化学
质子化
电化学
水溶液
密度泛函理论
铜
吸附
拉曼光谱
无机化学
质子
单晶
金属
电解质
反应中间体
光谱学
物理化学
计算化学
结晶学
催化作用
电极
离子
有机化学
物理
光学
量子力学
作者
Feng Shao,Zhaoming Xia,Futian You,Jun Kit Wong,Qi Hang Low,Hai Xiao,Boon Siang Yeo
标识
DOI:10.1002/anie.202214210
摘要
We have employed in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) and density functional theory (DFT) calculations to study the CO reduction reaction (CORR) on Cu single-crystal surfaces under various conditions. Coadsorbed and structure-/potential-dependent surface species, including *CO, Cu-Oad , and Cu-OHad , were identified using electrochemical spectroscopy and isotope labeling. The relative abundance of *OH follows a "volcano" trend with applied potentials in aqueous solutions, which is yet absent in absolute alcoholic solutions. Combined with DFT calculations, we propose that the surface H2 O can serve as a strong proton donor for the first protonation step in both the C1 and C2 pathways of CORR at various applied potentials in alkaline electrolytes, leaving adsorbed *OH on the surface. This work provides fresh insights into the initial protonation steps and identity of key interfacial intermediates formed during CORR on Cu surfaces.
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