In the current environmental and economic context, there is an urgent need to develop catalytic systems to efficiently activate and transform abundant small molecules while demonstrating selectivity when multielectron processes are involved. This is especially true for catalytic production of CH₄ from CO₂, as a limited number of active photo- or electro-catalysts have been described to date. Herein, we report the unprecedented reactivity of a molecular electrocatalyst physiadsorbed on a graphite electrode: the bioinspired [L^N2S2Ni^IIFe^IICp(CO)]⁺ (L^N2S2 = 2,2′-(2,2′-bipryridine-6,6′-diyl)bis(1,1′-diphenylethanethiolate) complex selectively and catalytically reduces CO₂ in acidic aqueous solution to produce a mixture of CH₄ and H₂. Under optimized conditions, at pH 4, Faradaic yields of 12% and 66% for CH₄ and H₂ production (TOF_CH4 = 214 s^–1, TOF_H2 ≈ 5.1 × 10³ s^–1) are measured, respectively. We demonstrate that this binuclear NiFe catalyst is stable for hours under controlled potential electrolysis conditions.

中文翻译：

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重新利用生物启发的NiFe加氢酶模型来减少CO ₂并选择性生产甲烷作为独特的基于C的产品

在当前的环境和经济背景下，当涉及多电子过程时，迫切需要开发催化系统以有效地活化和转化丰富的小分子同时表现出选择性。这对于从CO ₂催化生产CH ₄尤其如此，因为迄今为止已描述了有限数量的活性光催化剂或电催化剂。此，我们报告的分子电催化剂physiadsorbed的前所未有的反应性上的石墨电极：该仿生[L ^N2S2镍^II的Fe ^II CP（CO）] ⁺（L ^N2S2= 2,2'-（2,2'-联吡啶-6,6'-二基）双（1,1'-二苯乙硫醇酯）络合物在酸性水溶液中选择性地催化还原CO ₂以生成CH ₄和H的混合物₂。在优化条件下，在pH为4，12％的产率法拉第和CH 66％₄和H ₂生产（TOF _{CH 4} = 214小号^-1，TOF _{ħ 2} ≈5.1×10 ³小号^-1）分别测量。我们证明了这种双核NiFe催化剂在受控电位电解条件下可稳定保持数小时。