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首页> 外文期刊>Chemistry: A European journal >Unprecedentedly High Formic Acid Dehydrogenation Activity on an Iridium Complex with an N,N'-Diimine Ligand in Water
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Unprecedentedly High Formic Acid Dehydrogenation Activity on an Iridium Complex with an N,N'-Diimine Ligand in Water

机译：具有N，N'-二胺配体的铱配合物在水中的空前高的甲酸脱氢活性

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摘要

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.
机译：甲酸（FA）脱氢制氢很有希望。当前大多数用于FA脱氢的催化剂仅在碱或添加剂存在下才有效。我们在这里报告了新开发的铱络合物，其中包含在水中不需添加碱或添加剂的情况下用于FA脱氢的共轭N，N-二亚胺配体。 [Cp * Ir（L1）Cl] Cl（L1 = 2,2-bi-2-咪唑啉）在90°C时的周转频率（TOF）为487500h（-1），而在[Cp * Ir（L1）Cl] Cl（L1 = 2,2-bi-2-咪唑啉）时的周转率（TON）为2400000从[IrCp * Cl-2]（2）和2,2-bi-1,4,5,6-四氢嘧啶（L2）上原位制备的催化剂在80摄氏度下获得，迄今为止报道的FA脱氢的最高值。机理研究表明，[Ir-H]中间物种的形成是催化循环中决定速率的步骤。

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