催化作用
介孔材料
电解
氧化物
产品分销
化学工程
氢
材料科学
格式化
无机化学
可逆氢电极
选择性
电极
化学
电化学
工作电极
电解质
物理化学
冶金
有机化学
工程类
作者
Abhijit Dutta,Motiar Rahaman,N. Luedi,Miklós Mohos,Peter Broekmann
标识
DOI:10.1021/acscatal.6b00770
摘要
Mesoporous Cu foams formed by a template-assisted electrodeposition process have been identified as CO2 electrocatalysts that are highly selective toward C2 product formation (C2H4 and C2H6) with C2 efficiencies (FEC2) reaching 55%. The partial current of C2 product formation was found to be higher than that of the (parasitic) hydrogen evolution reaction (HER) at any potential studied (−0.4 to −1.0 vs the reversible hydrogen electrode). Moreover, formate production could largely be suppressed at any applied potential down to efficiencies (FEformate) of ≤6%. A key point of the Cu foam catalyst activation is the in operando reduction of a Cu2O phase, thereby creating a large abundance of surface sites active for C–C coupling. The cuprous oxide phase has been formed after the Cu electrodeposition step by exposing the large-surface area catalyst to air at room temperature. The superior selectivity of the Cu foam catalyst studied herein originates from a combination of two effects, the availability of specific surface sites for C–C coupling [dominant (100) surface texture] and the temporal trapping of gaseous intermediates (in particular CO and C2H4) inside the mesoporous catalyst material during CO2 electrolysis. A systematic CO2 electrolysis study reveals a strong dependence of the C2 efficiencies on the particular surface pore size of the mesoporous Cu catalysts with a maximal FEC2 between 50 and 100 μm pore diameters.
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