Unraveling the Influence of Oxygen Vacancy Concentration on Electrocatalytic CO2 Reduction to Formate over Indium Oxide Catalysts

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Qin Cheng, Ming Huang, Lei Xiao, Shiyong Mou, Xiaoli Zhao*, Yuqun Xie, Guodong Jiang, Xinyue Jiang and Fan Dong*, 
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引用次数: 14

Abstract

Rational engineering of oxygen vacancies in a metal oxide-based catalyst represents an effective strategy to regulate catalytic performances by influencing both their electrochemical active surface areas and the microelectronic structure. However, the precise control and modulation of the concentration and uniformity of oxygen vacancies on the catalyst surface still remains inadequately explored and poorly elucidated. Herein, we develop a facile and effective method to prepare a series of In2O3 nanorods with varying oxygen vacancy concentrations for efficient electrolytic CO2 reduction to formate. Experimental results and theoretical calculations reveal that the abundant oxygen vacancies in the In2O3 catalyst significantly improve CO2 activation and promote the production of *HCOO intermediates, achieving a maximum formate Faradaic efficiency of 91.2% at −1.27 V vs a reversible hydrogen electrode (RHE) with high partial current density and, meanwhile, superior stability. The underlying relationship between the oxygen vacancy concentration and CO2 reduction reaction (CO2RR) performance was further established. This work offers a feasible strategy to finely tune the oxygen vacancy concentration in p-block metal oxide-based catalysts for highly efficient electrolytic CO2RR.

Abstract Image

氧空位浓度对氧化铟催化剂上CO2电催化还原生成甲酸酯的影响
合理设计金属氧化物催化剂中的氧空位是通过影响其电化学活性表面积和微电子结构来调节催化性能的有效策略。然而,催化剂表面氧空位的浓度和均匀性的精确控制和调节仍然没有得到充分的探索和阐明。在此,我们开发了一种简单有效的方法来制备一系列具有不同氧空位浓度的In2O3纳米棒,用于有效的电解CO2还原成甲酸盐。实验结果和理论计算表明,In2O3催化剂中丰富的氧空位显著提高了CO2的活化,促进了*HCOO中间体的生成,在−1.27 V下,与具有高偏电流密度的可逆氢电极(RHE)相比,甲酸法拉第效率达到了91.2%的最大值,同时具有优异的稳定性。进一步建立了氧空位浓度与CO2还原反应(CO2RR)性能之间的内在关系。本研究提供了一种可行的策略来微调p嵌段金属氧化物基催化剂中的氧空位浓度,以实现高效的电解CO2RR。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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