Tailoring silver nanostructures for enhanced CO2 reduction: Insights from In-situ SERS and electrochemical studies

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Applied Catalysis A: General Pub Date : 2026-02-05 Epub Date: 2025-12-10 DOI:10.1016/j.apcata.2025.120743
E. Amaterz , O. Bajouk , B. Ravi , I. Rougeaux , R. Ramos , V. Faucheux , P. Chenevier
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引用次数: 0

Abstract

In this study, Ag structures with tunable morphologies were synthesized via different methods and evaluated for the electrochemical CO2 reduction (CO2RR) in both H-cell and zero-gap electrolyzer configurations. Scanning electron microscopy (SEM) confirmed that the Ag catalysts could be tuned to exhibit distinct morphologies, such as polygonal, flower-like, nanowires and rod-like structures. Among these, the rod-like Ag (Ag-Rod) catalyst exhibited the highest Faradaic efficiency for CO (>96 %), demonstrating excellent selectivity in both configurations. In-situ surface-enhanced Raman spectroscopy (SERS) was adopted to monitor the adsorption of reaction intermediates in real time, revealing dynamic changes in CO-related species and other adsorbates as a function of applied potential. The enhanced SERS response arising from the plasmonic properties of Ag enabled the direct observation of key reaction intermediates. The results show that the rod-like Ag structure exhibits superior CO selectivity, which is attributed to its morphology-dependent surface properties and favorable CO desorption dynamics. These findings highlight the critical role of structural tuning in governing CO2RR pathways, providing mechanistic insight into how morphology and plasmonic effects can be leveraged to design efficient and selective Ag-based electrocatalysts for CO2 conversion.
裁剪银纳米结构以增强二氧化碳还原:来自原位SERS和电化学研究的见解
在本研究中,通过不同的方法合成了具有可调形貌的Ag结构,并对氢电池和零间隙电解槽配置下的电化学CO2还原(CO2RR)进行了评估。扫描电子显微镜(SEM)证实,Ag催化剂可以调整成不同的形态,如多边形、花状、纳米线和棒状结构。其中,棒状Ag (Ag- rod)催化剂对CO的法拉第效率最高(>96 %),在两种构型下均表现出优异的选择性。采用原位表面增强拉曼光谱(SERS)实时监测反应中间体的吸附情况,揭示co相关物质和其他吸附物随应用电位的动态变化。银的等离子体特性增强了SERS响应,从而可以直接观察关键的反应中间体。结果表明,棒状Ag结构表现出优异的CO选择性,这是由于其形貌依赖的表面性质和良好的CO脱附动力学。这些发现强调了结构调整在控制CO2RR途径中的关键作用,为如何利用形态和等离子体效应来设计高效和选择性的银基二氧化碳转化电催化剂提供了机制见解。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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