TY - JOUR
T1 - Evaluation of the Flexibility for Catalytic Ozonation of Dichloromethane over Urchin-Like CuMnOxin Flue Gas with Complicated Components
AU - Xiang, Li
AU - Lin, Fawei
AU - Cai, Bohang
AU - Wang, Kaiwen
AU - Wang, Zhihua
AU - Yan, Beibei
AU - Chen, Guanyi
AU - He, Chi
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/9/20
Y1 - 2022/9/20
N2 - The evaluation of the poisoning effect of complex components in practical gas on DCM (dichloromethane) catalytic ozonation is of great significance for enhancing the technique's environmental flexibility. Herein, Ca, Pb, As, and NO/SO2 were selected as a typical alkaline-earth metal, heavy metal, metalloid, and acid gas, respectively, to evaluate their interferences on catalytic behaviors and surface properties of an optimized urchin-like CuMn catalyst. Ca/Pb loading weakens the formation of oxygen vacancies, oxygen mobility, and acidity due to the fusion of Mn-Ca/Pb-O, leading to their inferior catalytic performance with poor CO2 selectivity and mineralization rate. Noticeably, the presence of As induces excessively strong acidity, facilitating the inevitable formation of byproducts. Catalytic co-ozonation of NO/DCM is achieved with stoichiometric ozone addition. Unfortunately, SO2 introduction brings irreversible deactivation due to strong competition adsorption and the loss of active sites. Unexpectedly, Ca loading protects active sites from an attack by SO2. The formation of unstable sulfites and the released Mn-O structure offset the negative effect from SO2. Overall, the catalytic ozonation of DCM exhibits a distinctive priority in the antipoisoning of metals with the maintenance of DCM conversion. The construction of more stable acid sites should be the future direction of catalyst design; otherwise, catalytic ozonation should be arranged together with post heavy metal capture and a deacidification system.
AB - The evaluation of the poisoning effect of complex components in practical gas on DCM (dichloromethane) catalytic ozonation is of great significance for enhancing the technique's environmental flexibility. Herein, Ca, Pb, As, and NO/SO2 were selected as a typical alkaline-earth metal, heavy metal, metalloid, and acid gas, respectively, to evaluate their interferences on catalytic behaviors and surface properties of an optimized urchin-like CuMn catalyst. Ca/Pb loading weakens the formation of oxygen vacancies, oxygen mobility, and acidity due to the fusion of Mn-Ca/Pb-O, leading to their inferior catalytic performance with poor CO2 selectivity and mineralization rate. Noticeably, the presence of As induces excessively strong acidity, facilitating the inevitable formation of byproducts. Catalytic co-ozonation of NO/DCM is achieved with stoichiometric ozone addition. Unfortunately, SO2 introduction brings irreversible deactivation due to strong competition adsorption and the loss of active sites. Unexpectedly, Ca loading protects active sites from an attack by SO2. The formation of unstable sulfites and the released Mn-O structure offset the negative effect from SO2. Overall, the catalytic ozonation of DCM exhibits a distinctive priority in the antipoisoning of metals with the maintenance of DCM conversion. The construction of more stable acid sites should be the future direction of catalyst design; otherwise, catalytic ozonation should be arranged together with post heavy metal capture and a deacidification system.
KW - Catalytic ozonation
KW - Complex components
KW - CuMn
KW - Dichloromethane
KW - Poisoning effect
UR - https://www.scopus.com/pages/publications/85137910300
U2 - 10.1021/acs.est.2c03811
DO - 10.1021/acs.est.2c03811
M3 - 文章
C2 - 36074134
AN - SCOPUS:85137910300
SN - 0013-936X
VL - 56
SP - 13379
EP - 13390
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 18
ER -