TY - JOUR
T1 - To promote catalytic ozonation of toluene by tuning Brönsted acid sites via introducing alkali metals into the OMS-2-SO42-/ZSM-5 catalyst
AU - Hong, Wei
AU - Liu, Yan
AU - Jiang, Xinxin
AU - An, Chenguang
AU - Zhu, Tianle
AU - Sun, Ye
AU - Wang, Haining
AU - Shen, Fangxia
AU - Li, Xiang
N1 - Publisher Copyright:
© 2023 Elsevier B.V.
PY - 2023/4/15
Y1 - 2023/4/15
N2 - Although free hydroxyl radical (·OH) generated on OMS-2-based catalysts during the catalytic ozonation process have been shown as important reactive oxygen species (ROSs) for toluene degradation, improvement of surface ·OH formation ability remains challenging. Here, Na, K, Rb, and Cs-OMS-2-SO42-/ZSM-5 catalysts were prepared, characterized and evaluated for catalytic ozonation of toluene. Both characterizations and DFT calculations showed that the appropriate alkali metal introduction made the catalyst possess with appropriate crystalline, reducibility, and acidity, which was favorable for catalytic ozonation of toluene. Characterizations also showed that alkali metal introduction resulted in water molecule adsorption on Brönsted acid sites of the catalysts, which made water molecule activation by ozone to form ·OH more easily. The introduction of K+ content of ∼ 5.9 wt% yielded K-OMS-2-SO42-/ZSM-5 catalyst with the highest Brönsted acid sites and thus formed the most ·OH among the five prepared catalysts. As a result, the catalyst exhibited excellent toluene conversion and COx selectivity for catalytic ozonation of toluene at room temperature and ambient humidity. Furthermore, the catalytic activity of deactivated K-OMS-2-SO42-/ZSM-5 catalyst was recovered after regeneration by a combination of water washing and heat treatment. Finally, a complete mechanism for toluene catalytic ozonation, catalyst deactivation, and regeneration was proposed.
AB - Although free hydroxyl radical (·OH) generated on OMS-2-based catalysts during the catalytic ozonation process have been shown as important reactive oxygen species (ROSs) for toluene degradation, improvement of surface ·OH formation ability remains challenging. Here, Na, K, Rb, and Cs-OMS-2-SO42-/ZSM-5 catalysts were prepared, characterized and evaluated for catalytic ozonation of toluene. Both characterizations and DFT calculations showed that the appropriate alkali metal introduction made the catalyst possess with appropriate crystalline, reducibility, and acidity, which was favorable for catalytic ozonation of toluene. Characterizations also showed that alkali metal introduction resulted in water molecule adsorption on Brönsted acid sites of the catalysts, which made water molecule activation by ozone to form ·OH more easily. The introduction of K+ content of ∼ 5.9 wt% yielded K-OMS-2-SO42-/ZSM-5 catalyst with the highest Brönsted acid sites and thus formed the most ·OH among the five prepared catalysts. As a result, the catalyst exhibited excellent toluene conversion and COx selectivity for catalytic ozonation of toluene at room temperature and ambient humidity. Furthermore, the catalytic activity of deactivated K-OMS-2-SO42-/ZSM-5 catalyst was recovered after regeneration by a combination of water washing and heat treatment. Finally, a complete mechanism for toluene catalytic ozonation, catalyst deactivation, and regeneration was proposed.
KW - CO selectivity
KW - Catalyst deactivation
KW - Catalyst regeneration
KW - Free hydroxyl radical
KW - Reactive oxygen species
UR - https://www.scopus.com/pages/publications/85147201099
U2 - 10.1016/j.jhazmat.2023.130900
DO - 10.1016/j.jhazmat.2023.130900
M3 - 文章
C2 - 36731324
AN - SCOPUS:85147201099
SN - 0304-3894
VL - 448
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 130900
ER -