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 journalArticlepeer-review

89 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 languageEnglish
Pages (from-to)946-951
Number of pages6
JournalNature Catalysis
Volume1
Issue number12
DOIs
StatePublished - 1 Dec 2018

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