催化作用
纳米技术
电解质
电催化剂
石墨烯
过渡金属
材料科学
无机化学
化学工程
组合化学
电化学
电极
选择性
化学
物理化学
有机化学
工程类
作者
Ana Sofía Varela,Matthias Kroschel,Nathaniel Leonard,Wen Ju,Julian Steinberg,Alexander Bagger,Jan Rossmeisl,Peter Strasser
出处
期刊:ACS energy letters
[American Chemical Society]
日期:2018-03-05
卷期号:3 (4): 812-817
被引量:167
标识
DOI:10.1021/acsenergylett.8b00273
摘要
The electrochemical CO2 reduction reaction (CO2RR) is a promising route for converting CO2 and excess renewable energy into valuable chemicals and synthetic fuels. Recently, carbon-based solid materials containing dopant-levels of transition metal and nitrogen (M–N–C) have emerged as a cost-effective, energy-efficient catalyst for the direct coreduction of CO2 and H2O to CO. Fe–N–C catalysts are particularly interesting as they can reduce CO further to hydrocarbons. Despite these promising reports, the influence of the reaction conditions on the catalytic performance of Fe–N–C catalysts has not been addressed. Here, we study the role of the electrolyte on the CO2RR selectivity. Unlike hydrogen or methane generation, catalytic CO production is independent of the electrolyte pH on the normal hydrogen electrode potential scale, suggesting a decoupled elementary proton–electron transfer mechanism for CO formation. The similarity between this heterogeneous charge-transfer reaction mechanism and that of molecular metal–nitrogen porphyrin-type macrocyclic complexes strongly suggests that the carbon-embedded FeNx motifs of the solid-state electrocatalyst act as the primary catalytically active center and illustrates yet another example of unifying concepts between molecular and solid-state catalysis.
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