Unprecedentedly High Formic Acid Dehydrogenation Activity on an Iridium Complex with an N,N′‐Diimine Ligand in Water |
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Authors: | Zhijun Wang Dr. Sheng‐Mei Lu Dr. Jun Li Dr. Jijie Wang Prof. Can Li |
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Affiliation: | 1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023 (China).;2. Graduate University of Chinese Academy of Sciences, Beijing 100049 (China) |
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Abstract: | 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 487 500 h?1 with [Cp*Ir( L1 )Cl]Cl ( L1 =2,2′‐bi‐2‐imidazoline) at 90 °C and a turnover number (TON) of 2 400 000 with in situ prepared catalyst from [IrCp*Cl2]2 and 2,2′‐bi‐1,4,5,6‐tetrahydropyrimidine ( L2 ) at 80 °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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Keywords: | dehydrogenation diimine ligand formic acid hydrogen iridium complex |
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