TW477083B - Polymer electrolyte membrane for use in lithium batteries - Google Patents
Polymer electrolyte membrane for use in lithium batteries Download PDFInfo
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- TW477083B TW477083B TW089122360A TW89122360A TW477083B TW 477083 B TW477083 B TW 477083B TW 089122360 A TW089122360 A TW 089122360A TW 89122360 A TW89122360 A TW 89122360A TW 477083 B TW477083 B TW 477083B
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- 229910052744 lithium Inorganic materials 0.000 title claims description 6
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims description 4
- 239000012528 membrane Substances 0.000 title abstract description 5
- 239000005518 polymer electrolyte Substances 0.000 title 1
- 239000000203 mixture Substances 0.000 claims abstract description 14
- 229920002239 polyacrylonitrile Polymers 0.000 claims abstract description 10
- 239000002033 PVDF binder Substances 0.000 claims abstract description 7
- 229910010293 ceramic material Inorganic materials 0.000 claims abstract description 7
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims abstract description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 5
- 229920003229 poly(methyl methacrylate) Polymers 0.000 claims abstract description 5
- 229920000642 polymer Polymers 0.000 claims abstract description 5
- 239000004926 polymethyl methacrylate Substances 0.000 claims abstract description 5
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000002202 Polyethylene glycol Substances 0.000 claims abstract description 3
- 229920001223 polyethylene glycol Polymers 0.000 claims abstract description 3
- 229920000915 polyvinyl chloride Polymers 0.000 claims abstract description 3
- 239000004800 polyvinyl chloride Substances 0.000 claims abstract description 3
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims abstract description 3
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims abstract description 3
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims abstract description 3
- 125000004386 diacrylate group Chemical group 0.000 claims abstract 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims abstract 2
- -1 Polyethylene Polymers 0.000 claims description 6
- 230000002079 cooperative effect Effects 0.000 claims description 5
- 239000004698 Polyethylene Substances 0.000 claims description 2
- 229920000573 polyethylene Polymers 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 claims 1
- UOUJSJZBMCDAEU-UHFFFAOYSA-N chromium(3+);oxygen(2-) Chemical group [O-2].[O-2].[O-2].[Cr+3].[Cr+3] UOUJSJZBMCDAEU-UHFFFAOYSA-N 0.000 claims 1
- 239000011159 matrix material Substances 0.000 claims 1
- 239000002159 nanocrystal Substances 0.000 claims 1
- 230000003647 oxidation Effects 0.000 claims 1
- 238000007254 oxidation reaction Methods 0.000 claims 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 abstract 1
