Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2

Zhi Qin Liang; Tao Tao Zhuang; Ali Seifitokaldani; Jun Li; Chun Wei Huang; Chih Shan Tan; Yi Li; Phil De Luna; Cao Thang Dinh; Yongfeng Hu; Qunfeng Xiao; Pei Lun Hsieh; Yuhang Wang; Fengwang Li; Rafael Quintero-Bermudez; Yansong Zhou; Peining Chen; Yuanjie Pang; Shen Chuan Lo; Lih Juann Chen; Hairen Tan; Zheng Xu; Suling Zhao; David Sinton; Edward H. Sargent

doi:10.1038/s41467-018-06311-0

Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO₂

Zhi Qin Liang, Tao Tao Zhuang, Ali Seifitokaldani, Jun Li, Chun Wei Huang, Chih Shan Tan, Yi Li, Phil De Luna, Cao Thang Dinh, Yongfeng Hu, Qunfeng Xiao, Pei Lun Hsieh, Yuhang Wang, Fengwang Li, Rafael Quintero-Bermudez, Yansong Zhou, Peining Chen, Yuanjie Pang, Shen Chuan Lo, Lih Juann ChenHairen Tan, Zheng Xu, Suling Zhao, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

195 Scopus citations

Abstract

Copper-based materials are promising electrocatalysts for CO₂ reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO₂ reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO₂ reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C₂₊ products. We achieve a 40-fold enhancement in the ratio of C₂₊ to the competing CH₄ compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO₂ reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO₂ reduction to multi-carbon products.

Original language	English (US)
Article number	3828
Journal	Nature communications
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41467-018-06311-0
State	Published - Dec 1 2018

ASJC Scopus subject areas

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

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10.1038/s41467-018-06311-0

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Liang, Z. Q., Zhuang, T. T., Seifitokaldani, A., Li, J., Huang, C. W., Tan, C. S., Li, Y., De Luna, P., Dinh, C. T., Hu, Y., Xiao, Q., Hsieh, P. L., Wang, Y., Li, F., Quintero-Bermudez, R., Zhou, Y., Chen, P., Pang, Y., Lo, S. C., ... Sargent, E. H. (2018). Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO₂ Nature communications, 9(1), [3828]. https://doi.org/10.1038/s41467-018-06311-0

@article{93d1547a78f94d839d6c1aefcf44970c,

title = "Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2 ",

abstract = "Copper-based materials are promising electrocatalysts for CO2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C2+ products. We achieve a 40-fold enhancement in the ratio of C2+ to the competing CH4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO2 reduction to multi-carbon products.",

author = "Liang, {Zhi Qin} and Zhuang, {Tao Tao} and Ali Seifitokaldani and Jun Li and Huang, {Chun Wei} and Tan, {Chih Shan} and Yi Li and {De Luna}, Phil and Dinh, {Cao Thang} and Yongfeng Hu and Qunfeng Xiao and Hsieh, {Pei Lun} and Yuhang Wang and Fengwang Li and Rafael Quintero-Bermudez and Yansong Zhou and Peining Chen and Yuanjie Pang and Lo, {Shen Chuan} and Chen, {Lih Juann} and Hairen Tan and Zheng Xu and Suling Zhao and David Sinton and Sargent, {Edward H.}",

note = "Funding Information: This work was supported financially by the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, and the CIFAR Bio-Inspired Solar Energy program. Computations were performed on the SOSCIP Consortium{\textquoteright}s Blue Gene/Q computing platform. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada Ltd., Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. X-ray absorption spectra were performed on SXRMB beamlines at the Canadian Light Source (CLS), which is supported by the Canada Foundation for Innovation, Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. Z.L. acknowledges a scholarship from the China Scholarship Council (CSC) (201607090041) and Basic and Innovation Program, Beijing Jiaotong University (KSJB17016536). A.S. acknowledges Fonds de Recherche du Quebec-Nature et Technologies (FRQNT) for the postdoctoral fellowship award. P.D.L. acknowledges support from NSERC in the form of the Canada Graduate Scholarship. H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511) to support his postdoctoral research at University of Toronto. The authors thank C. Q. Zou, M. X. Liu, F. F. Fan, J. Xing and L. Gao from University of Toronto for fruitful discussions. Publisher Copyright: {\textcopyright} 2018, The Author(s).",

