首页|Molecular engineering binuclear copper catalysts for selective CO2 reduction to C2 products

Molecular engineering binuclear copper catalysts for selective CO2 reduction to C2 products

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Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO2 reduction(eCO2R),owing to their adaptable environments sur-rounding the copper metal centres.This investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular catalysts.The modulation of their coordination con-figuration through the introduction of organic groups aims to assess their efficacy in converting CO2 to C2 products.Our findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO2R behaviour.Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocy-cle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton transfer and the eCO2R process.Furthermore,we explore the impact of diverse electron-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH3)on the electron distri-bution in the molecular catalysts.Strategic placement of-OCH3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C2 products.This research provides fundamental insights into the design and optimization of binuclear Cu molecular cat-alysts for the electrochemical conversion of CO2 to value-added C2 products.

Molecular catalyst designSelective CO2 reductionC2 productsDensity functional theory calculations

Qi Zhao、Kai Lei、Bao Yu Xia、Rachel Crespo-Otero、Devis Di Tommaso

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Department of Chemistry,School of Physical and Chemical Sciences,Queen Mary University of London,London,E1 4NS,UK

Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education),Hubei Key Laboratory of Material Chemistry and Service Failure,State Key Laboratory of Materials Processing and Die & Mould Technology,School of Chemistry and Chemical Engineering,Huazhong University of Science and Technology(HUST),Wuhan 430074,Hubei,China

Department of Chemistry,University College London,London,WC1H OAJ,UK

Digital Environment Research Institute,Queen Mary University of London,Empire House,London E1 1HH,UK

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HUST-QMUL Strategic Partnership Research FundingChina Scholarship CouncilUK Materials and Molecular Modelling Hub for computational resources funded by EPSRCEPSRCQMUL Research-IT

2022-HUST-QMUL-SPRF-03EP/P020194/1EP/L000202

2024

10.1016/j.jechem.2024.01.060

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.93(6)
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