- 229910052814 silicon oxide Inorganic materials 0.000 abstract 1
- 150000003457 sulfones Chemical class 0.000 abstract 1
- 229920002554 vinyl polymer Polymers 0.000 abstract 1
- 229910001928 zirconium oxide Inorganic materials 0.000 abstract 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 6
- 239000000919 ceramic Substances 0.000 description 5
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 5
- 239000003792 electrolyte Substances 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- 229910001416 lithium ion Inorganic materials 0.000 description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 3
- 229910003002 lithium salt Inorganic materials 0.000 description 3
- 159000000002 lithium salts Chemical class 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 2
- 229910052693 Europium Inorganic materials 0.000 description 2
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- BGTOWKSIORTVQH-UHFFFAOYSA-N cyclopentanone Chemical compound O=C1CCCC1 BGTOWKSIORTVQH-UHFFFAOYSA-N 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 230000002687 intercalation Effects 0.000 description 2
- 238000009830 intercalation Methods 0.000 description 2
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 description 2
- 239000003586 protic polar solvent Substances 0.000 description 2
- 239000012266 salt solution Substances 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 1
- VWIIJDNADIEEDB-UHFFFAOYSA-N 3-methyl-1,3-oxazolidin-2-one Chemical compound CN1CCOC1=O VWIIJDNADIEEDB-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 1
- 229910013131 LiN Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 229910013880 LiPF4 Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000000010 aprotic solvent Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 239000001273 butane Substances 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 1
- 108010025899 gelatin film Proteins 0.000 description 1
- 229910000449 hafnium oxide Inorganic materials 0.000 description 1
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical compound [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 description 1
- 230000003100 immobilizing effect Effects 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- 239000010410 layer Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- IHLVCKWPAMTVTG-UHFFFAOYSA-N lithium;carbanide Chemical compound [Li+].[CH3-] IHLVCKWPAMTVTG-UHFFFAOYSA-N 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 1
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000005022 packaging material Substances 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229910052573 porcelain Inorganic materials 0.000 description 1
- 150000003282 rhenium compounds Chemical class 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/20—Manufacture of shaped structures of ion-exchange resins
