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

Xiao Chen^1,2, Shuaiqiang Jia^1,2, Chunjun Chen^1,2

¹Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, P. R. China.

Advanced Materials (Deerfield Beach, Fla.)

|November 17, 2023

Summary

This summary is machine-generated.

A new CuPEDOT catalyst stabilizes copper ions, enabling selective carbon dioxide (CO2) reduction to methane (CH4) with high efficiency and stability. This molecularly stable catalyst advances CO2 conversion research.

Keywords:

carbon dioxide reduction flow cell layered coordination polymer methane stability

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Simple Methods for the Preparation of Non-noble Metal Bulk-electrodes for Electrocatalytic Applications

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Area of Science:

Materials Science
Electrochemistry
Catalysis

Background:

Copper (Cu2+)-based materials are promising for CO2 electrocatalytic reduction (CO2 RR) but suffer from structural instability.
Reorganization of active sites during CO2 RR leads to catalyst deactivation and hinders structure-performance relationship studies.

Purpose of the Study:

To develop a strategy for stabilizing Cu2+ ions in CO2 RR catalysts.
To create a novel catalyst that prevents structural reorganization and promotes selective CO2 reduction to methane (CH4).

Main Methods:

Facile synthesis of a layered coordination polymer (CuPEDOT) by coordinating Cu2+ with 3,4-ethylenedioxythiophene (EDOT).
Electrocatalytic CO2 reduction reaction (CO2 RR) in a flow cell.
In situ spectroscopic characterization and theoretical calculations.

Main Results:

CuPEDOT achieved selective reduction of CO2 to CH4 with 62.7% Faradaic efficiency at 354 mA cm-2.
The catalyst demonstrated stability for at least 15 hours.
Stable Cu2+-EDOT coordination was maintained during CO2 RR, promoting CH4 formation over C2 products.

Conclusions:

The strong Cu2+-EDOT coordination prevents Cu2+ reduction and stabilizes the catalyst structure.
CuPEDOT offers a new approach for designing molecularly stable and highly active catalysts for CO2 RR.
This work provides insights into promoting CH4 selectivity by enhancing CO hydrogenation.