Chitosan -NH2 derived efficient Co3O4 catalyst for styrene catalytic oxidation: Simultaneously regulating particle size and Co valence

被引:5
作者
Chen, Yinye [1 ]
Gong, Wanyu [1 ]
Niu, Kui [1 ]
Wang, Xin [1 ]
Lin, Yidian [1 ]
Lin, Daifeng [2 ]
Jin, Hongjun [1 ]
Luo, Yongjin [1 ]
Qian, Qingrong [1 ]
Chen, Qinghua [1 ]
机构
[1] Fujian Normal Univ, Fujian Key Lab Pollut Control & Resource Reuse, Fuzhou 350007, Peoples R China
[2] Fujian Polytech Normal Univ, Fujian Prov Key Lab Coastal Basin Environm, Fuqing 350300, Peoples R China
关键词
Catalytic styrene oxidation; Co3O4; Chitosan functional group; Surface acidity; Reaction mechanism; OXYGEN VACANCIES; TEMPERATURE; PERFORMANCE; OXIDE;
D O I
10.1016/j.jcis.2024.01.007
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
In this study, a Co3O4 catalyst is synthesised using the chitosan-assisted sol-gel method, which simultaneously regulates the grain size, Co valence and surface acidity of the catalyst through a chitosan functional group. The complexation of the free -NH2 complex inhibits particle agglomeration; thus, the average particle size of the catalyst decreases from 82 to 31 nm. Concurrently, Raman spectroscopy, hydrogen temperature-programmed reduction, electron paramagnetic resonance spectroscopy and X-ray photoelectron spectroscopy experiments demonstrate that doping with chitosan N sources effectively modulates Co2+ to promote the formation of oxygen vacancies. In addition, water washing after catalyst preparation can considerably improve the low-temperature (below 250 degrees C) activity of the catalyst and eliminate the side effects of alkali metal on catalyst activity. Moreover, the presence of Br & oslash;nsted and Lewis acid sites promotes the adsorption of C8H8. Consequently, CS/Co3O4-W presents the highest catalytic oxidation activity for C8H8 at low temperatures (R-250 degrees(C) = 8.33 mu mol g(-1) s(-1), WHSV = 120,000 mL hr(-1)center dot g(-1)). In situ DRIFTS and O-18(2) isotope experiments demonstrate that the oxidation of the C8H8 reaction is primarily dominated by the Mars-van Krevelen mechanism. Furthermore, CS/Co3O4-W exhibits superior water resistance (1- and 2- vol% H2O), which has the potential to be implemented in industrial applications.
引用
收藏
页码:439 / 448
页数:10
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