Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper

Yuanjie Pang; Jun Li; Ziyun Wang; Chih Shan Tan; Pei Lun Hsieh; Tao Tao Zhuang; Zhi Qin Liang; Chengqin Zou; Xue Wang; Phil De Luna; Jonathan P. Edwards; Yi Xu; Fengwang Li; Cao Thang Dinh; Miao Zhong; Yuanhao Lou; Dan Wu; Lih Juann Chen; Edward H. Sargent; David Sinton

doi:10.1038/s41929-019-0225-7

Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper

Yuanjie Pang, Jun Li, Ziyun Wang, Chih Shan Tan, Pei Lun Hsieh, Tao Tao Zhuang, Zhi Qin Liang, Chengqin Zou, Xue Wang, Phil De Luna, Jonathan P. Edwards, Yi Xu, Fengwang Li, Cao Thang Dinh, Miao Zhong, Yuanhao Lou, Dan Wu, Lih Juann Chen, Edward H. Sargent, David Sinton^*

^*Corresponding author for this work

Chemistry

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

132 Scopus citations

Abstract

The renewable-energy-powered electrocatalytic conversion of carbon dioxide and carbon monoxide into carbon-based fuels provides a means for the storage of renewable energy. We sought to convert carbon monoxide—an increasingly available and low-cost feedstock that could benefit from an energy-efficient upgrade in value—into n-propanol, an alcohol that can be directly used as engine fuel. Here we report that a catalyst consisting of highly fragmented copper structures can bring C ₁ and C ₂ binding sites together, and thereby promote further coupling of these intermediates into n-propanol. Using this strategy, we achieved an n-propanol selectivity of 20% Faradaic efficiency at a low potential of −0.45 V versus the reversible hydrogen electrode (ohmic corrected) with a full-cell energetic efficiency of 10.8%. We achieved a high reaction rate that corresponds to a partial current density of 8.5 mA cm ^–2 for n-propanol.

Original language	English (US)
Pages (from-to)	251-258
Number of pages	8
Journal	Nature Catalysis
Volume	2
Issue number	3
DOIs	https://doi.org/10.1038/s41929-019-0225-7
State	Published - Mar 1 2019

ASJC Scopus subject areas

Catalysis
Bioengineering
Biochemistry
Process Chemistry and Technology

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10.1038/s41929-019-0225-7

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Pang, Y., Li, J., Wang, Z., Tan, C. S., Hsieh, P. L., Zhuang, T. T., Liang, Z. Q., Zou, C., Wang, X., De Luna, P., Edwards, J. P., Xu, Y., Li, F., Dinh, C. T., Zhong, M., Lou, Y., Wu, D., Chen, L. J., Sargent, E. H., & Sinton, D. (2019). Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper. Nature Catalysis, 2(3), 251-258. https://doi.org/10.1038/s41929-019-0225-7

@article{ccdc0175eea245a6bef84392eba13255,

title = "Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper",

abstract = " The renewable-energy-powered electrocatalytic conversion of carbon dioxide and carbon monoxide into carbon-based fuels provides a means for the storage of renewable energy. We sought to convert carbon monoxide—an increasingly available and low-cost feedstock that could benefit from an energy-efficient upgrade in value—into n-propanol, an alcohol that can be directly used as engine fuel. Here we report that a catalyst consisting of highly fragmented copper structures can bring C 1 and C 2 binding sites together, and thereby promote further coupling of these intermediates into n-propanol. Using this strategy, we achieved an n-propanol selectivity of 20% Faradaic efficiency at a low potential of −0.45 V versus the reversible hydrogen electrode (ohmic corrected) with a full-cell energetic efficiency of 10.8%. We achieved a high reaction rate that corresponds to a partial current density of 8.5 mA cm –2 for n-propanol.",

author = "Yuanjie Pang and Jun Li and Ziyun Wang and Tan, {Chih Shan} and Hsieh, {Pei Lun} and Zhuang, {Tao Tao} and Liang, {Zhi Qin} and Chengqin Zou and Xue Wang and {De Luna}, Phil and Edwards, {Jonathan P.} and Yi Xu and Fengwang Li and Dinh, {Cao Thang} and Miao Zhong and Yuanhao Lou and Dan Wu and Chen, {Lih Juann} and Sargent, {Edward H.} and David Sinton",

