Synergistic catalysis of NO and chlorobenzene over Mn3O4-CeO2 catalysts: Acid sites, catalytic pathway and mechanism

被引:3
作者
Xia, Guanghua [1 ]
Ye, Zhiping [2 ]
Xu, Chaoxing [3 ]
Wang, Guanjie [4 ,5 ]
Zhang, Yuan [1 ]
Yang, Binrui [1 ]
机构
[1] Taizhou Univ, Sch Life Sci, Taizhou 318000, Peoples R China
[2] Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Peoples R China
[3] Taizhou Environm Sci Design & Res Inst Co Ltd, Taizhou 318000, Peoples R China
[4] Zhejiang Univ, Taizhou Inst, Taizhou 318000, Peoples R China
[5] Zhejiang Univ, Zhejiang Key Lab Adv Solid State Energy Storage Te, Taizhou Inst, Taizhou 318000, Peoples R China
来源
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING | 2024年 / 12卷 / 05期
关键词
Dioxin; Mn-Ce bimetallic oxide; Degradation pathway; Synergistic catalystic; NOx; ACTIVE-SITES; COMBUSTION; REDUCTION;
D O I
10.1016/j.jece.2024.113674
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Catalyst active sites and surface acidity are crucial for the synergistic catalysis of NOx x and dioxins, determining the selectivity towards N2 2 and CO2. 2 . This study synthesized Mn3O4-CeO2 3 O 4-CeO 2 catalysts to investigate the influence of these sites on the catalytic performance for NO and chlorobenzene. Mn0.086Ce, 0.086 Ce, made by the redox method, showed the highest Mn-Ce interface, achieving nearly complete conversion of chlorobenzene and NO at 180 degrees C, with CO2 2 and N2 2 selectivity reaching about 80 % and 100 %, respectively. EPR, NH3-TPD 3-TPD and Py-IR analyses revealed that the Mn-Ce interface induces the formation of Lewis acid sites and oxygen vacancies, facilitating the adsorption and conversion of chlorobenzene, NH3, 3 , and NO. Mn adjacent to Lewis acid sites is the main active site, while Ce acts as an electron transfer agent. Based on the results of in-situ DRIFTS and TOF-SIMS, the possible degradation pathway for chlorobenzene was proposed and as follows: phenol, benzoquinone, maleic anhydride, propionic acid, CO2, 2 , and H2O. 2 O. The NH3-SCR 3-SCR reaction follows the Eley-Rideal mechanism at 150-300 degrees C.
引用
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页数:10
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