Porphyrin-based metal–organic frameworks anchored with Cu species for highly efficient electrocatalytic CO2 reduction to CH4

Abstract

The electrocatalytic carbon dioxide (CO2) reduction into methane (CH4) represents a promising strategy for sustainable carbon cycling. Nevertheless, this complex conversion, involving an eight-electron transfer process, faces significant challenges in achieving satisfactory catalytic activity and CH4 selectivity for practical applications. Herein, we employed a facile solvothermal reaction strategy to anchor copper (Cu) atoms in the porphyrin-based metal–organic framework (PMOF) to construct Cu single-atom catalysts, named the Cu-PMOF catalyst. The good combination of highly accessible Cu active sites, optimized Cu loading, and a loose structure in the Cu-PMOF electrode significantly enhanced the electrocatalytic performance for the conversion of CO2 to CH4. The highest Faradaic efficiency of CH4 reached 80.4% at a current density of −300 mA cm−2 in 1 M potassium hydroxide electrolytes with a flow cell configuration. Moreover, this Cu-PMOF electrode achieved a maximum partial current density of −337.5 mA cm−2 at a potential of −1.23 V versus reversible hydrogen electrode. Comprehensive experimental investigations revealed the Cu-PMOF electrode enabled a multi-step CO2 hydrogenation process, characterized by effective H2O activation and the sequential transformation of CO2 into crucial intermediates, ultimately leading to the selective formation of CH4.

Graphical abstract: Porphyrin-based metal–organic frameworks anchored with Cu species for highly efficient electrocatalytic CO2 reduction to CH4

Supplementary files

Article information

Article type
Paper
Submitted
25 Apr 2025
Accepted
09 Jul 2025
First published
10 Jul 2025

Green Chem., 2025, Advance Article

Porphyrin-based metal–organic frameworks anchored with Cu species for highly efficient electrocatalytic CO2 reduction to CH4

W. Cao, D. Yang, B. Li, Y. Mi, K. Qi, Y. Mao, Y. Zhao, H. Li and Z. He, Green Chem., 2025, Advance Article , DOI: 10.1039/D5GC02085A

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