journal article·2024-03

Highly Stable Layered Coordination Polymer Electrocatalyst toward Efficient CO2‐to‐CH4 Conversion

Xiao Chen, Shuaiqiang Jia, Chunjun Chen, Jiapeng Jiao, Jianxin Zhai, Ting Deng, Cheng Xue, Hailian Cheng, Mengke Dong, Wei Xia, Jianrong Zeng, Xueqing Xing, Haihong Wu, Mingyuan He, Buxing Han

Advanced Materials· Volume 36· Issue 11
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Abstract

Abstract Cu2+‐based materials, a class of promising catalysts for the electrocatalytic carbon dioxide reduction reaction (CO2RR) to value‐added chemicals, usually undergo inevitable and uncontrollable reorganization processes during the reaction, resulting in catalyst deactivation or the new active sites formation and bringing great challenges to exploring their structure–performance relationships. Herein, a facile strategy is reported for constructing Cu2+ and 3, 4‐ethylenedioxythiophene (EDOT) coordination to stabilize Cu2+ ions to prepare a novel layered coordination polymer (CuPEDOT). CuPEDOT enables selective reduction of CO2 to CH4 with 62.7% Faradaic efficiency at the current density of 354 mA cm−2 in a flow cell, and the catalyst is stable for at least 15 h. In situ spectroscopic characterization and theoretical calculations reveal that CuPEDOT catalyst can maintain the Cu2+‐EDOT coordination structurally stable in CO2RR and significantly promote the further hydrogenation of *CO intermediates, favoring the formation of CH4 instead of dimerization to C2 products. The strong coordination between EDOT and Cu2+ prevents the reduction of Cu2+ ions during CO2RR. The finding of this work provides a new perspective on designing molecularly stable, highly active catalysts for CO2RR.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Carbon dioxide utilization in catalysis

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 P. R. China

Institute of Eco‐Chongming 20 Cuiniao Road, Chenjia Town, Chongming District Shanghai 202162 P. R. China

Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China

Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 P. R. China

Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. China

Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China

Funding

National Key Research and Development Program of China · National Natural Science Foundation of China · China Postdoctoral Science Foundation

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