CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
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DOI：
10.1126/science.aas9100
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发表时间：
2018-05-18
期刊：
影响因子：
56.9
通讯作者：
Sargent, Edward H.
中科院分区：
文献类型：
--
作者：
Dinh, Cao-Thang;Burdyny, Thomas;Sargent, Edward H.
二氧化碳（CO2）电还原可以提供有用的乙烯源，但是低转化效率、低生产率和低催化剂稳定性限制了当前系统。在这里，我们报告说，铜电催化剂在碱性电解质中的突然反应界面还原CO2乙烯与70%的法拉第效率在-0.55伏的电位与可逆氢电极（RHE）。铜表面上或附近的氢氧离子降低了CO2还原和一氧化碳（CO）-CO偶联活化能垒;因此，乙烯在-0.165伏下的开始释放（相对于10摩尔氢氧化钾中的RHE）几乎与CO产生同时发生。通过引入基于聚合物的气体扩散层来增强操作稳定性，所述气体扩散层将反应界面夹在单独的疏水性和导电性载体之间，从而在最初的150个操作小时内提供恒定的乙烯选择性。
Carbon dioxide (CO2) electroreduction could provide a useful source of ethylene, but low conversion efficiency, low production rates, and low catalyst stability limit current systems. Here we report that a copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of -0.55 volts versus a reversible hydrogen electrode (RHE). Hydroxide ions on or near the copper surface lower the CO2 reduction and carbon monoxide (CO)-CO coupling activation energy barriers; as a result, onset of ethylene evolution at -0.165 volts versus an RHE in 10 molar potassium hydroxide occurs almost simultaneously with CO production. Operational stability was enhanced via the introduction of a polymer-based gas diffusion layer that sandwiches the reaction interface between separate hydrophobic and conductive supports, providing constant ethylene selectivity for an initial 150 operating hours.