Abstract
Electrochemical CO2 reduction has garnered significant interest in the conversion of sustainable energy to valuable fuels and chemicals. Cu-based bimetallic catalysts play a crucial role in enhancing *CO concentration on Cu sites for efficient C─C coupling reactions, particularly for C2 product generation. To enhance Cu's electronic structure and direct its selectivity toward C2 products, a novel strategy is proposed involving the in situ electropolymerization of a nano-thickness cobalt porphyrin polymeric network (EP-CoP) onto a copper electrode, resulting in the creation of a highly effective EP-CoP/Cu tandem catalyst. The even distribution of EP-CoP facilitates the initial reduction of CO2 to *CO intermediates, which then transition to Cu sites for efficient C─C coupling. DFT calculations confirm that the *CO enrichment from Co sites boosts *CO coverage on Cu sites, promoting C─C coupling for C2+ product formation. The EP-CoP/Cu gas diffusion electrode achieves an impressive current density of 726 mA cm−2 at −0.9 V versus reversible hydrogen electrode (RHE), with a 76.8% Faraday efficiency for total C2+ conversion and 43% for ethylene, demonstrating exceptional long-term stability in flow cells. These findings mark a significant step forward in developing a tandem catalyst system for the effective electrochemical production of ethylene.
Original language | English |
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Article number | 2404053 |
Number of pages | 8 |
Journal | Advanced Science |
Volume | 11 |
Issue number | 34 |
Early online date | 8 Jul 2024 |
DOIs | |
Publication status | Published - 11 Sept 2024 |
Scopus Subject Areas
- Medicine (miscellaneous)
- Chemical Engineering(all)
- Materials Science(all)
- Biochemistry, Genetics and Molecular Biology (miscellaneous)
- Engineering(all)
- Physics and Astronomy(all)
User-Defined Keywords
- cobalt porphyrin
- electrochemical CO2 reduction
- in situ electropolymerizing
- multi-carbon products
- tandem catalyst