期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 6, 页码 7030-7037出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b15685
关键词
CO2 electroreduction; Cu2O/Cu; nitrogen-doped carbon frameworks; core-shell structure; formate selectivity; durability
资金
- National Key R&D Program of China [2016YFE0106500]
- China Postdoctoral Science Foundation [2017M621265]
- National Natural Science Fund of China [21673061, 51408156]
- European Union [2014DFE90110]
Copper-based metal-organic frameworks (MOFs) and their derivatives have been used for CO2 electroreduction; however, they still have obvious drawbacks like poor selectivity and durability. Here, Cu_btc (btc = benzene-1,3,5-tricarboxylate)-derived Cu2O/Cu anchored in a nitrogen-doped porous carbon framework (Cu2O/Cu@NC) was prepared for CO2 electroreduction. Cu2O/Cu@NC-800 (carbonizing Cu_btc at 800 degrees C) produced formate and ethanol concurrently with an overpotential as low as similar to 380 mV. However, it exhibited higher selectivity toward formate against ethanol, with the maximum formate faradaic efficiencies of 70.5% at -0.68 V vs a reversible hydrogen electrode (RHE), which was 1.79 and 1.84 times higher than that of Cu2O/Cu@NC-700 and Cu2O/Cu@NC-900. This superior performance remained stable for over 30 h. The enhancement in activity and selectivity was attributed to (i) a higher Cu content and well-dispersed Cu2O/Cu nanoparticles inside the carbon frameworks, which provided abundant active reaction sites, and (ii) a higher content of N doped into the Cu2O/Cu lattice to possibly facilitate *OCHO generation. These findings provided a convenient strategy to enhance the activity and selectivity of catalysts for efficient CO2 electroreduction.
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