Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

Xue Wang; Ziyun Wang; F. Pelayo García de Arquer; Cao Thang Dinh; Adnan Ozden; Yuguang C. Li; Dae Hyun Nam; Jun Li; Yi Sheng Liu; Joshua Wicks; Zitao Chen; Miaofang Chi; Bin Chen; Ying Wang; Jason Tam; Jane Y. Howe; Andrew Proppe; Petar Todorović; Fengwang Li; Tao Tao Zhuang; Christine M. Gabardo; Ahmad R. Kirmani; Christopher McCallum; Sung Fu Hung; Yanwei Lum; Mingchuan Luo; Yimeng Min; Aoni Xu; Colin P. O’Brien; Bello Stephen; Bin Sun; Alexander H. Ip; Lee J. Richter; Shana O. Kelley; David Sinton; Edward H. Sargent

doi:10.1038/s41560-020-0607-8

Efficient electrically powered CO₂-to-ethanol via suppression of deoxygenation

Xue Wang, Ziyun Wang, F. Pelayo García de Arquer, Cao Thang Dinh, Adnan Ozden, Yuguang C. Li, Dae Hyun Nam, Jun Li, Yi Sheng Liu, Joshua Wicks, Zitao Chen, Miaofang Chi, Bin Chen, Ying Wang, Jason Tam, Jane Y. Howe, Andrew Proppe, Petar Todorović, Fengwang Li, Tao Tao ZhuangChristine M. Gabardo, Ahmad R. Kirmani, Christopher McCallum, Sung Fu Hung, Yanwei Lum, Mingchuan Luo, Yimeng Min, Aoni Xu, Colin P. O’Brien, Bello Stephen, Bin Sun, Alexander H. Ip, Lee J. Richter, Shana O. Kelley, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

Department of Applied Chemistry

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

398 Scopus citations

Abstract

The carbon dioxide electroreduction reaction (CO₂RR) provides ways to produce ethanol but its Faradaic efficiency could be further improved, especially in CO₂RR studies reported at a total current density exceeding 10 mA cm⁻². Here we report a class of catalysts that achieve an ethanol Faradaic efficiency of (52 ± 1)% and an ethanol cathodic energy efficiency of 31%. We exploit the fact that suppression of the deoxygenation of the intermediate HOCCH* to ethylene promotes ethanol production, and hence that confinement using capping layers having strong electron-donating ability on active catalysts promotes C–C coupling and increases the reaction energy of HOCCH* deoxygenation. Thus, we have developed an electrocatalyst with confined reaction volume by coating Cu catalysts with nitrogen-doped carbon. Spectroscopy suggests that the strong electron-donating ability and confinement of the nitrogen-doped carbon layers leads to the observed pronounced selectivity towards ethanol.

Original language	English
Pages (from-to)	478-486
Number of pages	9
Journal	Nature Energy
Volume	5
Issue number	6
DOIs	https://doi.org/10.1038/s41560-020-0607-8
State	Published - 1 Jun 2020

UN SDGs

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

Access to Document

10.1038/s41560-020-0607-8

Cite this

Wang, X., Wang, Z., García de Arquer, F. P., Dinh, C. T., Ozden, A., Li, Y. C., Nam, D. H., Li, J., Liu, Y. S., Wicks, J., Chen, Z., Chi, M., Chen, B., Wang, Y., Tam, J., Howe, J. Y., Proppe, A., Todorović, P., Li, F., ... Sargent, E. H. (2020). Efficient electrically powered CO₂-to-ethanol via suppression of deoxygenation. Nature Energy, 5(6), 478-486. https://doi.org/10.1038/s41560-020-0607-8

@article{86c0bc6329344e8d971ed801e5513744,

title = "Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation",

abstract = "The carbon dioxide electroreduction reaction (CO2RR) provides ways to produce ethanol but its Faradaic efficiency could be further improved, especially in CO2RR studies reported at a total current density exceeding 10 mA cm−2. Here we report a class of catalysts that achieve an ethanol Faradaic efficiency of (52 ± 1)% and an ethanol cathodic energy efficiency of 31%. We exploit the fact that suppression of the deoxygenation of the intermediate HOCCH* to ethylene promotes ethanol production, and hence that confinement using capping layers having strong electron-donating ability on active catalysts promotes C–C coupling and increases the reaction energy of HOCCH* deoxygenation. Thus, we have developed an electrocatalyst with confined reaction volume by coating Cu catalysts with nitrogen-doped carbon. Spectroscopy suggests that the strong electron-donating ability and confinement of the nitrogen-doped carbon layers leads to the observed pronounced selectivity towards ethanol.",

author = "Xue Wang and Ziyun Wang and {Garc{\'i}a de Arquer}, {F. Pelayo} and Dinh, {Cao Thang} and Adnan Ozden and Li, {Yuguang C.} and Nam, {Dae Hyun} and Jun Li and Liu, {Yi Sheng} and Joshua Wicks and Zitao Chen and Miaofang Chi and Bin Chen and Ying Wang and Jason Tam and Howe, {Jane Y.} and Andrew Proppe and Petar Todorovi{\'c} and Fengwang Li and Zhuang, {Tao Tao} and Gabardo, {Christine M.} and Kirmani, {Ahmad R.} and Christopher McCallum and Hung, {Sung Fu} and Yanwei Lum and Mingchuan Luo and Yimeng Min and Aoni Xu and O{\textquoteright}Brien, {Colin P.} and Bello Stephen and Bin Sun and Ip, {Alexander H.} and Richter, {Lee J.} and Kelley, {Shana O.} and David Sinton and Sargent, {Edward H.}",

