In Situ Electropolymerizing Toward EP-CoP/Cu Tandem Catalyst for Enhanced Electrochemical CO2-to-Ethylene Conversion

Chao Wang, Yifan Sun, Yuzhuo Chen, Yiting Zhang, Liangliang Yue, Lianhuan Han*, Liubin Zhao*, Xunjin Zhu*, Dongping Zhan*

*Corresponding author for this work

Research output: Contribution to journalJournal articlepeer-review

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 languageEnglish
Article number2404053
Number of pages8
JournalAdvanced Science
Volume11
Issue number34
Early online date8 Jul 2024
DOIs
Publication statusPublished - 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

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