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Elucidating electrochemical CO2 reduction reaction processes on Cu(hkl) single-crystal surfaces by in situ Raman spectroscopy
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-08-05 , DOI: 10.1039/d2ee01334g
Yu Zhao , Xia-Guang Zhang , Bodappa Nataraju , Weimin Yang , Qian Liang , Petar Radjenovic , Yao-Hui Wang , Yue-Jiao Zhang , Jin-Chao Dong , Zhong-qun Tian , Jian-Feng Li

Cupric materials are known to catalyze the electrochemical CO2 reduction reaction (CO2RR) and significantly improve the selectivity of multi-carbon products. Surface facets and structural effects play a critical role in the CO2RR. However, these surface mechanisms are poorly understood, and identifying trace intermediates on atomically-flat Cu(hkl) single-crystal surfaces, in situ, is a tremendously challenging task requiring sophisticated technical know-how. Here, in situ Raman spectroscopy was used to provide critical evidence of CO2RR intermediates, especially the selectivity-determining intermediates *OCCO and *CH2CHO on Cu(hkl) surfaces. Combining the spectroscopic results with theoretical calculations, Cu(111) facilitates the generation of C1 products through the formation of *COOH and *CO, while Cu(110) further generates C2 through the pathway of *OCCO and *CH2CHO. In addition, high KHCO3 concentrations facilitate the formation of the *OCCO structure, promoting C2 products. This work provides a significant breakthrough for understanding the CO2RR mechanism that can guide the design of high-efficiency catalysts.

中文翻译:

通过原位拉曼光谱阐明 Cu(hkl) 单晶表面上的电化学 CO2 还原反应过程

已知铜材料可催化电化学 CO 2还原反应 (CO 2 RR) 并显着提高多碳产物的选择性。表面刻面和结构效应在 CO 2 RR中起着关键作用。然而,人们对这些表面机制知之甚少,在原子级平坦的 Cu( hkl ) 单晶表面上原位识别痕量中间体是一项极具挑战性的任务,需要复杂的技术知识。在这里,原位拉曼光谱用于提供 CO 2 RR 中间体的关键证据,尤其是决定选择性的中间体 *OCCO 和 *CH 2 CHO on Cu(hkl ) 表面。将光谱结果与理论计算相结合,Cu(111)通过*COOH和*CO的形成促进C 1产物的生成,而Cu(110)通过*OCCO和*CH 2 CHO的途径进一步生成C 2 。此外,高浓度的 KHCO 3促进 *OCCO 结构的形成,促进 C 2产物的形成。该工作为理解可指导高效催化剂设计的CO 2 RR机理提供了重大突破。
更新日期:2022-08-05
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