Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions

Mengyang Fan; Rui Kai Miao; Pengfei Ou; Yi Xu; Zih-Yi Lin; Tsung-Ju Lee; Sung-Fu Hung; Ke Xie; Jianan Erick Huang; Weiyan Ni; Jun Li; Yong Zhao; Adnan Ozden; Colin P. O’Brien; Yuanjun Chen; Yurou Celine Xiao; Shijie Liu; Joshua Wicks; Xue Wang; Jehad Abed; Erfan Shirzadi; Edward H. Sargent; David Sinton

doi:10.1038/s41467-023-38935-2

Nature Communications (Jun 2023)

Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions

Mengyang Fan,
Rui Kai Miao,
Pengfei Ou,
Yi Xu,
Zih-Yi Lin,
Tsung-Ju Lee,
Sung-Fu Hung,
Ke Xie,
Jianan Erick Huang,
Weiyan Ni,
Jun Li,
Yong Zhao,
Adnan Ozden,
Colin P. O’Brien,
Yuanjun Chen,
Yurou Celine Xiao,
Shijie Liu,
Joshua Wicks,
Xue Wang,
Jehad Abed,
Erfan Shirzadi,
Edward H. Sargent,
David Sinton

Affiliations

Mengyang Fan: Department of Mechanical and Industrial Engineering, University of Toronto
Rui Kai Miao: Department of Mechanical and Industrial Engineering, University of Toronto
Pengfei Ou: Department of Electrical and Computer Engineering, University of Toronto
Yi Xu: Department of Mechanical and Industrial Engineering, University of Toronto
Zih-Yi Lin: Department of Applied Chemistry, National Yang Ming Chiao Tung University
Tsung-Ju Lee: Department of Applied Chemistry, National Yang Ming Chiao Tung University
Sung-Fu Hung: Department of Applied Chemistry, National Yang Ming Chiao Tung University
Ke Xie: Department of Electrical and Computer Engineering, University of Toronto
Jianan Erick Huang: Department of Electrical and Computer Engineering, University of Toronto
Weiyan Ni: Department of Electrical and Computer Engineering, University of Toronto
Jun Li: Department of Mechanical and Industrial Engineering, University of Toronto
Yong Zhao: Department of Mechanical and Industrial Engineering, University of Toronto
Adnan Ozden: Department of Mechanical and Industrial Engineering, University of Toronto
Colin P. O’Brien: Department of Mechanical and Industrial Engineering, University of Toronto
Yuanjun Chen: Department of Electrical and Computer Engineering, University of Toronto
Yurou Celine Xiao: Department of Mechanical and Industrial Engineering, University of Toronto
Shijie Liu: Department of Mechanical and Industrial Engineering, University of Toronto
Joshua Wicks: Department of Electrical and Computer Engineering, University of Toronto
Xue Wang: Department of Electrical and Computer Engineering, University of Toronto
Jehad Abed: Department of Electrical and Computer Engineering, University of Toronto
Erfan Shirzadi: Department of Electrical and Computer Engineering, University of Toronto
Edward H. Sargent: Department of Electrical and Computer Engineering, University of Toronto
David Sinton: Department of Mechanical and Industrial Engineering, University of Toronto

DOI: https://doi.org/10.1038/s41467-023-38935-2
Journal volume & issue: Vol. 14, no. 1
pp. 1 – 8

Abstract

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Abstract Renewable CH4 produced from electrocatalytic CO2 reduction is viewed as a sustainable and versatile energy carrier, compatible with existing infrastructure. However, conventional alkaline and neutral CO2-to-CH4 systems suffer CO2 loss to carbonates, and recovering the lost CO2 requires input energy exceeding the heating value of the produced CH4. Here we pursue CH4-selective electrocatalysis in acidic conditions via a coordination method, stabilizing free Cu ions by bonding Cu with multidentate donor sites. We find that hexadentate donor sites in ethylenediaminetetraacetic acid enable the chelation of Cu ions, regulating Cu cluster size and forming Cu-N/O single sites that achieve high CH4 selectivity in acidic conditions. We report a CH4 Faradaic efficiency of 71% (at 100 mA cm−2) with <3% loss in total input CO2 that results in an overall energy intensity (254 GJ/tonne CH4), half that of existing electroproduction routes.

Published in Nature Communications

ISSN: 2041-1723 (Online)
Publisher: Nature Portfolio
Country of publisher: United Kingdom
LCC subjects: Science
Website: https://www.nature.com/ncomms/

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