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标题翻译：处理

公开(公告)号：WO2014174465A2

公开(公告)日：2014-10-30

申请号：PCT/IB2014/060946

申请日：2014-04-23

申请人： NOVAUCD

发明人： PHILLIPS, Andrew , GRAVE, Christian , BINDRA, Gurmeet Singh , O'CONNOR, Crystal , KHLEBNIKOV, Vsevolod

IPC分类号： B01J31/18

CPC分类号： H01M8/0612 , B01J19/24 , B01J31/0237 , B01J31/0272 , B01J31/0275 , B01J31/146 , B01J31/1805 , B01J31/184 , B01J31/189 , B01J31/2243 , B01J31/226 , B01J31/2295 , B01J31/2404 , B01J2219/00164 , B01J2219/24 , B01J2231/76 , B01J2531/0241 , B01J2531/0255 , B01J2531/821 , B01J2531/825 , B01J2531/842 , B01J2531/845 , B01J2531/847 , C01B3/04 , C01B3/06 , C07F15/002 , C07F15/0026 , C07F15/0046 , C07F15/0053 , H01M8/10 , H01M2008/1095 , Y02E60/324 , Y02E60/364

摘要： The present invention relates to a process for the production of hydrogen comprising contacting at least one complex of formula (I), (I) wherein: X - is an anion; M is a metal selected from Ru, Os, Fe, Co and Ni; D is optionally present and is one or more monodentate or multidentate donor ligands; Y 1 is selected from CR 13 , B and N; Z 1 and Z 2 are each independently selected from =N, =P, NR 14 , PR 15 , O, S and Se; or Z 2 is a direct bond between carbocyclic ring B and substituent R 4 ; each of A and B is independently a saturated, unsaturated or partially unsaturated carbocyclic hydrocarbon ring; R 3 and R 4 are each independently selected from H, C 1-6 -alkyl, aryl and C 1-6 -haloalkyl, and a linker group optionally attached to a solid support; or R 3 and R 4 together form the following moiety: (AB) Y 2 is a direct single bond or double bond, or is CR 18 ; R 1 , R 2 , R 5-13 and R 16-18 are each independently selected from H, C 1-6 -alkyl, C 2-6 -alkenyl, C 2-6 -alkynyl, aryl, C 1-6 -haloalkyl, NR 19 R 20 and a linker group optionally attached to a solid support; or two or more of said R 1-13 and R 16-18 groups are linked, together with the carbons to which they are attached, to form a saturated or unsaturated hydrocarbon group; R 14 , R 15 , R 19 and R 20 are each independently selected from H, C 1-6 -alkyl, C 2-6 -alkenyl, C 2-6 -alkynyl, aryl, C 1-6 -haloalkyl, and a linker group optionally attached to a solid support; with at least one substrate of formula (II), R 21 R 22 NH-BHR 23 R 24, wherein R 21 to R 24 are each independently selected from H, C 1-6 -alkyl, fluoro- substituted C 1-6 -alkyl, C 6-14 -aryl and C 6-14 -aralkyl, or any two of R 21 , R 22 , R 23 and R 24 are linked to form a C 3-10 -alkylene group or C 3-10 -alkenylene group, which together with the nitrogen and/or boron atoms to which they are attached, forms a cyclic group; or a substrate comprising two, three or four substrates of formula (II) linked via one or more bridging groups so as to form a dimeric, trimeric or tetrameric species, and wherein the bridging group is selected from straight or branched C 1-6 -alkylene optionally substituted by one or more fluoro groups, boron, C 6-14 -aryl and C 6-14 -aralkyl; or a substrate comprising two, three or four substrates of formula (II) which are joined so as to form a fused cyclic dimeric, trimeric or tetrameric species. Further aspects of the invention relate to a hydrogen generation system comprising a complex of formula (I), a substrate of formula (II) and a solvent, and to the use of complexes of formula (I) in fuel cells. Another aspect of the invention relates to novel complexes of formula (I).

摘要翻译：本发明涉及一种生产氢的方法，包括使至少一种式（I），（I）的配合物与其中：X-是阴离子; M是选自Ru，Os，Fe，Co和Ni的金属; D任选存在并且是一个或多个单齿或多齿供体配体; Y1选自CR13，B和N; Z1和Z2各自独立地选自= N，= P，NR14，PR15，O，S和Se; 或Z2是碳环B和取代基R4之间的直接键; A和B各自独立地为饱和的，不饱和的或部分不饱和的碳环烃环; R 3和R 4各自独立地选自H，C 1-6 - 烷基，芳基和C 1-6 - 卤代烷基，和连接基团任选地连接到固体载体上; 或者R 3和R 4一起形成下列部分：（AB）Y 2是直接单键或双键，或是CR 18; R 1，R 2，R 5-13和R 16-18各自独立地选自H，C 1-6 - 烷基，C 2-6 - 烯基，C 2-6 - 炔基，芳基，C 1-6 - 卤代烷基，NR 19 R 20和任选地附着在坚实的支撑下; 或者所述R1-13和R16-18基团中的两个或更多个与它们所连接的碳一起连接形成饱和或不饱和烃基; R 14，R 15，R 19和R 20各自独立地选自H，C 1-6 - 烷基，C 2-6 - 烯基，C 2-6 - 炔基，芳基，C 1-6 - 卤代烷基和任选地连接到固体支持物 ; 与式（II）的至少一个底物R 21 R 22 NH-BHR 23 R 24，其中R 21至R 24各自独立地选自H，C 1-6 - 烷基，氟取代的C 1-6 - 烷基，C 6-14 - 芳基和C 6-14 - 烷基或R 21，R 22，R 23和R 24中的任何两个连接形成C 3-10 - 亚烷基或C 3-10亚烯基，它们与它们所连接的氮原子和/或硼原子一起形成环状基团或包含通过一个或多个桥连基团连接的二，三或四个式（II）底物的底物，以形成二聚，三聚或四聚物种，并且其中桥连基团选自直链或支链C 1-6 - 亚烷基任选被一个或多个氟基取代，硼，C 6-14 - 芳基和C 6-14 - 芳烷基; 或包含二，三或四个式（II）底物的底物，其被连接以形成稠合的环状二聚体，三聚体或四聚体物质。本发明的另外方面涉及包含式（I）的配合物，式（II）的底物和溶剂的氢生成系统，以及在燃料电池中使用式（I）的络合物。本发明的另一方面涉及式（I）的新型配合物。

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