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Identifying Intermediates in CO2-to-C2H4 Electrochemical Reduction by In Situ Surface-Enhanced Raman Spectroscopy
Wen-Wen Wang1,2,3, Feng Chen1,4, Meng-Jiao Sun1,4
1State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou350002, China.
None:
Production of value-added C2+ products is an important topic in the research of electrochemical CO2 reduction reaction (CO2RR), and in situ spectroscopy identifies key intermediates and provides important details for a deeper understanding of the reaction mechanism. Applying a "borrowing" surface-enhanced Raman spectroscopy (SERS) strategy, core-shell Au@Cu2O nanocatalysts with different shell thickness were used to probe the CO2RR pathways on the surface of Cu2O in both neutral (KHCO3 + KCl) and alkaline (KOH) electrolytes. In situ Raman spectroscopic measurements showed that the SERS effect occurs at the apparent shell thicknesses of up to 100 nm. Comparative analysis uncovers the correlation between low-frequency-binding (LFB) and high-frequency-binding (HFB) *CO intermediates and electrochemical selectivity. A higher *COLFB/*COHFB ratio favors the generation of C2H4, while abundant *COHFB leads to predominant CO formation.
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