鹽/拉米夫定（Abacavir sulfate/lamivudine 1362934 阿德福韋雙異戊酿氧甲醋（Adefovir dipivoxil) 安普那韋（Amprenavir); 阿托那韋硫酸鹽（Atazanavir sulfate); 地拉韋定甲擴酸鹽（Delavirdinemesilate)； 二去氧胞苷：扎西他濱（Zalcitabine): 二去氧肌苷；去羥肌苷（Didanosine);
依發韋侖（Efavirenz); 恩曲他濱（Emtricitabine)； 福善那韋耗（Fosamprenavir calcium); 膦甲酸三鈉（Foscarnet sodium); 印地那韋硫酸鹽（Indinavir sulfate)； 拉米夫定(Lamivudine ) ； 拉米夫定 / 齊多夫定（Lamivudine/Zidovudine); 洛匹那韋（Lopinavir); 洛匹那韋/利托那韋（Lopinavir/ritonavir); 尼非那韋甲磺酸鹽（Nelfinavirmesilate); 那韋拉平（Nevirapine); 利托那韋（Ritonavir); 沙克那韋甲擴酸鹽（Saquinavir mesilate); 司他夫定（Stavudine); 替諾福韋雙異丙醯氧基甲酯富馬酸鹽/恩曲他濱（ Tenofovir disoproxil fumarate/emtricitabine ); 替普那韋（Tipranavir); 1362934 月多夫疋（Zidovudine)。 9· &申請專利範圍第6項之組合，其 分之一係選自 Truvada、Viread、Emtriva、 、或女普那韋（Amprenavir)抗病毒化合物 1〇·如申請專利範圍第4或5項之藥學 於醫療。： Π.如申請專利範圍第6至9項中？壬一 用於醫療》 ' 1 2 .如申請專利範圍第.1至3項中任一 ~ I 係用於在抗反轉錄病毒或抗.嗜肝；DNA病毒 療。. H如申諍專利範圍第6至9項宁任一 用於在抗反轉錄病毒或抗嗜肝.0ΝΑ病毒治 〇 1 4.如申請專利範圍第1至3項中任一 係用於治療HIV或HIV相關病症之方法。 1 5.如申請專利範圍第6至9項中任一 用於治療HIV或HIV相關病症之方法。 中該等活性成 d4T ' Sustiva ο 組成物，係用 . .-· .· 項之組合，係 _ . · i之化合" %， 治療方面之醫 項之組合，係 療方面之醫療 項之化合物， 項之組合，係
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