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

Author(s)

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
Jehad Abed
Erfan Shirzadi
Edward H. Sargent
David Sinton

Detail(s)

Original language	English
Article number	3314
Journal / Publication	Nature Communications
Volume	14
Online published	7 Jun 2023
Publication status	Published - 2023
Externally published	Yes

Link(s)

DOI	DOI https://doi.org/10.1038/s41467-023-38935-2 Final Published version
	Check@CityULib
Attachment(s)	Documents 155745622.pdf Final Published version, 2.04 MB, PDF Publisher's Copyright Statement This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/
Link to Scopus	https://www.scopus.com/record/display.uri?eid=2-s2.0-85161221899&origin=recordpage
Permanent Link	https://scholars.cityu.edu.hk/en/publications/publication(d43e81d3-b82e-4bc0-a0c1-329bf4daffc9).html

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.

© The Author(s) 2023

Research Area(s)

SDG 13 - Climate Action

Bibliographic Note

Citation Format(s)

[ RIS ] [ BibTeX ]

Single-site decorated copper enables energy- and carbon-efficient CO₂ methanation in acidic conditions. / Fan, Mengyang; Miao, Rui Kai; Ou, Pengfei et al.
In: Nature Communications, Vol. 14, 3314, 2023.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

Fan, M, Miao, RK, Ou, P, Xu, Y, Lin, Z-Y, Lee, T-J, Hung, S-F, Xie, K, Huang, JE, Ni, W, Li, J, Zhao, Y, Ozden, A, O’Brien, CP, Chen, Y, Xiao, YC, Liu, S, Wicks, J, Wang, X, Abed, J, Shirzadi, E, Sargent, EH & Sinton, D 2023, 'Single-site decorated copper enables energy- and carbon-efficient CO₂ methanation in acidic conditions', Nature Communications, vol. 14, 3314. https://doi.org/10.1038/s41467-023-38935-2

Fan, M., Miao, R. K., Ou, P., Xu, Y., Lin, Z.-Y., Lee, T.-J., Hung, S.-F., Xie, K., Huang, J. E., Ni, W., Li, J., Zhao, Y., Ozden, A., O’Brien, C. P., Chen, Y., Xiao, Y. C., Liu, S., Wicks, J., Wang, X., ... Sinton, D. (2023). Single-site decorated copper enables energy- and carbon-efficient CO₂ methanation in acidic conditions. Nature Communications, 14, Article 3314. https://doi.org/10.1038/s41467-023-38935-2

Fan M, Miao RK, Ou P, Xu Y, Lin ZY, Lee TJ et al. Single-site decorated copper enables energy- and carbon-efficient CO₂ methanation in acidic conditions. Nature Communications. 2023;14:3314. Epub 2023 Jun 7. doi: 10.1038/s41467-023-38935-2

Fan, Mengyang ; Miao, Rui Kai ; Ou, Pengfei et al. / Single-site decorated copper enables energy- and carbon-efficient CO₂ methanation in acidic conditions. In: Nature Communications. 2023 ; Vol. 14.

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