Boosting SO2-tolerant oxidation of Hg0 and chlorobenzene over MnCo2O4@TiO2 catalyst via constructing shielding effects

被引:6
|
作者
Shi, Qiqi [1 ]
Gao, Pei [1 ]
Shen, Boxiong [1 ,5 ]
Zhang, Xiao [1 ]
Li, Shuhao [1 ,3 ,4 ]
Lyu, Honghong [1 ]
Liu, Shiyao [2 ]
Kang, Dongrui [1 ]
Zhang, Chenguang [1 ]
机构
[1] Hebei Univ Technol, Sch Energy & Environm Engn, Tianjin Key Lab Clean Energy & Pollut Control, Tianjin 300401, Peoples R China
[2] Zhejiang Univ, Inst Adv Machines, Hangzhou 310000, Peoples R China
[3] Swinburne Univ Technol, Sch Sci Comp & Engn Technol, Dept Chem & Biotechnol, Melbourne, Vic 3122, Australia
[4] CSIRO Mfg, Private Bag 10, South Clayton, Vic 3169, Australia
[5] Hebei Univ Technol, 5340 Xiping Rd, Tianjin, Peoples R China
基金
中国国家自然科学基金;
关键词
Elemental mercury; CVOCs; Simultaneous oxidation; Stability; Flue gas; ELEMENTAL MERCURY REMOVAL; IN-SITU; OXIDE CATALYST; FLUE-GAS; MN; SCR; CE; CO; MECHANISMS; NOX;
D O I
10.1016/j.seppur.2023.125845
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Currently, it was still challenging to improve the SO2-tolerant catalytic oxidation of Hg0 and chlorobenzene in flue gas. Herein, we developed a MnCo2O4@TiO2 core-shell material that employed a self-shielding mechanism to prevent sulfate deposition. The optimal MnCo2O4@TiO2-2 catalyst achieved 100 % Hg0 removal efficiency at 250 degrees C under 150-600 ppm SO2, and also showed enhanced SO2 resistance during chlorobenzene conversion at 275 degrees C. The strong interaction between MnCo2O4 and TiO2 facilitated the electronic transfer from MnCo2O4 to TiO2, thereby producing more Co3+ and maintaining the high reactivity. Further, the mesoporous TiO2 layer facilitated the generation of moderate acid sites, improved the distribution of surface oxygen species, and weakened SO2 adsorption on catalyst. Under the protection of mesoporous TiO2 layer, the generation of Mn/Co sulfates could be inhibited effectively. In particular, the suitable TiO2 shell balanced the chemical adsorption and oxidation processes of Hg0 on the catalyst. This enhancement led to improved single Hg0 removal efficiency and SO2-tolerant Hg0 removal performance. During chlorobenzene degradation in presence of SO2, the oxidation path of chlorobenzene on MnCo2O4@TiO2 occurred via chlorobenzene -> phenolates -> maleates -> formates/ace-tates -> CO2 and H2O. Although sulfate formation would cover the active surface and inhibit the reaction path, the TiO2 shell could attenuate this negative effect. This study provided a new approach for the development of SO2-tolerant transition metal oxide with superior performance, holding significant academic and practical value.
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页数:13
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