| abstract |
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). |