- C08J5/22—Films, membranes or diaphragms
- C08J5/2206—Films, membranes or diaphragms based on organic and/or inorganic macromolecular compounds
- C08J5/2218—Synthetic macromolecular compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/14—Dynamic membranes
- B01D69/141—Heterogeneous membranes, e.g. containing dispersed material; Mixed matrix membranes
- B01D69/1411—Heterogeneous membranes, e.g. containing dispersed material; Mixed matrix membranes containing dispersed material in a continuous matrix
- B01D69/14111—Heterogeneous membranes, e.g. containing dispersed material; Mixed matrix membranes containing dispersed material in a continuous matrix with nanoscale dispersed material, e.g. nanoparticles
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/14—Dynamic membranes
- B01D69/141—Heterogeneous membranes, e.g. containing dispersed material; Mixed matrix membranes
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Manufacturing & Machinery (AREA)
- Dispersion Chemistry (AREA)
- Nanotechnology (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Health & Medical Sciences (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Secondary Cells (AREA)
Description
477083 A7 _ B7 五、發明說明(1 ) 本發明係有關於供用於電化學電池之包括陶瓷物質的 凝膠狀膜。 鋰離子電池已成爲最被看好的行動應用上之電池系統 。其應用範圍涵蓋高階電子設備(例如,行動電話、攝錄 影機),以至於電動車輛用之電池。 此類電池係由陰極、陽極、隔離物以及非水_性之*解 質所構成。具代表性之陰極包括L i ( Μ η M e Z ) 2〇4 ,Li (CoMez)〇2, Li (CoNixMez) 〇2 或其它鋰層閭化合物以及嵌插化合物。陽極則可以係鋰金 屬,碳,石墨,石墨碳或其它鏵層.間化合物以及嵌插化合 物或合金。至於電解質,則使用鋰鹽溶液,例如, LiPF^LiPF4>LiCl〇4^LiAsF6^ LiCF3S〇3,LiN (CF3S〇2)2 或 L i C ( C F 3 S〇2 ) 3,以及以上這些的混合物,在無 質子溶劑中之溶液。 已知之凝膠狀膜,有以將液態鋰鹽溶液(例如,溶解 1在有機溶劑之混合物中的鋰鹽)固定化而製成者。日本專 利J P 1 028409 1號揭示有供用於鋰離子電池中 之,以聚丙烯腈(PAN)以及聚偏二氟乙烯(PVDF )製成之聚合物膜。Abraham等人(Electrochim. Acta, 1998,2399-2412)發表一種電池原型,係 以Li Mn2〇4爲陰極,以石墨爲陽極,並包括基於聚丙 敏Jt之電解質。這些電池在室溫底下均具有、良好之電傳導 性。 本紙張尺度適用中國國家標準(CNS)A4規格(210 X 297公釐) (請先閱讀背面之注意事項再填寫本頁) 訂---------線‘ 經濟部智慧財羞局員工消費合作社印製 -4- 477083 -……............ _ Sim 2ίν. 丨附件一:第89122360號專利申請案中文說明書修正頁 ! 民國90年12月呈 五、發明説明(2 ) 上述之膜在室溫底下具有在1 〇 — 3 s c m — 1之程度的 離子電導係數。然而,其共通特點爲,當溫度在室溫以上 時,化學穩定性以及機械穩定性差。
Scrosati ( Solid State Ionic Mater., 1 9 9 4, 1 1 1 - 1 1 7 )敘述沸石在凝膠狀膜中之利用,並針對 該膜對於鋰金屬之影響作探討。
Appetecchi 等人(J. Electrochem. Soc., 1 9 9 8, 4 1 2 6 — 4 1 3 2 )利用諸如r — L i A 1〇2之陶瓷粉 末添加於聚氧化乙烯基體,以期降低鋰的鈍化之增進趨勢 。然而,該混合物具有二個嚴重的缺點。其最適操作溫度 過高,係在80 °C ;而其電導係數又過低,僅及0 · 6至 1·〇χ10— 4Scm 一 匕 因此,本發明之目的,係在提供一種具有改良之穩定 性以及鋰離子電傳導性之電解質。 本發明之目的係藉由利用基於聚合物之凝膠狀膜加以 達成,該聚合物係選自以聚丙烯腈、聚甲基丙烯酸甲酯、 聚氯乙烯、聚乙烯硕、聚乙二醇二丙烯酸酯、聚乙烯吡咯 烷酮、聚偏二氟乙烯所構成之群組或其混合物,並包括選 自以氧化鋁、氧化矽、氧化鈦以及氧化鍩所構成之群組的 陶瓷材料以及其混合物加以達成。 過去已有發現,奈米結晶陶瓷粉末之添加,可以導致 整體穩定性之提升。該奈米結晶陶瓷粉末係以佔該膜的重 量的1至9 %之比例添加,而較佳之比例爲5至7 %之間 。所有習知之,供用於電化學電池的具有導電性之鹽類以 本紙張尺度適用中國國家標準(CNS ) A4規格(210X297公釐) (請先閲讀背面之注意事項再填寫本頁) 衣· !訂! 經濟部智慧財產局員工消費合作社印製 -5- 477083 A7
