JP5150251B2 - 活性化可能な粒子、調製、および使用 - Google Patents
活性化可能な粒子、調製、および使用 Download PDFInfo
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- JP5150251B2 JP5150251B2 JP2007512273A JP2007512273A JP5150251B2 JP 5150251 B2 JP5150251 B2 JP 5150251B2 JP 2007512273 A JP2007512273 A JP 2007512273A JP 2007512273 A JP2007512273 A JP 2007512273A JP 5150251 B2 JP5150251 B2 JP 5150251B2
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- A61N5/00—Radiation therapy
- A61N5/10—X-ray therapy; Gamma-ray therapy; Particle-irradiation therapy
- A61N2005/1092—Details
- A61N2005/1098—Enhancing the effect of the particle by an injected agent or implanted device
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Description
− X線を吸収し、紫外−可視エネルギーを放射する第1の無機化合物、および、紫外−可視エネルギーを吸収し、水又は酸素と接触してフリーラジカルを生成する無機又は有機の第2の化合物を含む核、並びに
− 所望により、生体適合性コーティング、
を含む、(X線で励起された場合に、フリーラジカル又は熱を発生させ得る)生体適合性複合粒子又はナノ粒子凝集体に基づく。
− ターゲティング剤、
− 生体適合性を確保又は改善する分子、又は
− 粒子が免疫系から逃れること(並びに、特にマクロファージおよびSREとの相互作用を回避すること)を可能にする分子、
とすることができる。
− TiO2の層で被覆されているY2O3:Gdを含むコアと、好ましくは機能化されているSiO2コーティングとを含む粒子又は凝集体。好ましくは、コアは形状が丸いか又は球状であり、サイズが約5〜50nm(典型的には、約30nm)であり、TiO2層の厚さは約5〜30nm(典型的には、約5nm)であり、コーティングの厚さは約1〜50nm(典型的には、約5nm)である。
− Y2O3:Tbのマイクロ粒子とTiO2のマイクロ粒子を含む核、および、好ましくは機能化されている、デキストランをベースにするコーティングを含む粒子又はナノ粒子凝集体。
− TiO2の層で被覆されているHfGeO4を含むコアと、好ましくは機能化されているSiO2コーティングとを含む粒子又は凝集体。
− 粒子又は凝集体を形成するため、前述のような2種類の化合物を混合する工程、および、所望により
− 粒子又は凝集体をコーティングする工程、
を含む、前述のような粒子又はナノ粒子凝集体の製造方法に関する。
− 第1の無機化合物を含む粒子コアを調製する工程、
− このようにして形成されるコアを、第2の化合物を含む層で被覆する工程、および、好ましくは、
− このようにして得られた粒子又は凝集体を多孔質材料でコーティングする工程、
を含む。
− 均質な媒体中でYCl3、EuCl3およびクラウンエーテルと一緒に還元して、Y2O3:Euナノ粒子を製造し、
− 酸性溶液中でTiCl4を沈殿させることにより、TiO2層を加えることができ、その後、
− 塩基性媒体中でケイ酸ナトリウムを沈殿させることにより、任意選択的なシリカ層を得る。
− ハフニウムと非晶質ゲルマニウム塩の共沈によりコアを合成する工程、
− TiO2で被覆する工程、および
− TEOSおよび/又はケイ酸ナトリウムを使用してSiO2でコーティングする工程、
を含む。
− 表面X線(20〜50keV):表面付近のナノ粒子を励起させる(数ミリメートルの透過)。
− 診断用X線(50〜150keV)。
− 6cmの組織厚さまで透過できる200〜500keVのX線(正中電圧)。
− 1000keV〜25,000keVのX線(メガボルト)。例えば、前立腺癌の治療のためのナノ粒子の励起は、15,000keVのエネルギーを有する5つの集束X線で行うことができる。
