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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Electrocatalysis of hydrogen production of active site analogues of the iron hydrogenase enzyme:structure/function relationships
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Electrocatalysis of hydrogen production of active site analogues of the iron hydrogenase enzyme:structure/function relationships

机译：铁氢化酶活性位点类似物的产氢电催化：结构/功能关系

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A series of binuclear Fe~IFe~I complexes,(mu-SEt)_2[Fe(CO)_2L]_2 (L=CO (1),PMe_3(1-P)),(mu-SRS)[Fe-(CO)_2L]_2 (R=CH_2CH_2 (mu-edt):L=CO (2),PMe_3(2-P);R=CH_2CH_2CH_2(mu-pdt):L=CO (3),PMe_3 (3-P);and R=o-CH_2C_6H_4CH_2 (mu-o-xyldt):L=CO (4),PMe_3 (4-P)),that serve as structural models for the active sites of Fe-hydrogenase are shown to be electrocatalysts for H_2 production in the presence of acetic acid in acetonitrile.The redox levels for H_2 production were established by spectroelectrochemistry to be Fe~0Fe~0 for the all-CO complexes and Fe~IFe~0 for the PMe_3-substituted derivatives.As electrocatalysts,the PMe_3 derivatives are more stable and more sensitive to acid concentration than the all-CO complexes.The eoectrocatalysis initiated by electrochemical reduction of these diiron complexes,which subsequently,under weak acid conditions,undergo protonation of the reduced iron center to produce H_2.An(eta~2-H_2)Fe~(II)-Fe~(o/I) intermediate is suggested and probable electrochemical mechanisms are discussed.
机译：一系列双核Fe〜IFe〜I配合物，（mu-SEt）_2 [Fe（CO）_2L] _2（L = CO（1），PMe_3（1-P）），（mu-SRS）[Fe-（ CO）_2L] _2（R = CH_2CH_2（mu-edt）：L = CO（2），PMe_3（2-P）; R = CH_2CH_2CH_2（mu-pdt）：L = CO（3），PMe_3（3-P ）;并且R = o-CH_2C_6H_4CH_2（mu-o-xyldt）：L = CO（4），PMe_3（4-P））被证明是Fe-加氢酶活性位点的结构模型在乙腈中存在乙酸的情况下生成H_2。通过光谱电化学将H_2生成的氧化还原水平确定为全CO配合物为Fe〜0Fe〜0，而被PMe_3-取代的衍生物为Fe〜IFe〜0。 PME_3衍生物比全CO配合物更稳定，对酸浓度更敏感。通过电化学还原这些二铁配合物引发的电催化，随后在弱酸条件下对还原的铁中心进行质​​子化生成H_2。建议使用（η〜2-H_2）Fe〜（II）-Fe〜（o / I）中间体，可能的电化学方法讨论机制。

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