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Probing Cation Effects on *CO Intermediates from Electroreduction of CO2 through Operando Raman Spectroscopy

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Title
Probing Cation Effects on *CO Intermediates from Electroreduction of CO2 through Operando Raman Spectroscopy
Author(s)
Si Young Lee; Jimin Kim; Bak, Gwangsu; Lee, Eunchong; Kim, Dayeon; Yoo, Suhwan; Jiwon Kim; Hyewon Yun; Yun Jeong Hwang
Publication Date
2023-10
Journal
Journal of the American Chemical Society, v.145, no.42, pp.23068 - 23075
Publisher
AMER CHEMICAL SOC
Abstract
Cations in an electrolyte modulate microenvironments near the catalyst surface and affect product distribution from an electrochemical CO2 reduction reaction, and thus, their interaction with intermediate states has been tried to be probed. Herein, we directly observed the cation effect on *CO intermediates on the Cu(OH)2-derived catalyst in real time through operando surface-enhanced Raman spectroscopy at high overpotentials (-1.0 VRHE). Atop *CO peaks are composed of low-frequency binding *CO (*COLFB) and high-frequency binding *CO (*COHFB) because of their adsorption sites. These two *CO intermediates are found to have different sensitivities to the cation-induced field, and each *CO is proposed to be suitably stabilized for efficient C-C coupling. The proportions between *COHFB and *COLFB are dependent on the type of alkali cations, and the increases in the *COHFB ratio have a high correlation with selective C2H4 production under K+ and Cs+, indicating that *COHFB is the dominant and fast active species. In addition, as the hydrated cation size decreases, *COLFB is more sensitively red-shifted than *COHFB, which promotes C-C coupling and suppresses C1 products. Through time-resolved operando measurements, dynamic changes between the two *CO species are observed, showing the rapid initial adsorption of *COHFB and subsequently reaching a steady ratio between *COLFB and *COHFB.
URI
https://pr.ibs.re.kr/handle/8788114/14398
DOI
10.1021/jacs.3c05799
ISSN
0002-7863
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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