Low coordination number copper catalysts for electrochemical CO2 methanation in a membrane electrode assembly

Yi Xu, Fengwang Li, Aoni Xu, Jonathan P. Edwards, Sung Fu Hung, Christine M. Gabardo, Colin P. O’Brien, Shijie Liu, Xue Wang, Yuhang Li, Joshua Wicks, Rui Kai Miao, Yuan Liu, Jun Li, Jianan Erick Huang, Jehad Abed, Yuhang Wang, Edward H. Sargent, David Sinton*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

37 Scopus citations

Abstract

The electrochemical conversion of CO2 to methane provides a means to store intermittent renewable electricity in the form of a carbon-neutral hydrocarbon fuel that benefits from an established global distribution network. The stability and selectivity of reported approaches reside below technoeconomic-related requirements. Membrane electrode assembly-based reactors offer a known path to stability; however, highly alkaline conditions on the cathode favour C-C coupling and multi-carbon products. In computational studies herein, we find that copper in a low coordination number favours methane even under highly alkaline conditions. Experimentally, we develop a carbon nanoparticle moderator strategy that confines a copper-complex catalyst when employed in a membrane electrode assembly. In-situ XAS measurements confirm that increased carbon nanoparticle loadings can reduce the metallic copper coordination number. At a copper coordination number of 4.2 we demonstrate a CO2-to-methane selectivity of 62%, a methane partial current density of 136 mA cm−2, and > 110 hours of stable operation.

Original languageEnglish
Article number2932
JournalNature Communications
Volume12
Issue number1
DOIs
StatePublished - Dec 2021

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