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Accelerating CO2 electroreduction to multicarbon products via synergistic electric-thermal field on copper nanoneedles.

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Title: Accelerating CO2 electroreduction to multicarbon products via synergistic electric-thermal field on copper nanoneedles.
Authors: Yang, B
Liu, K
Li, H
Liu, C
Fu, J
Li, H
Huang, JE
Ou, P
Alkayyali, T
Cai, C
Duan, Y
Liu, H
An, P
Zhang, N
Li, W
Qiu, X
Jia, C
Hu, J
Chai, L
Lin, Z
Gao, Y
Miyauchi, M
Cortés, E
Maier, SA
Liu, M
Item Type: Journal Article
Abstract: Electrochemical CO2 reduction is a promising way to mitigate CO2 emissions and close the anthropogenic carbon cycle. Among products from CO2RR, multicarbon chemicals, such as ethylene and ethanol with high energy density, are more valuable. However, the selectivity and reaction rate of C2 production are unsatisfactory due to the sluggish thermodynamics and kinetics of C-C coupling. The electric field and thermal field have been studied and utilized to promote catalytic reactions, as they can regulate the thermodynamic and kinetic barriers of reactions. Either raising the potential or heating the electrolyte can enhance C-C coupling, but these come at the cost of increasing side reactions, such as the hydrogen evolution reaction. Here, we present a generic strategy to enhance the local electric field and temperature simultaneously and dramatically improve the electric-thermal synergy desired in electrocatalysis. A conformal coating of ∼5 nm of polytetrafluoroethylene significantly improves the catalytic ability of copper nanoneedles (∼7-fold electric field and ∼40 K temperature enhancement at the tips compared with bare copper nanoneedles experimentally), resulting in an improved C2 Faradaic efficiency of over 86% at a partial current density of more than 250 mA cm-2 and a record-high C2 turnover frequency of 11.5 ± 0.3 s-1 Cu site-1. Combined with its low cost and scalability, the electric-thermal strategy for a state-of-the-art catalyst not only offers new insight into improving activity and selectivity of value-added C2 products as we demonstrated but also inspires advances in efficiency and/or selectivity of other valuable electro-/photocatalysis such as hydrogen evolution, nitrogen reduction, and hydrogen peroxide electrosynthesis.
Issue Date: 23-Feb-2022
Date of Acceptance: 1-Feb-2022
URI: http://hdl.handle.net/10044/1/94553
DOI: 10.1021/jacs.1c11253
ISSN: 0002-7863
Publisher: American Chemical Society
Start Page: 3039
End Page: 3049
Journal / Book Title: Journal of the American Chemical Society
Volume: 144
Issue: 7
Copyright Statement: © 2022 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in J. Am. Chem. Soc., after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.1c11253
Keywords: General Chemistry
03 Chemical Sciences
Publication Status: Published
Conference Place: United States
Embargo Date: 2023-02-02
Online Publication Date: 2022-02-03
Appears in Collections:Physics
Experimental Solid State
Faculty of Natural Sciences