High-Curvature Transition-Metal Chalcogenide Nanostructures with a Pronounced Proximity Effect Enable Fast and Selective CO2 Electroreduction
Angewandte Chemie International Edition 59(22):8706-8712 May 2020 

Gao, Fei-Yue; Hu, Shao-Jin; Zhang, Xiao-Long; Zheng, Ya-Rong; Wang, Hui-Juan; Niu, Zhuang-Zhuang; Yang, Peng-Peng; Bao, Rui-Cheng; Ma, Tao; Dang, Zheng; Guan, Yong; Zheng, Xu-Sheng; Zheng, Xiao; Zhu, Jun-Fa; Gao, Min-Rui; Yu, Shu-Hong


A considerable challenge in the conversion of carbon dioxide into useful fuels comes from the activation of CO2 to CO2 .- or other intermediates, which often requires precious-metal catalysts, high overpotentials, and/or electrolyte additives (e.g., ionic liquids). We report a microwave heating strategy for synthesizing a transition-metal chalcogenide nanostructure that efficiently catalyzes CO2 electroreduction to carbon monoxide (CO). We found that the cadmium sulfide (CdS) nanoneedle arrays exhibit an unprecedented current density of 212 mA cm-2 with 95.5±4.0 % CO Faraday efficiency at -1.2 V versus a reversible hydrogen electrode (RHE; without iR correction). Experimental and computational studies show that the high-curvature CdS nanostructured catalyst has a pronounced proximity effect which gives rise to large electric field enhancement, which can concentrate alkali-metal cations resulting in the enhanced CO2 electroreduction efficiency.


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