機能化された界面活性剤(Y−AOT3、Eu−AOT3、およびGd−AOT3)から、エルビウム又はガドリニウムがドープされているY2O3ナノ粒子を合成した。好適な界面活性剤混合物(所望の最終濃度に基づく[Eu−AOT3]/[Y−AOT3]=0.01;0.05;0.1;0.15)をイソオクタン又はシクロヘキサン中に分散させた。ミセル形成を促進するため水を添加した。得られる材料のサイズに影響を与えるミセルサイズを、混合物に添加する水の量で制御した。塩基を添加することにより水酸化物を形成した。次いで、水/エタノール混合物で粒子を洗浄し、乾燥させ、800℃で加熱し、結晶性ナノ粒子を形成した。
水性媒体中におけるハフニウム(HfOCl2,8H2O)および非晶質ゲルマニウム(GeO2)塩の単純な共沈により、コア材料、HfGeO4を合成した。1100℃又はそれより低温で4時間〜10時間熱処理した後、HfGeO4をナノ粒子の形態で結晶化させた。
シリカがコーティングされたナノ粒子の生体適合性および試験管内での無毒性を、試験管内で細胞株MCF7、KBおよびUClで試験した。ナノ粒子(粒子30〜1000pg/細胞1000個)を前記細胞と一緒に24時間、48時間、および72時間インキュベートした。細胞生存を以下のように評価した:
表面レセプタによる細胞内への粒子(表面ターゲティング成分を有する)のターゲティングおよび特異的透過を、共焦点レーザー走査顕微鏡で観察した。(レビー(Levy)ら、化学材料2002年、14(9)、3715頁;ナノケミストリー:「生物学的用途のための多官能性ナノクリニックの合成およびキャラクタリゼーション」(Chem. Mater. 2002, 14(9), pp3715;Nanochemistry:“Synthesis and Characterization of Multifunctional Nanoclinics for Biological Applications”)に記載されるように)ナノ粒子をシリカでコーティングし、化学結合によりLHRHで機能化した。ナノ粒子をMCF7細胞(LHRHレセプタを有する)と一緒に24時間インキュベートし、共焦点レーザー走査顕微鏡で観察した。24時間後に記録された画像に対応する図5は、細胞膜および核中のナノ粒子の蓄積を示す。
等張液(PBS、塩水)中に1〜20mg/mlの範囲の濃度でナノ粒子を分散させ、0.5mlの容積で、静脈、腫瘍内、又は腹腔内経路で注入した。注入の24時間〜48時間後、以下のように動物をX線に曝露させた:
− 転移の診断又は治療のために全身。標準的なX線撮影装置でX線を発生させることができる。
− 固形腫瘍又は特定の身体部位の治療のために集中(focused)。
− 1回注入した後、複数回X線に曝露、
− 複数回(数週間空けて)注入した後、それぞれ1回又は複数回曝露、
− 複数回(数日空けて)注入した後、1回又は複数回曝露。
Claims (31)
- X線で励起された場合に、フリーラジカルを発生させ得る、生体適合性複合粒子又はナノ粒子凝集体であって、
X線を吸収し、紫外−可視エネルギーを放射する第1の無機化合物、および、紫外−可視エネルギーを吸収し、水又は酸素と接触してフリーラジカルを生成する第2の無機又は有機化合物を含む核
を含む、生体適合性複合粒子又はナノ粒子凝集体。 - さらに、生体適合性コーティングを含む、請求項1に記載の粒子又はナノ粒子凝集体。
- サイズが4〜250nmであることを特徴とする、請求項1又は2に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物は、希土類元素でドープされている酸化物、水酸化物、酸硫化物又は塩の形態であることを特徴とする、請求項1〜3のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物は、Gd、Eu、Tb、Er、Nb、Pr、およびCeからなる群から選択される希土類元素でドープされているY2O3、(Y,Gd)2O3、CaWO4、GdO2S、LaOBr、YTaO3、BaFCl、Gd2O2S、Gd3Ga5O12、HfGeO4、Rb3Lu(PO4)2、およびCs3Lu(PO4)2からなる群から選択されることを特徴とする、請求項1〜4のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物が、Gd、Eu又はTbでドープされているY2O3からなる群から選択されることを特徴とする、請求項5に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物が、Zrを有する混合溶液中のHfGeO4であることを特徴とする、請求項5に記載の粒子又はナノ粒子凝集体。
