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用于电化学将CO转化为CO的银-铜气凝胶。

Ag-Cu aerogel for electrochemical CO conversion to CO.

作者信息

Wang Wenbo, Gong Shanhe, Liu Jun, Ge Yang, Wang Jie, Lv Xiaomeng

机构信息

School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, PR China.

School of the Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, PR China.

出版信息

J Colloid Interface Sci. 2021 Aug;595:159-167. doi: 10.1016/j.jcis.2021.03.120. Epub 2021 Mar 25.

Abstract

The current strategy of electrocatalytic CO reduction reaction (eCORR) to generate useful chemicals and hydrocarbons is supposed to effectively mitigate the greenhouse effect. The practical application for eCORR in aqueous solutions, however, still was encumbered by its high overpotential, low activity and poor selectivity due to CO mass transfer and intermediate stability. Electrocatalytic materials with reduced overpotential and high efficiency and selectivity are exploited for further development. Herein, Ag and Cu precursors were co-reduced to generate Ag-Cu bimetallic aerogel after further freeze drying. Compared with Ag aerogel, the optimal AgCu can effectively decrease overpotential, improve selectivity and current density, and keep electrochemical stability. At -0.89 V vs. RHE, the Faraday efficiency reached 89.40% and the CO partial current density of -5.86 mA cm was obtained. The intrinsic property of metal aerogel (hydrophobic, hierarchical porous structure, conductivity), presence of rich grain boundaries and geometric effect and the introduction of Cu leading to improvement of adsorption between the catalyst and the *COOH intermediate in AgCu, contribute to the enhanced performance. Furthermore, the strategy of constructing metal aerogel will improve metal catalyst performance towards eCORR and pave way for further industrial applications.

摘要

目前通过电催化一氧化碳还原反应(eCORR)生成有用化学品和碳氢化合物的策略被认为能够有效缓解温室效应。然而,由于一氧化碳传质和中间体稳定性问题,eCORR在水溶液中的实际应用仍然受到高过电位、低活性和差选择性的阻碍。人们正在开发具有降低过电位以及高效率和选择性的电催化材料以进一步发展。在此,银和铜前驱体被共还原,经过进一步冷冻干燥后生成银-铜双金属气凝胶。与银气凝胶相比,最优的银铜双金属气凝胶能够有效降低过电位,提高选择性和电流密度,并保持电化学稳定性。在相对于可逆氢电极(RHE)为-0.89 V时,法拉第效率达到89.40%,并获得了-5.86 mA cm的一氧化碳分电流密度。金属气凝胶的固有特性(疏水性、分级多孔结构、导电性)、丰富晶界的存在和几何效应以及铜的引入导致银铜双金属气凝胶中催化剂与*COOH中间体之间吸附作用的改善,共同促成了性能的提升。此外,构建金属气凝胶的策略将提高金属催化剂对eCORR的性能,并为进一步的工业应用铺平道路。

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