year = "2020",

month = jun,

day = "1",

doi = "10.1038/s41560-020-0607-8",

language = "English",

volume = "5",

pages = "478--486",

journal = "Nature Energy",

issn = "2058-7546",

publisher = "Springer Nature",

number = "6",

}

Wang, X, Wang, Z, García de Arquer, FP, Dinh, CT, Ozden, A, Li, YC, Nam, DH, Li, J, Liu, YS, Wicks, J, Chen, Z, Chi, M, Chen, B, Wang, Y, Tam, J, Howe, JY, Proppe, A, Todorović, P, Li, F, Zhuang, TT, Gabardo, CM, Kirmani, AR, McCallum, C, Hung, SF, Lum, Y, Luo, M, Min, Y, Xu, A, O’Brien, CP, Stephen, B, Sun, B, Ip, AH, Richter, LJ, Kelley, SO, Sinton, D & Sargent, EH 2020, 'Efficient electrically powered CO₂-to-ethanol via suppression of deoxygenation', Nature Energy, vol. 5, no. 6, pp. 478-486. https://doi.org/10.1038/s41560-020-0607-8

TY - JOUR

T1 - Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

AU - Wang, Xue

AU - Wang, Ziyun

AU - García de Arquer, F. Pelayo

AU - Dinh, Cao Thang

AU - Ozden, Adnan

AU - Li, Yuguang C.

AU - Nam, Dae Hyun

AU - Li, Jun

AU - Liu, Yi Sheng

AU - Wicks, Joshua

AU - Chen, Zitao

AU - Chi, Miaofang

AU - Chen, Bin

AU - Wang, Ying

AU - Tam, Jason

AU - Howe, Jane Y.

AU - Proppe, Andrew

AU - Todorović, Petar

AU - Li, Fengwang

AU - Zhuang, Tao Tao

AU - Gabardo, Christine M.

AU - Kirmani, Ahmad R.

AU - McCallum, Christopher

AU - Hung, Sung Fu

AU - Lum, Yanwei

AU - Luo, Mingchuan

AU - Min, Yimeng

AU - Xu, Aoni

AU - O’Brien, Colin P.

AU - Stephen, Bello

AU - Sun, Bin

AU - Ip, Alexander H.

AU - Richter, Lee J.

AU - Kelley, Shana O.

AU - Sinton, David

AU - Sargent, Edward H.

PY - 2020/6/1

Y1 - 2020/6/1

N2 - The carbon dioxide electroreduction reaction (CO2RR) provides ways to produce ethanol but its Faradaic efficiency could be further improved, especially in CO2RR studies reported at a total current density exceeding 10 mA cm−2. Here we report a class of catalysts that achieve an ethanol Faradaic efficiency of (52 ± 1)% and an ethanol cathodic energy efficiency of 31%. We exploit the fact that suppression of the deoxygenation of the intermediate HOCCH* to ethylene promotes ethanol production, and hence that confinement using capping layers having strong electron-donating ability on active catalysts promotes C–C coupling and increases the reaction energy of HOCCH* deoxygenation. Thus, we have developed an electrocatalyst with confined reaction volume by coating Cu catalysts with nitrogen-doped carbon. Spectroscopy suggests that the strong electron-donating ability and confinement of the nitrogen-doped carbon layers leads to the observed pronounced selectivity towards ethanol.

AB - The carbon dioxide electroreduction reaction (CO2RR) provides ways to produce ethanol but its Faradaic efficiency could be further improved, especially in CO2RR studies reported at a total current density exceeding 10 mA cm−2. Here we report a class of catalysts that achieve an ethanol Faradaic efficiency of (52 ± 1)% and an ethanol cathodic energy efficiency of 31%. We exploit the fact that suppression of the deoxygenation of the intermediate HOCCH* to ethylene promotes ethanol production, and hence that confinement using capping layers having strong electron-donating ability on active catalysts promotes C–C coupling and increases the reaction energy of HOCCH* deoxygenation. Thus, we have developed an electrocatalyst with confined reaction volume by coating Cu catalysts with nitrogen-doped carbon. Spectroscopy suggests that the strong electron-donating ability and confinement of the nitrogen-doped carbon layers leads to the observed pronounced selectivity towards ethanol.

UR - http://www.scopus.com/inward/record.url?scp=85084419355&partnerID=8YFLogxK

U2 - 10.1038/s41560-020-0607-8

DO - 10.1038/s41560-020-0607-8

M3 - Article

AN - SCOPUS:85084419355

SN - 2058-7546

VL - 5

SP - 478

EP - 486

JO - Nature Energy

JF - Nature Energy

IS - 6

ER -

Efficient electrically powered CO₂-to-ethanol via suppression of deoxygenation

Abstract

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this