Author
Listed:
- Fengwang Li
(University of Toronto)
- Arnaud Thevenon
(California Institute of Technology)
- Alonso Rosas-Hernández
(California Institute of Technology)
- Ziyun Wang
(University of Toronto)
- Yilin Li
(University of Toronto)
- Christine M. Gabardo
(University of Toronto)
- Adnan Ozden
(University of Toronto)
- Cao Thang Dinh
(University of Toronto)
- Jun Li
(University of Toronto
University of Toronto)
- Yuhang Wang
(University of Toronto)
- Jonathan P. Edwards
(University of Toronto)
- Yi Xu
(University of Toronto)
- Christopher McCallum
(University of Toronto)
- Lizhi Tao
(University of California)
- Zhi-Qin Liang
(University of Toronto)
- Mingchuan Luo
(University of Toronto)
- Xue Wang
(University of Toronto)
- Huihui Li
(University of Toronto)
- Colin P. O’Brien
(University of Toronto)
- Chih-Shan Tan
(University of Toronto)
- Dae-Hyun Nam
(University of Toronto)
- Rafael Quintero-Bermudez
(University of Toronto)
- Tao-Tao Zhuang
(University of Toronto)
- Yuguang C. Li
(University of Toronto)
- Zhiji Han
(California Institute of Technology)
- R. David Britt
(University of California)
- David Sinton
(University of Toronto)
- Theodor Agapie
(California Institute of Technology)
- Jonas C. Peters
(California Institute of Technology)
- Edward H. Sargent
(University of Toronto)
Abstract
The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources1. However, the highly selective generation of economically desirable products such as ethylene from the carbon dioxide reduction reaction (CO2RR) remains a challenge2. Tuning the stabilities of intermediates to favour a desired reaction pathway can improve selectivity3–5, and this has recently been explored for the reaction on copper by controlling morphology6, grain boundaries7, facets8, oxidation state9 and dopants10. Unfortunately, the Faradaic efficiency for ethylene is still low in neutral media (60 per cent at a partial current density of 7 milliamperes per square centimetre in the best catalyst reported so far9), resulting in a low energy efficiency. Here we present a molecular tuning strategy—the functionalization of the surface of electrocatalysts with organic molecules—that stabilizes intermediates for more selective CO2RR to ethylene. Using electrochemical, operando/in situ spectroscopic and computational studies, we investigate the influence of a library of molecules, derived by electro-dimerization of arylpyridiniums11, adsorbed on copper. We find that the adhered molecules improve the stabilization of an ‘atop-bound’ CO intermediate (that is, an intermediate bound to a single copper atom), thereby favouring further reduction to ethylene. As a result of this strategy, we report the CO2RR to ethylene with a Faradaic efficiency of 72 per cent at a partial current density of 230 milliamperes per square centimetre in a liquid-electrolyte flow cell in a neutral medium. We report stable ethylene electrosynthesis for 190 hours in a system based on a membrane-electrode assembly that provides a full-cell energy efficiency of 20 per cent. We anticipate that this may be generalized to enable molecular strategies to complement heterogeneous catalysts by stabilizing intermediates through local molecular tuning.
Suggested Citation
Fengwang Li & Arnaud Thevenon & Alonso Rosas-Hernández & Ziyun Wang & Yilin Li & Christine M. Gabardo & Adnan Ozden & Cao Thang Dinh & Jun Li & Yuhang Wang & Jonathan P. Edwards & Yi Xu & Christopher , 2020.
"Molecular tuning of CO2-to-ethylene conversion,"
Nature, Nature, vol. 577(7791), pages 509-513, January.
Handle:
RePEc:nat:nature:v:577:y:2020:i:7791:d:10.1038_s41586-019-1782-2
DOI: 10.1038/s41586-019-1782-2
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