Insight into the catalytic performance and reaction routes for toluene total oxidation over facilely prepared Mn-Cu bimetallic oxide catalysts

被引:90
|
作者
Li, Jian-Rong [1 ,2 ,3 ]
Zhang, Wan-Peng [1 ,2 ,3 ]
Li, Chang [1 ,2 ]
Xiao, Hang [1 ,2 ,3 ]
He, Chi [4 ,5 ]
机构
[1] Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
[2] Chinese Acad Sci, Key Lab Urban Environm & Hlth, Inst Urban Environm, Xiamen 361021, Peoples R China
[3] Chinese Acad Sci, Zhejiang Key Lab Urban Environm Proc & Pollut Con, Ningbo Urban Environm Observat & Res Stn, Ningbo 315800, Peoples R China
[4] Xi An Jiao Tong Univ, Sch Energy & Power Engn, State Key Lab Multiphase Flow Power Engn, Xian 710049, Shaanxi, Peoples R China
[5] Univ Chinese Acad Sci, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
基金
中国国家自然科学基金;
关键词
Catalytic oxidation; Toluene; Hydrothermal-redox; Mn-Cu bimetallic oxides; PTR-MS; MANGANESE OXIDE; PTR-MS; COPPER CATALYST; COMBUSTION; SPINEL; REMOVAL; METHANOL; CO; COPRECIPITATION; PRECIPITATION;
D O I
10.1016/j.apsusc.2021.149179
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Developing facile preparation method to obtain the satisfied low-temperature catalytic performance of transitional metal oxide-based materials is still a challenge in deep degradation of VOCs. Here, a series of Mn-Cu bimetallic oxide catalysts were prepared by one-step hydrothermal-redox method for catalytic total oxidation of toluene. The CH3COOH concentration, Cu/Mn molar ratio and calcination temperature greatly affected the crystal structure, micromorphology and catalytic performance. Amongst, MnCu spinel structured catalyst exhibited excellent low-temperature catalytic activity, superior durability and water resistance in toluene total oxidation owing to its abundant surface adsorbed oxygen species, higher amount of Cu+ and Mn3+ and excellent low-temperature reducibility. The reaction rate of MnCu was 7.0 times higher than that of MnCu0.5 at 210 ?C. The cyclic redox process with enough oxygen vacancy played a vital role in toluene oxidation. The deep oxidation of benzene was the key step in the toluene oxidation. Proton transfer reaction-mass spectrometry (PTRMS) results revealed the reaction intermediates including benzaldehyde, benzene and phenol, which further decomposed to acetone, ethanol, acetic acid, ketone and acetaldehyde by ring opening before total mineralization. Therefore, PTR-MS provided a facile method to investigate the reaction mechanism of toluene oxidation.
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页数:14
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