note = "Funding Information: This work was supported by the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy programme, and the University of Toronto Connaught Program. This research used synchrotron resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by the Argonne National Laboratory, and was supported by the US DOE under contract no. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. The authors thank Z. Finfrock and M. J. Ward for technical support at the Sector 20BM beamline. D.S. acknowledges the NSERC E.W.R. Steacie Memorial Fellowship. J.L. acknowledges the Banting Postdoctoral Fellowships program. All DFT computations were performed on the IBM BlueGene/Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. Publisher Copyright: {\textcopyright} 2019, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2019",

month = mar,

day = "1",

doi = "10.1038/s41929-019-0225-7",

language = "English (US)",

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Pang, Y, Li, J, Wang, Z, Tan, CS, Hsieh, PL, Zhuang, TT, Liang, ZQ, Zou, C, Wang, X, De Luna, P, Edwards, JP, Xu, Y, Li, F, Dinh, CT, Zhong, M, Lou, Y, Wu, D, Chen, LJ, Sargent, EH & Sinton, D 2019, 'Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper', Nature Catalysis, vol. 2, no. 3, pp. 251-258. https://doi.org/10.1038/s41929-019-0225-7

TY - JOUR

T1 - Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper

AU - Pang, Yuanjie

AU - Li, Jun

AU - Wang, Ziyun

AU - Tan, Chih Shan

AU - Hsieh, Pei Lun

AU - Zhuang, Tao Tao

AU - Liang, Zhi Qin

AU - Zou, Chengqin

AU - Wang, Xue

AU - De Luna, Phil

AU - Edwards, Jonathan P.

AU - Xu, Yi

AU - Li, Fengwang

AU - Dinh, Cao Thang

AU - Zhong, Miao

AU - Lou, Yuanhao

AU - Wu, Dan

AU - Chen, Lih Juann

AU - Sargent, Edward H.

AU - Sinton, David

N1 - Funding Information: This work was supported by the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy programme, and the University of Toronto Connaught Program. This research used synchrotron resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by the Argonne National Laboratory, and was supported by the US DOE under contract no. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. The authors thank Z. Finfrock and M. J. Ward for technical support at the Sector 20BM beamline. D.S. acknowledges the NSERC E.W.R. Steacie Memorial Fellowship. J.L. acknowledges the Banting Postdoctoral Fellowships program. All DFT computations were performed on the IBM BlueGene/Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). SOSCIP is funded by the Federal Economic Development Agency of Southern Ontario, the Province of Ontario, IBM Canada, Ontario Centres of Excellence, Mitacs and 15 Ontario academic member institutions. Publisher Copyright: © 2019, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2019/3/1

Y1 - 2019/3/1

N2 - The renewable-energy-powered electrocatalytic conversion of carbon dioxide and carbon monoxide into carbon-based fuels provides a means for the storage of renewable energy. We sought to convert carbon monoxide—an increasingly available and low-cost feedstock that could benefit from an energy-efficient upgrade in value—into n-propanol, an alcohol that can be directly used as engine fuel. Here we report that a catalyst consisting of highly fragmented copper structures can bring C 1 and C 2 binding sites together, and thereby promote further coupling of these intermediates into n-propanol. Using this strategy, we achieved an n-propanol selectivity of 20% Faradaic efficiency at a low potential of −0.45 V versus the reversible hydrogen electrode (ohmic corrected) with a full-cell energetic efficiency of 10.8%. We achieved a high reaction rate that corresponds to a partial current density of 8.5 mA cm –2 for n-propanol.

AB - The renewable-energy-powered electrocatalytic conversion of carbon dioxide and carbon monoxide into carbon-based fuels provides a means for the storage of renewable energy. We sought to convert carbon monoxide—an increasingly available and low-cost feedstock that could benefit from an energy-efficient upgrade in value—into n-propanol, an alcohol that can be directly used as engine fuel. Here we report that a catalyst consisting of highly fragmented copper structures can bring C 1 and C 2 binding sites together, and thereby promote further coupling of these intermediates into n-propanol. Using this strategy, we achieved an n-propanol selectivity of 20% Faradaic efficiency at a low potential of −0.45 V versus the reversible hydrogen electrode (ohmic corrected) with a full-cell energetic efficiency of 10.8%. We achieved a high reaction rate that corresponds to a partial current density of 8.5 mA cm –2 for n-propanol.

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DO - 10.1038/s41929-019-0225-7

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JO - Nature Catalysis

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ER -

Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper

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