N-modulated Cu0-Cu+ Sites for C1/C2 Selectivity Regulation of Carbon Dioxide Electrocatalytic Reduction
Journal of Alloys and Compounds(2024)
摘要
Controlling the valence states of copper is pivotal in determining the selectivity of products in CO2 electroreduction. In this study, we developed a Cu doped carbon catalyst (CuNC) derived from a metal-organic framework (MOFs) through a straightforward solution reaction and calcination method. The N-modulated Cu0-Cu+ sites exhibited adjustable C1 and C2 selectivity in electrocatalytic CO2 reduction (CER). Specifically, the CuNC-700 demonstrated an impressive C2 Faradaic efficiency (FE) of 56.0% at -1.0V vs reversible hydrogen electrode (RHE), and a remarkable C1 FE of 56.7% with a total current density of 600mA/cm2 at -1.6V vs RHE. In the entire potential range, the CuNC-700 consistently maintained high FE values of > 92% for CER, while the FE values for hydrogen evolution reaction is below 8%. This study unveiled the correlation between the selectivity and the valence states of copper. At low applied potentials, the abundance of N-modulated Cu0-Cu+ sites led to the predominant production of the C2 products. The Cu0 played a primary role in activating CO2 and facilitating subsequent electron transfer, while the Cu+ enhanced the adsorption of *CO, further promoting the C-C coupling. Under high applied potentials, both Cu2+ and Cu+ were converted to Cu0, favoring the methanation process. This research paves the way for future design of Cu-based MOF-derived materials, enabling precise regulation of C1/C2 selectivity in CER.
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关键词
Selectivity regulation,Carbon dioxide,MOF,Valence states of copper
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