首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Selenium makes the difference: protonation of [FeFe]-hydrogenase mimics with diselenolato ligands
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Selenium makes the difference: protonation of [FeFe]-hydrogenase mimics with diselenolato ligands

机译:硒使得差异:[Fefe]的质子化 - 氢酶与蛋白质配体的模拟物

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摘要

The synthetic models of the active site of an [FeFe]-hydrogenase containing a Sn atom in the bridgehead of the diselenato ligand, namely [Fe-2(CO)(6){mu-(SeCH2Se)SnMe2}], 3 and [Fe-2(CO)(6){mu-(SeCH2)(2)SnMe2}], 4 have been synthesized and characterized by different spectroscopic methods. The protonation properties of complex 4 have been investigated by monitoring the IR spectra in the carbonyl stretching region, H-1 NMR in the hydride region as well as the Se-77{H} NMR upon addition of strong and moderate acids wherein the protonation of the active site of the [FeFe]-hydrogenase at one of its internal basic sites is considered an essential step in the catalytic cycle. Furthermore, we investigated the redox properties and the catalytic behaviour of complexes 3 and 4 in the presence of AcOH as a source of protons suggesting an ECE (E = electrochemical process, C = chemical process) mechanism.
机译:含有酪蛋白配体的桥头中含有Sn原子的氢原子的活性位点的合成模型,即[Fe-2(CO)(6){MU-(SECH2SE)SNME2}],3和[ Fe-2(CO)(6){MU-(SECH2)(2)SNME2}],4已经合成并通过不同的光谱方法表征。 通过监测碳基拉伸区域中的IR光谱,氢化物区域H-1nMR中的IR光谱以及在加入强且中等酸的情况下SE-77 {H} NMR来研究复合物4的质子化性质。 其内部基本位点之一的[FeFE] - 氢酶的活性位点被认为是催化循环中的重要步骤。 此外,我们研究了ACOH存在中络合物3和4的氧化还原性能和催化行为,作为构成ECE(E =电化学过程,C =化学过程)机制的质子的源。

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