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用于高效电催化二氧化碳还原的取向排列的硫化铟纳米棒

Aligned InS Nanorods for Efficient Electrocatalytic Carbon Dioxide Reduction.

作者信息

Zhang Yanlong, Lan Jiao, Xie Feng, Peng Ming, Liu Jilei, Chan Ting-Shan, Tan Yongwen

机构信息

College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body, Hunan University, Changsha, Hunan 410082, China.

College of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan University, Changsha, Hunan 410082, China.

出版信息

ACS Appl Mater Interfaces. 2022 Jun 8;14(22):25257-25266. doi: 10.1021/acsami.2c01152. Epub 2022 May 24.

Abstract

Electrochemical CO reduction technology can combine renewable energy sources with carbon capture and storage to convert CO into industrial chemicals. However, the catalytic activity under high current density and long-term electrocatalysis process may deteriorate due to agglomeration, catalytic polymerization, element dissolution, and phase change of active substances. Here, we report a scalable and facile method to fabricate aligned InS nanorods by chemical dealloying. The resulting aligned InS nanorods exhibit a remarkable CORR activity for selective formate production at a wide potential window, achieving over 90% faradic efficiencies from -0.5 to -1.0 V vs reversible hydrogen electrode (RHE) under gas diffusion cell, as well as continuously long-term operation without deterioration. In situ electrochemical Raman spectroscopy measurements reveal that the OCHO species (Bidentate adsorption) are the intermediates that occurred in the reaction of CO reduction to formate. Meanwhile, the presence of sulfur can accelerate the activation of HO to react with CO, promoting the formation of OCHO intermediates on the catalyst surface. Significantly, through additional coupling anodic methanol oxidation reaction (MOR), the unusual two-electrode electrolytic system allows highly energy-efficient and value-added formate manufacturing, thereby reducing energy consumption.

摘要

电化学CO还原技术可以将可再生能源与碳捕获和存储相结合,将CO转化为工业化学品。然而,在高电流密度下的催化活性以及长期电催化过程中,由于活性物质的团聚、催化聚合、元素溶解和相变,其催化活性可能会降低。在此,我们报道了一种通过化学脱合金制备排列整齐的InS纳米棒的可扩展且简便的方法。所得排列整齐的InS纳米棒在宽电位窗口下对选择性生成甲酸盐表现出显著的CORR活性,在气体扩散池中相对于可逆氢电极(RHE)在-0.5至-1.0 V的电位范围内实现了超过90%的法拉第效率,并且能够持续长期运行而不发生性能恶化。原位电化学拉曼光谱测量表明,OCHO物种(双齿吸附)是CO还原生成甲酸盐反应中的中间体。同时,硫的存在可以加速HO的活化以与CO反应,促进催化剂表面OCHO中间体的形成。值得注意的是,通过额外耦合阳极甲醇氧化反应(MOR),这种独特的双电极电解系统能够实现高能效和高附加值的甲酸盐生产,从而降低能源消耗。

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