Yi Xu1, Fengwang Li2, Aoni Xu2, Jonathan P Edwards1, Sung-Fu Hung2,3, Christine M Gabardo1, Colin P O'Brien1, Shijie Liu1, Xue Wang2, Yuhang Li2, Joshua Wicks2, Rui Kai Miao1, Yuan Liu2, Jun Li1,2, Jianan Erick Huang2, Jehad Abed2,4, Yuhang Wang2, Edward H Sargent5, David Sinton6. 1. Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, ON, Canada. 2. Department of Electrical and Computer Engineering, University of Toronto, Toronto, ON, Canada. 3. Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu, Taiwan. 4. Department of Materials Science and Engineering, University of Toronto, Toronto, ON, Canada. 5. Department of Electrical and Computer Engineering, University of Toronto, Toronto, ON, Canada. ted.sargent@utoronto.ca. 6. Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, ON, Canada. sinton@mie.utoronto.ca.
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.
The electrochemical conversion of n class="Chemical">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 coppercoordination number. At a coppercoordination 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.
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