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Molecular understanding of cation effects on double layers and their significance to CO-CO dimerization

National Science Review 2023年第9期10卷 125-135页

作者： Jia-Bo Le Ao Chen Yongbo Kuang Jun Cheng Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of Sciences State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical EngineeringXiamen University Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)

cation effects have been shown in numerous experiments to play a significant role in electro *** understand these effects at the molecular level,we systematically investigate the structures and capacitances of electric double layers with a variety of cations as counter charges at Pt(111)-COad/water interfaces with ab initio molecular *** is encouraging to find that the computed Helmholtz capacitances for different cations are in quantitative agreement with experiments,and that the trend of cation effects on capacitances shows clear correlation with the structures of interface cations of differing sizes and hydration *** importantly,we demonstrate the Helmholtz capacitance as the key descriptor for measuring the activity of CO-CO dimerization,the rate-determining step for C2+formation in electroreduction of CO and *** work provides atomistic insights into cation effects on electric double layers and electrocatalysis that are crucial for optimizing electrode and electrolyte materials.

关键词： cation effect electrocatalysis electric double layer CO-CO dimerization ab initio molecular dynamics

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cation effects in electrocatalytic reduction reactions:Recent advances

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Chinese Journal of Catalysis 2024年第8期63卷 16-32页

作者： Qinghui Ren Liang Xu Mengyu Lv Zhiyuan Zhang Zhenhua Li Mingfei Shao Xue Duan State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou 324000ZhejiangChina

Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high-value-added chemicals or *** design and modification of electrocatalysts have been widely implemented to improve their performance in these ***,bottle-necks are encountered,making it challenging to further improve performance through catalyst development ***,cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction *** review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction ***,we introduce the mechanisms underlying cation *** then provide a comprehensive overview of their application in electroreduction *** techniques and theoretical calcula-tion methods for studying cation effects are also ***,we address remaining challeng-es and future perspectives in this *** hope that this review offers fundamental insights and design guidance for utilizing cation effects,thereby advancing their development.

关键词： Electrocatalysis Reduction reaction cation effect Mechanism Application

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Electro-oxidation cross-coupling of primary and secondary alcohols by constructing intermediate-enriched micro-environment

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Science China Chemistry 2023年第8期66卷 2408-2415页

作者： Leitao Xu Cairong Wang Yelin Yao Wei Chen Zhonghuan Zhu Jingcheng Wu Ming Yang Yandong Wu Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangshaHunan410082China School of Chemistry and Chemical Engineering Jishou UniversityJishou416000China

Electrocatalytic dehydrogenative cross-coupling of various alcohols in aqueous electrolytes functionalizes alcohols to form structurally diverse long-carbon-chain ***,it remains challenging to achieve the high selectivity because of the high reactivity of involved carbonyl intermediates and different oxidation rates for the ***,the synthesis ofα,β-unsaturated ketones from alcohols was realized by the electro-oxidation cross-coupling in aqueous solutions by a“salting-out”strategy to engineer the micro-environment at electrocatalytic reaction *** calculations and electrochemical measurements demonstrated that concentrated local intermediates could inhibit the over-oxidation of alcohols and accelerate the coupling reaction kinetics between the *** strategy can couple primary and secondary alcohols to formα,β-unsaturated carbonyl compounds with a selectivity of 87% and be easily scaled up to gram *** study provides an attractive strategy for broadening the diversity of organic products in electrocatalysis.

关键词： electro-oxidation of alcohols cross-coupling cation effect microenvironment

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