Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide

Tao Tao Zhuang; Yuanjie Pang; Zhi Qin Liang; Ziyun Wang; Yi Li; Chih Shan Tan; Jun Li; Cao Thang Dinh; Phil De Luna; Pei Lun Hsieh; Thomas Burdyny; Hui Hui Li; Mengxia Liu; Yuhang Wang; Fengwang Li; Andrew Proppe; Andrew Johnston; Dae Hyun Nam; Zhen Yu Wu; Ya Rong Zheng; Alexander H. Ip; Hairen Tan; Lih Juann Chen; Shu Hong Yu; Shana O. Kelley; David Sinton; Edward H. Sargent

doi:10.1038/s41929-018-0168-4

Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide

Tao Tao Zhuang, Yuanjie Pang, Zhi Qin Liang, Ziyun Wang, Yi Li, Chih Shan Tan, Jun Li, Cao Thang Dinh, Phil De Luna, Pei Lun Hsieh, Thomas Burdyny, Hui Hui Li, Mengxia Liu, Yuhang Wang, Fengwang Li, Andrew Proppe, Andrew Johnston, Dae Hyun Nam, Zhen Yu Wu, Ya Rong ZhengAlexander H. Ip, Hairen Tan, Lih Juann Chen, Shu Hong Yu, Shana O. Kelley, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

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

195 Scopus citations

Abstract

The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu₂O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 ± 1% at a conversion rate of 7.8 ± 0.5 mA cm⁻² at −0.56 V versus a reversible hydrogen electrode.

Original language	English (US)
Pages (from-to)	946-951
Number of pages	6
Journal	Nature Catalysis
Volume	1
Issue number	12
DOIs	https://doi.org/10.1038/s41929-018-0168-4
State	Published - Dec 1 2018
Externally published	Yes

ASJC Scopus subject areas

Catalysis
Bioengineering
Biochemistry
Process Chemistry and Technology

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1038/s41929-018-0168-4

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Zhuang, T. T., Pang, Y., Liang, Z. Q., Wang, Z., Li, Y., Tan, C. S., Li, J., Dinh, C. T., De Luna, P., Hsieh, P. L., Burdyny, T., Li, H. H., Liu, M., Wang, Y., Li, F., Proppe, A., Johnston, A., Nam, D. H., Wu, Z. Y., ... Sargent, E. H. (2018). Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide. Nature Catalysis, 1(12), 946-951. https://doi.org/10.1038/s41929-018-0168-4

@article{b4cdcf9d4912472494b52615c93f58ad,

title = "Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide",

abstract = "The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu2O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 ± 1% at a conversion rate of 7.8 ± 0.5 mA cm−2 at −0.56 V versus a reversible hydrogen electrode.",

author = "Zhuang, {Tao Tao} and Yuanjie Pang and Liang, {Zhi Qin} and Ziyun Wang and Yi Li and Tan, {Chih Shan} and Jun Li and Dinh, {Cao Thang} and {De Luna}, Phil and Hsieh, {Pei Lun} and Thomas Burdyny and Li, {Hui Hui} and Mengxia Liu and Yuhang Wang and Fengwang Li and Andrew Proppe and Andrew Johnston and Nam, {Dae Hyun} and Wu, {Zhen Yu} and Zheng, {Ya Rong} and Ip, {Alexander H.} and Hairen Tan and Chen, {Lih Juann} and Yu, {Shu Hong} and Kelley, {Shana O.} and David Sinton and Sargent, {Edward H.}",

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 program and University of Toronto Connaught grant. The authors thank T. P. Wu, Z. Finfrock and L. Ma for technical support at the 9BM beam-line of the Advanced Photon Source (Lemont, IL). This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by 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. S.H.Y. acknowledges funding from the National Natural Science Foundation of China (Grant 21431006) and the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (Grant 21521001). The authors thank X. Wang and A. Seifitokaldani from the University of Toronto for fruitful discussions. Publisher Copyright: {\textcopyright} 2018, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2018",

month = dec,

day = "1",

doi = "10.1038/s41929-018-0168-4",

language = "English (US)",

volume = "1",

pages = "946--951",

journal = "Nature Catalysis",

issn = "2520-1158",

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Zhuang, TT, Pang, Y, Liang, ZQ, Wang, Z, Li, Y, Tan, CS, Li, J, Dinh, CT, De Luna, P, Hsieh, PL, Burdyny, T, Li, HH, Liu, M, Wang, Y, Li, F, Proppe, A, Johnston, A, Nam, DH, Wu, ZY, Zheng, YR, Ip, AH, Tan, H, Chen, LJ, Yu, SH, Kelley, SO, Sinton, D & Sargent, EH 2018, 'Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide', Nature Catalysis, vol. 1, no. 12, pp. 946-951. https://doi.org/10.1038/s41929-018-0168-4

TY - JOUR

T1 - Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide

AU - Zhuang, Tao Tao

AU - Pang, Yuanjie

AU - Liang, Zhi Qin

AU - Wang, Ziyun

AU - Li, Yi

AU - Tan, Chih Shan

AU - Li, Jun

AU - Dinh, Cao Thang

AU - De Luna, Phil

AU - Hsieh, Pei Lun

AU - Burdyny, Thomas

AU - Li, Hui Hui

AU - Liu, Mengxia

AU - Wang, Yuhang

AU - Li, Fengwang

AU - Proppe, Andrew

AU - Johnston, Andrew

AU - Nam, Dae Hyun

AU - Wu, Zhen Yu

AU - Zheng, Ya Rong

AU - Ip, Alexander H.

AU - Tan, Hairen

AU - Chen, Lih Juann

AU - Yu, Shu Hong

AU - Kelley, Shana O.

AU - Sinton, David

AU - Sargent, Edward H.

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 program and University of Toronto Connaught grant. The authors thank T. P. Wu, Z. Finfrock and L. Ma for technical support at the 9BM beam-line of the Advanced Photon Source (Lemont, IL). This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by 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. S.H.Y. acknowledges funding from the National Natural Science Foundation of China (Grant 21431006) and the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (Grant 21521001). The authors thank X. Wang and A. Seifitokaldani from the University of Toronto for fruitful discussions. Publisher Copyright: © 2018, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2018/12/1

Y1 - 2018/12/1

N2 - The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu2O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 ± 1% at a conversion rate of 7.8 ± 0.5 mA cm−2 at −0.56 V versus a reversible hydrogen electrode.

AB - The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu2O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 ± 1% at a conversion rate of 7.8 ± 0.5 mA cm−2 at −0.56 V versus a reversible hydrogen electrode.

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U2 - 10.1038/s41929-018-0168-4

DO - 10.1038/s41929-018-0168-4

M3 - Article

AN - SCOPUS:85055997943

VL - 1

SP - 946

EP - 951

JO - Nature Catalysis

JF - Nature Catalysis

SN - 2520-1158

IS - 12

ER -

Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide

Abstract

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