year = "2018",

month = dec,

day = "1",

doi = "10.1038/s41467-018-06311-0",

language = "English (US)",

volume = "9",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Publishing Group",

number = "1",

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Liang, ZQ, Zhuang, TT, Seifitokaldani, A, Li, J, Huang, CW, Tan, CS, Li, Y, De Luna, P, Dinh, CT, Hu, Y, Xiao, Q, Hsieh, PL, Wang, Y, Li, F, Quintero-Bermudez, R, Zhou, Y, Chen, P, Pang, Y, Lo, SC, Chen, LJ, Tan, H, Xu, Z, Zhao, S, Sinton, D & Sargent, EH 2018, 'Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO₂ ', Nature communications, vol. 9, no. 1, 3828. https://doi.org/10.1038/s41467-018-06311-0

TY - JOUR

T1 - Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2

AU - Liang, Zhi Qin

AU - Zhuang, Tao Tao

AU - Seifitokaldani, Ali

AU - Li, Jun

AU - Huang, Chun Wei

AU - Tan, Chih Shan

AU - Li, Yi

AU - De Luna, Phil

AU - Dinh, Cao Thang

AU - Hu, Yongfeng

AU - Xiao, Qunfeng

AU - Hsieh, Pei Lun

AU - Wang, Yuhang

AU - Li, Fengwang

AU - Quintero-Bermudez, Rafael

AU - Zhou, Yansong

AU - Chen, Peining

AU - Pang, Yuanjie

AU - Lo, Shen Chuan

AU - Chen, Lih Juann

AU - Tan, Hairen

AU - Xu, Zheng

AU - Zhao, Suling

AU - Sinton, David

AU - Sargent, Edward H.

N1 - Funding Information: This work was supported financially by the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, and the CIFAR Bio-Inspired Solar Energy program. Computations were performed on the SOSCIP Consortium’s Blue Gene/Q computing platform. SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada Ltd., Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. X-ray absorption spectra were performed on SXRMB beamlines at the Canadian Light Source (CLS), which is supported by the Canada Foundation for Innovation, Natural Sciences and Engineering Research Council of Canada, the University of Saskatchewan, the Government of Saskatchewan, Western Economic Diversification Canada, the National Research Council Canada, and the Canadian Institutes of Health Research. Z.L. acknowledges a scholarship from the China Scholarship Council (CSC) (201607090041) and Basic and Innovation Program, Beijing Jiaotong University (KSJB17016536). A.S. acknowledges Fonds de Recherche du Quebec-Nature et Technologies (FRQNT) for the postdoctoral fellowship award. P.D.L. acknowledges support from NSERC in the form of the Canada Graduate Scholarship. H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511) to support his postdoctoral research at University of Toronto. The authors thank C. Q. Zou, M. X. Liu, F. F. Fan, J. Xing and L. Gao from University of Toronto for fruitful discussions. Publisher Copyright: © 2018, The Author(s).

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Copper-based materials are promising electrocatalysts for CO2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C2+ products. We achieve a 40-fold enhancement in the ratio of C2+ to the competing CH4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO2 reduction to multi-carbon products.

AB - Copper-based materials are promising electrocatalysts for CO2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C2+ products. We achieve a 40-fold enhancement in the ratio of C2+ to the competing CH4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO2 reduction to multi-carbon products.

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U2 - 10.1038/s41467-018-06311-0

DO - 10.1038/s41467-018-06311-0

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VL - 9

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 3828

ER -

Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO₂

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