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

Institute of Electronics

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

380 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
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 - 1 Dec 2018

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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{154557ae2dbd4701835284801425c3ab,

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 Chih-Shan Tan 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 Lih-Juann Chen and Yu, {Shu Hong} and Kelley, {Shana O.} and David Sinton and Sargent, {Edward H.}",

year = "2018",

month = dec,

day = "1",

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

language = "English",

volume = "1",

pages = "946--951",

journal = "Nature Catalysis",

issn = "2520-1158",

publisher = "Nature Publishing Group",

number = "12",

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Zhuang, TT, Pang, Y, Liang, ZQ, Wang, Z, Li, Y, Tan, C-S, 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, L-J, 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.

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.

UR - https://www.mendeley.com/catalogue/3fe3e9a9-0c7a-3f49-ac51-55df461301e2/

U2 - 10.1038/s41929-018-0168-4

DO - 10.1038/s41929-018-0168-4

M3 - Article

SN - 2520-1158

VL - 1

SP - 946

EP - 951

JO - Nature Catalysis

JF - Nature Catalysis

IS - 12

ER -

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

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