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Unveiling the Cation Effects on Electrocatalytic CO 2 Reduction via Operando Surface‐enhanced Raman Spectroscopy
Author(s) -
Chen Dexiang,
Wei Yunjia,
Sun Zixuan,
Zhao Xing,
Tang Xiao,
Zhu Xiangnan,
Li Guoqun,
Yao Lei,
Chen Shuying,
Lin Richen,
Wang Jiawei,
Li Qiang,
Fan Xingce,
Qiu Teng,
Hao Qi
Publication year - 2025
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202409569
Abstract The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) can be significantly improved by the presence of alkali metal cations, yet the underlying mechanisms remain unclear. In this study, we developed clean Cu nanoparticles with tailored curvatures to modulate the local concentration of K + cations and investigate their effects on CO 2 RR. The adjustment of particle curvature allows for direct control over cation concentrations within the electrochemical double layer, enabling broad‐range modulation of cation concentration without concerns regarding solubility limitations or anionic interference. By tuning the plasmonic modes of the Cu particles, we achieved highly sensitive surface‐enhanced Raman spectroscopy (SERS) under resonant conditions, facilitating in situ tracking of the short‐lived intermediates in CO 2 RR. Our results revealed that K + cations not only stabilize *COOH and *CO species and reduce the reaction energy barrier for C─C coupling but also increase the surface coverage of *CO, particularly for bridge *CO configurations. Furthermore, our findings suggest that the interactions between bridge *CO and atop *CO play a crucial role in facilitating the C─C coupling, offering insights for the design of electrocatalysts for CO 2 RR.

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