Ce-Mn binary oxides supported on Al2O3 (Ce-Mn/Al2O3), with enhanced activity and stability for catalytic ozonation of benzoic acid, were synthesized using a facile impregnation method. The competitive synergetic effects between cerium and manganese significantly influenced the structural characteristics and catalytic performance of the catalysts depending on the impregnation sequence. Catalysts prepared via the one-step impregnation process exhibited a higher concentration of homogeneous Ce3+ species on the catalyst surface. This led to an increase in surface oxygen vacancies, thereby enhancing catalytic activity. In contrast, the two-step impregnation process resulted in fewer oxygen vacancies due to reduced competitive effects between cerium and manganese. Overall, the optimized Ce-Mn/Al2O3 catalysts demonstrated improved catalytic performance in ozonation reactions, highlighting the importance of impregnation method and calcination conditions in tailoring catalyst properties for enhanced activity and stability. Oxygen vacancies play a crucial role as active sites for ozone adsorption and dissociation into *O-2 and *O, facilitated by the reduction of Mn4+ to Mn3+ and the oxidation of Ce3+ to Ce4+. This process forms an electron closed loop that maintains electron balance. The synergistic interactions between cerium and manganese enable rapid electron transfer between Ce4+ and Mn3+, facilitating the regeneration of Ce3+ and Mn4+. Due to the increase of the dual redox conjugate pairs and the surface reactive oxygen species, the catalytic ozonation activity and stability of Ce-Mn/Al2O3 was enhanced.
机构:
Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Hu, Rui
Li, Jia-Ying
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Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Li, Jia-Ying
Yu, Qiyi
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China United Engn Corp Ltd, Hangzhou 310052, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Yu, Qiyi
Yang, Sui-Qin
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Changsha Univ Sci & Technol, Sch Hydraul & Environm Engn, Changsha 410114, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Yang, Sui-Qin
Ci, Xinbo
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Hebei Think do Water Treatment Technol Co Ltd, Shijiazhuang 050035, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Ci, Xinbo
Qu, Bing
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Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Qu, Bing
Yang, Liwei
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Shandong Zhangqiu Blower Co Ltd, Jinan 250200, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Yang, Liwei
Liu, Zheng-Qian
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Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Liu, Zheng-Qian
Liu, Hongquan
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Hebei Think do Water Treatment Technol Co Ltd, Shijiazhuang 050035, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Liu, Hongquan
Yang, Jingjing
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Suzhou Univ Sci & Technol, Key Lab Suzhou Sponge City Technol, Suzhou 215009, Peoples R China
Suzhou Univ Sci & Technol, Sch Environm Sci & Engn, Suzhou 215009, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Yang, Jingjing
Sun, Shiquan
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Changsha Univ Sci & Technol, Sch Hydraul & Environm Engn, Changsha 410114, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
Sun, Shiquan
Cui, Yu-Hong
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Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R ChinaHuazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China