氯甲烷
尖晶石
二氯甲烷
催化作用
电催化剂
化学
X射线光电子能谱
无机化学
化学工程
电化学
材料科学
物理化学
有机化学
冶金
电极
工程类
溶剂
作者
Jing Yang,Shiying Fan,Xinyong Li,Yiyuan Tao,Jingang Wang,Guohua Chen
标识
DOI:10.1016/j.cej.2023.144040
摘要
Electrochemical selective dechlorination of dichloromethane (DCM) to chloromethane is a promising and sustainable strategy of resources. However, the current lack of high-performance electrocatalysts and complicated dechlorination mechanisms pose significant challenges. In this study, we report a series of Cu single-atom catalysts (SACs) supported on Co3O4-β spinel with a tube-in-tube nanofiber structure, denoted as Cux SACs/Co3O4-β, where x represents the theoretical Cu loading (0.26 wt%, 0.30 wt% and 0.50 wt%). These catalysts effectively dechlorinate DCM, producing high-value hydrocarbons like chloromethane and methane. Notably, Cu0.30 SACs/Co3O4-β exhibited a high chloromethane production rate (2931 μmol g−1h−1) and selectivity (76%) at −2.98 V vs (Ag/AgCl/Me4NCl) due to the synergy of cobaltosic oxide (Co3O4) spinel and Cu single atom. X-ray photoelectron spectroscopy and electron paramagnetic resonance experiments confirmed the presence of additional surface oxygen vacancies in Cu0.30 SACs/Co3O4-β, which improved the electrocatalysis performance for DCM dechlorination. Furthermore, a concerted dechlorination mechanism was suggested based on the transfer coefficient α. This research paves the way for the development of novel spinel electrocatalysts and the advancement of dechlorination reactions.
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