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

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

doi:10.1038/s41467-021-23065-4

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

Journal Article · Tue May 18 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-23065-4· OSTI ID:1784990

^[1]; ^[1]; Xu, Aoni ^[1]; ^[1]; ^[2]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; Huang, Jianan Erick ^[1]; ^[1]; ^[1]; ^[1]; ^[1]

Univ. of Toronto, ON (Canada)
Univ. of Toronto, ON (Canada); National Yang Ming Chiao Tung Univ., Hsinchu (Taiwan)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1784990

Alternate ID(s):: OSTI ID: 1787781

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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