- 前記第2の化合物が、半導体化合物から選択される無機化合物であることを特徴とする、請求項1〜7のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 無機化合物がドープされている、請求項8に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物が前記核のコアを形成し、前記第2の化合物が前記コアの表面で層又はナノ粒子を形成することを特徴とする、請求項1〜9のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記核の2種類の無機化合物が、複数の連続した層に配置されていることを特徴とする、請求項1〜10のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記第1の無機化合物によって形成される前記核のコアのサイズが、5〜50nmであり、前記コアの表面に前記第2の化合物によって形成される層の厚さが1〜30nmであることを特徴とする、請求項11に記載の粒子又はナノ粒子凝集体。
- 前記コアの2種類の化合物が、ナノ粒子混合物の形態で存在することを特徴とする、請求項1〜10のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記第2の化合物に対する前記第1の化合物の量又は濃度の比が、0.2〜5であることを特徴とする、請求項1〜13のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 生体組織又は細胞の特異的ターゲティングを可能にする表面成分を更に含むことを特徴とする、請求項1〜14のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 小分子およびフリーラジカルの拡散を可能にするコーティングを含有することを特徴とする、請求項1〜15のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記コーティングが、多孔質非晶質又は結晶性構造で構成されることを特徴とする、請求項16に記載の粒子又はナノ粒子凝集体。
- 生体組織又は細胞の特異的ターゲティングを可能にする前記表面成分が、コーティングに結合していることを特徴とする、請求項15〜17のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 前記表面ターゲティング成分が、ペプチド、ポリペプチド、ヌクレオチド、ポリヌクレオチド、ホルモン、およびビタミンから選ばれるヒト又は動物の身体中に存在する分子に対する親和性を示す生物学的又は化学的構造であることを特徴とする、請求項15〜18のいずれか一項に記載の粒子又はナノ粒子凝集体。
- TiO2の層で被覆されているY2O3:Gdを含むコアと、SiO2をベースにするコーティングとを含むことを特徴とする、粒子又はナノ粒子凝集体。
- Y2O3:Tbのマイクロ粒子とTiO2のマイクロ粒子を含む核、およびデキストランをベースにするコーティングを含むことを特徴とする、粒子又はナノ粒子凝集体。
- 形状が球状であることを特徴とする、請求項1〜21のいずれか一項に記載の粒子又はナノ粒子凝集体。
- 粒子又は凝集体を形成するため、請求項1〜22に記載の2種類の化合物を混合する工程を含む、請求項1〜22のいずれか一項に記載の粒子又はナノ粒子凝集体の製造方法。
- さらに、粒子又は凝集体をコーティングする工程を含む、請求項23に記載の方法。
- 前記第1の無機化合物を含む前記粒子のコアを調製する工程、および
このようにして形成された前記コアを、前記第2の化合物を含む層で被覆する工程、
を含むことを特徴とする、請求項23又は24に記載の方法。 - 請求項1〜22のいずれか一項に記載の粒子又はナノ粒子凝集体を含む医薬又は診断用組成物。
- X線と組み合わせて標的細胞を破壊するための医薬品を製造するための、請求項1〜22のいずれか一項に記載の粒子又はナノ粒子凝集体、又は請求項26に記載の組成物の使用。
- 紫外線と組み合わせて表在又は体腔の標的細胞を破壊するための医薬品を製造するための、請求項1〜22のいずれか一項に記載の粒子又はナノ粒子凝集体、又は請求項26に記載の組成物の使用。
- X線又は紫外線と組み合わせて細胞、組織又は器官を検出又は視覚化するための作用剤を製造するための、請求項1〜22のいずれか一項に記載の粒子又はナノ粒子凝集体、又は請求項26に記載の組成物の使用。
- 前記標的細胞が癌細胞であることを特徴とする、請求項27、28又は29に記載の使用。
- 前記X線又は紫外線を前記医薬品または作用剤に適用するシステムが、放射線治療又は放射線撮影法である、請求項27〜30のいずれか一項に記載の使用。
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PCT/FR2005/001145 WO2005120590A1 (fr) | 2004-05-10 | 2005-05-09 | Particules activables, preparation et utilisations |
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