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

Research output: Contribution to journalArticlepeer-review

31 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 languageEnglish
Pages (from-to)478-486
Number of pages9
JournalNature Energy
Volume5
Issue number6
DOIs
StatePublished - 1 Jun 2020

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