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 and Edward H. Sargent ()
Additional contact information
Xue Wang: University of Toronto
Ziyun Wang: University of Toronto
F. Pelayo García de Arquer: University of Toronto
Cao-Thang Dinh: University of Toronto
Adnan Ozden: University of Toronto
Yuguang C. Li: University of Toronto
Dae-Hyun Nam: University of Toronto
Jun Li: University of Toronto
Yi-Sheng Liu: Advanced Light Source, Lawrence Berkeley National Laboratory
Joshua Wicks: University of Toronto
Zitao Chen: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Miaofang Chi: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Bin Chen: University of Toronto
Ying Wang: University of Toronto
Jason Tam: University of Toronto
Jane Y. Howe: University of Toronto
Andrew Proppe: University of Toronto
Petar Todorović: University of Toronto
Fengwang Li: University of Toronto
Tao-Tao Zhuang: University of Toronto
Christine M. Gabardo: University of Toronto
Ahmad R. Kirmani: Materials Science and Engineering Division, National Institute of Standards and Technology (NIST)
Christopher McCallum: University of Toronto
Sung-Fu Hung: University of Toronto
Yanwei Lum: University of Toronto
Mingchuan Luo: University of Toronto
Yimeng Min: University of Toronto
Aoni Xu: University of Toronto
Colin P. O’Brien: University of Toronto
Bello Stephen: Hitachi HTA Microscopy Lab
Bin Sun: University of Toronto
Alexander H. Ip: University of Toronto
Lee J. Richter: Materials Science and Engineering Division, National Institute of Standards and Technology (NIST)
Shana O. Kelley: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto

Nature Energy, 2020, vol. 5, issue 6, 478-486

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41560-020-0607-8

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