CATALYST AND PROCESS FOR THE PRODUCTION OF HYDROGEN FROM AMMONIA BORANES

摘要

The invention relates to a process for the preparation of a compound of formula (I) wherein at least one complex of formula (I) is reacted with at least one substrate of formula (II), R ²¹ R ²² NH-BHR ²³ R ²⁴ or a dimer, trimmer or tetramer species (II) linked via one or more bridging groups to form a fused cyclic dimer, trimmer or tetramer species, or a substrate comprising two, three or four substrates of formula (II) / RTI comprising contacting the substrate with a substrate comprising one, three, or four substrates, In the above formula (I) 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 the carbocyclic ring B and the substituent R ⁴ ; Each 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) In this formula, Y ² is a direct single bond or a double bond, or CR ¹⁸ ; R ^1, R ^2, R ^5-13 and R ^16-18 are each independently 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 on a solid support; Or two or more of said R ^1-13 and R ^16-18 groups are taken together with the carbon 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 _1-20 -alkyl, C _2-6 -alkenyl, C _2-6 -alkynyl, aryl, C _1-6 -haloalkyl, And a linker group optionally substituted on a solid support; The formula (II), R ²¹ R ²² in ^{NH-BHR 23 R 24, R} 21 to R ²⁴ are each independently H, C _1-6-alkyl, fluoro-substituted -C _1-6 - alkyl, C _6-14 -aryl and C _6-14 -aralkyl, or two of R ²¹ , R ²² , R ²³ and R ²⁴ are connected to form a C _3-10 -alkylene or C _3-10 -alkenylene group Form a cyclic group together with the nitrogen atom and / or the boron atom attached thereto; The bridging group is selected from straight or branched C _1-6 -alkylene, boron, C _6-14 -aryl and C _6-14-aralkyl optionally substituted with one or more fluoro groups. Further aspects of the present invention are directed to a hydrogen generating system comprising a complex of formula (I), a substrate of formula (II) and a solvent, and a complex of formula (I) in a fuel cell. Another aspect of the invention relates to novel complexes of formula (I).