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首页> 外文期刊>Chemistry: A European journal >Electrochemical insights into the mechanisms of proton reduction by [Fe-2(CO)(6){mu-SCH2N(R)CH2S}] complexes related to the [2Fe](H) subsite of [FeFe]hydrogenase
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Electrochemical insights into the mechanisms of proton reduction by [Fe-2(CO)(6){mu-SCH2N(R)CH2S}] complexes related to the [2Fe](H) subsite of [FeFe]hydrogenase

机译：电化学洞察[Fe-2（CO）（6）{mu-SCH2N（R）CH2S}]络合物与[FeFe]氢化酶[2Fe]（H）亚位点相关的质子还原机理

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摘要

Electrochemical investigations on a structural analogue of the [2Fe](H) subsite of [FeFe]H-2 ases, namely, [Fe-2(CO)(6){mu-SCH2N(CH2CH2OCH3)CH2S}] (1), were conducted in MeCN/NBu4PF6 in the presence of HBF4/Et2O or HOTS. Two different catalytic proton reduction processes operate, depending on the strength and the concentration of the acid used. The first process, which takes place around -1.2 V for both HBF4/Et2O and HOTS, is limited by the slow release of H-2 from the product of the {2H(+)/2e} pathway, 1-2H. The second catalytic process, which occurs at higher acid concentrations, takes place at different potentials depending on the acid present. We propose that this second mechanism is initiated by protonation of 1-2H when HBF4/Et2O is used, whereas the reduction of 1-2H is the initial step in the presence of the weaker acid HOTS. The potential of the second process, which occurs around -1.4V (reduction potential of 1-3H(+)) or around -1.6V (the reduction potential of 1-2H) is thus dependent on the strength of the available proton source.
机译：[FeFe] H-2的[2Fe]（H）子位点的结构类似物，即[Fe-2（CO）（6）{mu-SCH2N（CH2CH2OCH3）CH2S}]的电化学研究，（1），在HBF4 / Et2O或HOTS存在下于MeCN / NBu4PF6中进行。根据所用酸的强度和浓度，有两种不同的催化质子还原过程。对于HBF4 / Et2O和HOTS来说，第一个过程发生在-1.2 V左右，但受到{-2H（+）/ 2e}途径1-2H产物H-2缓慢释放的限制。第二催化过程在较高的酸浓度下发生，取决于存在的酸在不同的电势下发生。我们建议，当使用HBF4 / Et2O时，第二个机理是由1-2H的质子化引发的，而在弱酸HOTS存在下，1-2H的还原是起始步骤。因此，第二个过程的电势大约在-1.4V（1-3H（+）的还原电势）或-1.6V（1-2H的还原电势）左右，取决于可用质子源的强度。

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