期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 21, 期 36, 页码 12592-12595出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201502086
关键词
dehydrogenation; diimine ligand; formic acid; hydrogen; iridium complex
资金
- National Natural Science Foundation of China (NSFC) [21090340]
Hydrogen production from the dehydrogenation of formic acid (FA) is promising. Most of the current catalysts for FA dehydrogenation are effective only in the presence of bases or additives. We report here newly developed iridium complexes containing conjugated N,N-diimine ligands for FA dehydrogenation in water without the addition of bases or additives. A turnover frequency (TOF) of 487500h(-1) with [Cp*Ir(L1)Cl]Cl (L1=2,2-bi-2-imidazoline) at 90 degrees C and a turnover number (TON) of 2400000 with in situ prepared catalyst from [IrCp*Cl-2](2) and 2,2-bi-1,4,5,6-tetrahydropyrimidine (L2) at 80 degrees C were obtained, the highest values reported for FA dehydrogenation to date. A mechanistic study reveals that the formation of [Ir-H] intermediate species is the rate-determining step in the catalytic cycle.
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