Role of Ethylene Diamine Tetraacetate as an Additive in Electrolyte on Intermediate Stabilization in Electrochemical CO2 Reduction.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2025-03-12 DOI:10.1002/cssc.202402471
Seokwoo Choe, Yu Jin Kim, Jeongu You, Kyeounghak Kim, Youn Jeong Jang
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Abstract

Although an electrochemical CO2 reduction reaction (ECO2RR) can provide an ideal route to produce CH4, its selectivity is significantly hindered due to kinetically complex steps. To improve CH4 selectivity, this study focuses on microenvironmental engineering using an additive of ethylene diamine tetraacetate (EDTA) in electrolyte. EDTA interacts with the Cu catalyst, altering its electronic structure and promoting CO2 activation, in addition, it forms additional hydrogen bonding with key intermediates of *CO and *CHO leading to their stabilization. These phenomena were experimentally and theoretically demonstrated as exhibiting the facilitated CO2 adsorption and the *CO to *CHO conversion with suppressing *CO desorption. As a result, Cu-loaded N-doped Carbon (Cu/N:C) with EDTA additive in electrolyte shows a significantly enhanced CH4 selectivity, reaching a faradaic efficiency (FE) of 48% and a partial current density (JCH4) of 15.0 mA cm-2 at ‒1.8 VRHE. This performance surpasses that of pristine Cu/N:C, which exhibited marginal FE and JCH4 values of 32%, and 6.8 mA cm-2, respectively. It obviously emphasizes the importance of intermediate stabilization via microenvironmental engineering for selective CH4 production. This approach provides great insight into developing an effective ECO2RR system for promoting CO2 to value-added chemicals and fuel conversion.

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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
期刊最新文献
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