Electron-Rich Ce–O–Con+ Site Boosts Propane Total Oxidation and SO2 Tolerance on the Co3O4 Catalyst
催化作用
丙烷
化学
无机化学
材料科学
有机化学
生物化学
作者
Yanfei Zheng,Qian Zhao,Weinuo Xu,Rui Han,Qingling Liu
出处
期刊:ACS Sustainable Chemistry & Engineering [American Chemical Society] 日期:2025-01-17
标识
DOI:10.1021/acssuschemeng.4c09591
摘要
Light alkanes are widely found in industrial and vehicle exhausts, which pose a serious threat to the environment and human health. Herein, 0.05Ce–Co3O4 with atomic dispersion of Ce species in the Co3O4 was synthesized by a simple sol–gel method. It achieves 90% propane conversion at 186 °C, about 102 °C lower than that of the commercial Pt/Al2O3 catalyst. Moreover, it showed excellent long-term stability (140 h), water resistance (5.5 vol %), and sulfur resistance stability. Combined with characterization and theoretical calculation, it was confirmed that atomically dispersed Ce is confined in the Co3O4 lattice and induces an electron-rich Co site (Ce–O–Con+), which enhances propane adsorption and promotes the cleavage of the C–H bond. Besides, the oxygen vacancies of the 0.05Ce–Co3O4 are significantly increased, leading to a remarkable strength in the adsorption activation capacity for gaseous oxygen and oxygen species mobility, which is conducive to the deep oxidation of propane. Significantly, this unique active site also inhibits SO2 adsorption, endowing the product with excellent SO2-tolerance stability. Further, the monolithic catalyst presents excellent performance against various VOCs below 300 °C and still maintains good sulfur resistance. This study provides a new clue to design efficient C–H bond activation catalysts that are attractive for practical applications.