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High-Curvature Transition-Metal Chalcogenide Nanostructures with a Pronounced Proximity Effect Enable Fast and Selective CO2 Electroreduction.
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-02-03 , DOI: 10.1002/anie.201912348
Fei-Yue Gao 1 , Shao-Jin Hu 2 , Xiao-Long Zhang 1 , Ya-Rong Zheng 1 , Hui-Juan Wang 3 , Zhuang-Zhuang Niu 1 , Peng-Peng Yang 1 , Rui-Cheng Bao 1 , Tao Ma 1 , Zheng Dang 4 , Yong Guan 4 , Xu-Sheng Zheng 4 , Xiao Zheng 2 , Jun-Fa Zhu 4 , Min-Rui Gao 1 , Shu-Hong Yu 1
Affiliation  

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.

中文翻译:

具有明显邻近效应的高曲率过渡金属硫族化物纳米结构可实现快速,选择性的CO2电还原。

将二氧化碳转化为有用燃料的一个巨大挑战来自将二氧化碳转化为二氧化碳或其他中间体的过程,这通常需要贵金属催化剂,高电势和/或电解质添加剂(例如,离子液体)。我们报告了微波加热策略,用于合成过渡金属硫属元素化物纳米结构,该结构可以有效地催化将CO2电还原为一氧化碳(CO)。我们发现,相对于可逆氢电极(RHE;无iR校正),硫化镉(CdS)纳米针阵列在-1.2 V时具有212 mA cm-2的空前电流密度和95.5±4.0%CO法拉第效率。实验和计算研究表明,高曲率CdS纳米结构催化剂具有显着的邻近效应,可产生较大的电场增强,
更新日期:2019-12-29
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