The C–C bond cleavage inhibition and intermediates adsorption enhancement co-boost the selective electrooxidation of ethylene glycol on silver-palladium hollow nanocubes

IF 17.2 1区 化学 Q1 CHEMISTRY, APPLIED
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI:10.1016/S1872-2067(26)65015-2
Zi-Hang Wang, Wei Zhong, Si-Qi Li, Bin Sun, Hao Lan, Xiao-Yu Zhang, Xin Wang, Yu Chen, Xuan Ai
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引用次数: 0

Abstract

Efficient electrooxidation of ethylene glycol (EG) to glycolic acid (GA) is highly desirable for biomass valorization and EG recycling, which remains challenging owing to side reactions involving C–C bond cleavage. Herein, the bimetallic AgPd hollow nanocubes (AgPd hNCs) are successfully prepared via a solvothermal-assisted Galvanic replacement strategy. Both theoretical calculations and experimental results indicate that the electronic interplay between the Pd atom and Ag atom hinders C–C bond breaking and enhances the adsorption of critical intermediates, resulting in high selectivity toward GA production. Benefiting from these features, AgPd hNCs achieve a Faradaic efficiency of 93% toward GA formation and a 2.8-fold increase in mass activity compared to Pd black. Moreover, the strong oxygen affinity of Ag promotes the removal of CO-like intermediates from the Pd surface, resulting in superior EG oxidation stability. This study highlights a generalizable Ag-based strategy to modulate bimetallic interfaces for selective oxidation reaction of specific functional groups, contributing to the rational design of electrocatalysts for biomass upgrading.
C-C键解理抑制和中间体吸附增强共同促进了乙二醇在银钯空心纳米立方上的选择性电氧化
乙二醇(EG)的高效电氧化为乙醇酸(GA)是生物质增值和EG回收的理想选择,但由于涉及C-C键切割的副反应,这仍然具有挑战性。本文通过溶剂热辅助电替换策略成功制备了双金属AgPd空心纳米立方(AgPd hNCs)。理论计算和实验结果都表明,钯原子和银原子之间的电子相互作用阻碍了C-C键的断裂,增强了对关键中间体的吸附,从而产生了高选择性的GA。得益于这些特性,AgPd hNCs对GA形成的法拉第效率达到93%,质量活性比Pd黑提高2.8倍。此外,Ag的强氧亲和力促进了co类中间体从Pd表面的去除,从而获得了优异的EG氧化稳定性。本研究强调了一种基于银的通用策略来调节双金属界面以进行特定官能团的选择性氧化反应,有助于生物质升级电催化剂的合理设计。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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