纳米孪晶铜上 CO 电化学还原高效生成甲烷。
Highly Selective Electrochemical Reduction of CO into Methane on Nanotwinned Cu.
机构信息
Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, California 90095-1595, United States.
Department of Mechanical and Aerospace Engineering and the Andlinger Center for Energy and the Environment, Princeton University, Princeton, New Jersey 08544-5263, United States.
出版信息
J Am Chem Soc. 2023 Apr 26;145(16):9136-9143. doi: 10.1021/jacs.3c00847. Epub 2023 Apr 18.
The electrochemical carbon dioxide reduction reaction (CORR) is a promising route to close the carbon cycle by reducing CO into valuable fuels and chemicals. Electrocatalysts with high selectivity toward a single product are economically desirable yet challenging to achieve. Herein, we demonstrated a highly (111)-oriented Cu foil electrocatalyst with dense twin boundaries (TB) (tw-Cu) that showed a high Faradaic efficiency of 86.1 ± 5.3% toward CH at -1.2 ± 0.02 V vs the reversible hydrogen electrode. Theoretical studies suggested that tw-Cu can significantly lower the reduction barrier for the rate-determining hydrogenation of CO compared to planar Cu(111) under working conditions, which suppressed the competing C-C coupling, leading to the experimentally observed high CH selectivity.
电化学二氧化碳还原反应 (CORR) 是通过将 CO 还原为有价值的燃料和化学品来闭合碳循环的一种很有前景的途径。具有高选择性生成单一产物的电催化剂具有经济上的吸引力，但却难以实现。在此，我们展示了一种具有高密度孪晶界（TB）的高度（111）取向的铜箔电催化剂（tw-Cu），在-1.2 ± 0.02 V 相对于可逆氢电极时，其对 CH 的法拉第效率高达 86.1 ± 5.3%。理论研究表明，与工作条件下的平面 Cu(111)相比，tw-Cu 可以显著降低 CO 加氢反应的速率决定步骤的还原势垒，从而抑制了竞争的 C-C 偶联，导致实验观察到的高 CH 选择性。
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