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

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 AbedErfan Shirzadi, Edward H. Sargent^*, David Sinton^*

^*Corresponding author for this work

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

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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.

© The Author(s) 2023

Original language	English
Article number	3314
Journal	Nature Communications
Volume	14
Online published	7 Jun 2023
DOIs	https://doi.org/10.1038/s41467-023-38935-2
Publication status	Published - 2023
Externally published	Yes

Funding

The authors acknowledge support from the Natural Sciences and Engineering Research Council (NSERC) of Canada, Natural Resources Canada—Clean Growth Program, and the Natural Gas Innovation Fund (NGIF). The infrastructure provided through the Canada Foundation for Innovation and the Ontario Research Fund supported the work. R.K.M. thanks NSERC, Hatch, and the Government of Ontario for their support through graduate scholarships. P.O. thanks the Climate Positive Energy for its support through Rising Stars in Clean Energy Postdoctoral Fellowship. Synchrotron experiments were carried out at SXRMB beamline at the Canadian Light Source (CLS). S.F.H. thanks for the supports from the National Science and Technology Council, Taiwan (Contract No. NSTC 111−2628-M-A49-007) and the support from the Yushan Young Scholar Program, Ministry of Education, Taiwan. W.N. acknowledges the financial support of the Postdoc. Mobility Fellowship from the Swiss National Science Foundation (SNSF) (No. P500PN_202906). We acknowledge the help from Dr. Qunfeng Xiao, Dr. Mohsen Shakouri, and Dr. Alisa Paterson for their kind technical assistance.

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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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

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title = "Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions",

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.{\textcopyright} The Author(s) 2023 ",

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

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year = "2023",

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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

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T1 - Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions

AU - Fan, Mengyang

AU - Miao, Rui Kai

AU - Ou, Pengfei

AU - Xu, Yi

AU - Lin, Zih-Yi

AU - Lee, Tsung-Ju

AU - Hung, Sung-Fu

AU - Xie, Ke

AU - Huang, Jianan Erick

AU - Ni, Weiyan

AU - Li, Jun

AU - Zhao, Yong

AU - Ozden, Adnan

AU - O’Brien, Colin P.

AU - Chen, Yuanjun

AU - Xiao, Yurou Celine

AU - Liu, Shijie

AU - Wicks, Joshua

AU - Wang, Xue

AU - Abed, Jehad

AU - Shirzadi, Erfan

AU - Sargent, Edward H.

AU - Sinton, David

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N2 - 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

AB - 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

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