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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
Nature communications, 05/2021, Letnik: 12, Številka: 1Journal Article
Abstract The electrochemical conversion of CO 2 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 CO 2 -to-methane selectivity of 62%, a methane partial current density of 136 mA cm −2 , and > 110 hours of stable operation.
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JCR | SNIP | JCR | SNIP | JCR | SNIP | JCR | SNIP |
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in: SICRIS
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