及溶劑,均可用作電解質。所用之電解質可以作L· i f / 6 ’ LiBF4,LiCl〇4,LiAsF6, LiCF3S〇3,LiN (CF3S〇2) 2 或 L i C ( C F 3 S〇2 ) 3,以及以上這些的混合物在非質 子溶劑中所形成的溶液。而非質子溶劑可以係諸如E C, DMC,P〜C,DEC,BC,VC,環戊酮類,硕戊環 類,DMS,3 —甲基一 1 ,3 —噁唑烷一 2 —酮,γ -丁內酯 ’ EMC,MPC,BMC,EPC,BEC, DPC,一乙氧甲院,丁 HF,2 —甲基四氫d夫喃,1 , 3 -二氧雜戊環,醋酸甲酯,醋酸乙酯以及其混合物。 以下說明本發明之一通例。 理論上,依據導電性鹽類之組成,有二種臆可供使用 ,即LiPF6或LiCl〇4在碳靡乙二J享酯—碳酸二甲 酯(E C / D M C )混合物中之溶液,或 L i C (CF3S〇2) 3 (甲基鋰化物)在EC/DMC 混合物中之溶液。 尤爲適當之凝膠狀膜,係基於聚丙烯腈(PAN), 聚甲基丙烯酸甲酯(PM Μ A),或聚偏二氟乙烯者。也 使用奈米結晶陶瓷粉末,係以A 1 2〇3之使用爲特佳。 針對電導係數之探討,係利用聚丙烯腈(P A N )膜 ,及L 1 PF6作爲導電性鹽類,以及碳酸乙二醇_ (EC )與碳酸二甲酯(D M C )作爲溶廣!j。該膜之電導係數係 在高览室溫之溫度下量測,以在4 〇 °C與8 0 °C之間爲佳 ,爲時1600小時,以與由PAN,L i PF6,EC/ 本紙張尺度適用中國國家標準(CNS)A4規格(210 X 297公釐) (請先閱讀背面之注意事項再填寫本頁) -___I l· I I I ^ . I-_______. 經濟部智慧財產局員工消費合作社印製 -6- 477083 A7 ------- B7_____ 五、發明說明(4) DMC以及A 1 2〇3所構成之膜作比較。在不含·瓷塡充 材料之膜的情況下,發現在8 0 0小時之後即有嚴重之劣 化。而在經A 1 2 0 3塡充之膜的情況下,可以觀察到電導 係數能夠維持固定不變。 這些凝膠狀膜可以供用於電化學電池,尤其以供用於 電池爲佳,而係以供用於遨離子電池爲特佳。 (請先閱讀背面之注意事項再填寫本頁) 訂----------% 經濟部智慧財產局員工消費合作社印製 本紙張尺度適用中國國家標準(CNS)A4規格(210 X 297公釐)
Claims (1)
- 477083 A8B8C8D8 經濟部智慧財產局員工消費合作社印製 六、申請專利範圍 1 · 一種基於聚合物之凝膠狀膜,該聚合物係選自以 聚丙烯腈,聚甲基丙烯酸甲酯,聚氯乙烯,聚乙烯碾,聚 乙二醇二丙烯酸酯,聚乙烯吡咯烷酮,聚偏二氟乙烯所構 成之群組或其混合物,並包括選自以氧化鋁,氧化矽,氧 化鈦以及氧化鉻所構成之群組的陶瓷材料以及其混合物。 2 ·如申請專利範圍第1項之凝膠狀膜,其中其包括 奈米結晶。 3 ·如申請專利範圍第1項之凝膠狀膜,其中陶瓷材 料的濃度係佔該膜重量的1至9 %。 4 ·如申請專利範圍第1項之凝膠狀膜,其中該陶瓷 材料的濃度係佔該膜重量的5至7 %。 5 ·如申請專利範圍第1項之凝膠狀膜,其中使用聚 丙烯腈、聚甲基丙烯酸甲酯、聚偏二氟乙烯或其混合物作 爲聚合物基體,使用氧化轉作爲啜瓷材料。 6 ·如申請專利範圍第1至5項中任一項的凝膠狀膜 ,其中該膜在4 0 °C至8 0 t間之溫度下可用於I定電傳 導性。 7 .如申請專利範圍第1至5項中任一項的凝膠狀膜 ,其中該膜可用於電化學電池。 8 .如申請專利範圍第7項之凝膠狀膜,其中該膜可 供用於電池,包含二次鋰電池。 本紙張尺度適用中國國家標準(CNS)A4規格(210 X 297公釐) --丨丨丨丨I丨—•丨丨·丨丨丨丨丨丨丨訂·u丨丨II丨丨 · (請先閲讀背面之注意事項再填寫本頁) -8-
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19951872A DE19951872A1 (de) | 1999-10-28 | 1999-10-28 | Polymer Elektrolyt-Membran zum Einsatz in Lithium Batterien |
Publications (1)
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TW477083B true TW477083B (en) | 2002-02-21 |
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Application Number | Title | Priority Date | Filing Date |
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TW089122360A TW477083B (en) | 1999-10-28 | 2000-10-24 | Polymer electrolyte membrane for use in lithium batteries |
Country Status (2)
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DE (1) | DE19951872A1 (zh) |
TW (1) | TW477083B (zh) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
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KR100659820B1 (ko) | 2004-11-17 | 2006-12-19 | 삼성에스디아이 주식회사 | 리튬 이온 이차 전지 |
IT201800010452A1 (it) | 2018-11-20 | 2020-05-20 | Univ Degli Studi G Dannunzio | Materiali nanocompositi elettrofilati a base cu2o/carbone come anodi per batterie a litio |
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1999
- 1999-10-28 DE DE19951872A patent/DE19951872A1/de not_active Withdrawn
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2000
- 2000-10-24 TW TW089122360A patent/TW477083B/zh not_active IP Right Cessation
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