TY - JOUR
T1 - Biotemplate Fabrication of Hollow Tubular Ce xSr1- xTiO3with Regulable Surface Acidity and Oxygen Mobility for Efficient Destruction of Chlorobenzene
T2 - Intrinsic Synergy Effect and Reaction Mechanism
AU - Sun, Yukun
AU - Xu, Shuai
AU - Bai, Bo
AU - Li, Lu
AU - Kang, Yu
AU - Hu, Xingquan
AU - Liao, Zehuihuang
AU - He, Chi
N1 - Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/5/3
Y1 - 2022/5/3
N2 - Developing economic and applicable catalysts with elegant chlorine resistance and organic byproduct inhibition capability is of great significance for chlorinated volatile organic compounds (Cl-VOCs) eco-friendly purification. Here, ternary CexSr1-xTiO3catalysts with tunable surface acidity and oxygen species mobility were creatively fabricated using the hollow tubular-structured fruit hair of Platanus (FHP; a widespread greenery waste) as the scaffolding biotemplate. It is shown that the oxygen vacancy (Ov) triggered by the presence of Ce can optimize the synergy between the Lewis acid sites (LAS) and Brønsted acid sites (BAS). High concentration of Ovand BAS promotes the C-Cl cleavage of chlorobenzene (CB) and accelerates the desorption of Cl•radicals as inorganic chlorine. Simultaneously, the strong electron transfer within Ti-Ce-Sr linkage increases the acidity of LAS, resulting in the superior reducibility of Ce0.4Sr0.6TiO3and facilitating the deep oxidation of dechlorination intermediates. Additionally, the spatial confinement of the tubular structure remarkably accelerates the CB flow rate and reduces the residence time of byproducts over the prepared catalysts. Owing to these, CB can be efficiently destructed over Ce0.4Sr0.6TiO3with selectivity of CO2and inorganic chlorine dramatically enhanced, respectively, approximately 16 and 21 times at 275 °C compared to those of pure SrTiO3. The present work provides a feasible and promising strategy for engineering efficient catalysts for heterogeneous thermocatalytic reactions for industrial-scale Cl-CVOC destruction.
AB - Developing economic and applicable catalysts with elegant chlorine resistance and organic byproduct inhibition capability is of great significance for chlorinated volatile organic compounds (Cl-VOCs) eco-friendly purification. Here, ternary CexSr1-xTiO3catalysts with tunable surface acidity and oxygen species mobility were creatively fabricated using the hollow tubular-structured fruit hair of Platanus (FHP; a widespread greenery waste) as the scaffolding biotemplate. It is shown that the oxygen vacancy (Ov) triggered by the presence of Ce can optimize the synergy between the Lewis acid sites (LAS) and Brønsted acid sites (BAS). High concentration of Ovand BAS promotes the C-Cl cleavage of chlorobenzene (CB) and accelerates the desorption of Cl•radicals as inorganic chlorine. Simultaneously, the strong electron transfer within Ti-Ce-Sr linkage increases the acidity of LAS, resulting in the superior reducibility of Ce0.4Sr0.6TiO3and facilitating the deep oxidation of dechlorination intermediates. Additionally, the spatial confinement of the tubular structure remarkably accelerates the CB flow rate and reduces the residence time of byproducts over the prepared catalysts. Owing to these, CB can be efficiently destructed over Ce0.4Sr0.6TiO3with selectivity of CO2and inorganic chlorine dramatically enhanced, respectively, approximately 16 and 21 times at 275 °C compared to those of pure SrTiO3. The present work provides a feasible and promising strategy for engineering efficient catalysts for heterogeneous thermocatalytic reactions for industrial-scale Cl-CVOC destruction.
KW - biotemplate
KW - byproduct inhibition
KW - catalytic destruction
KW - chlorobenzene
KW - hollow tubular Ce SrTiO
KW - synergy mechanism
UR - https://www.scopus.com/pages/publications/85127587441
U2 - 10.1021/acs.est.2c00270
DO - 10.1021/acs.est.2c00270
M3 - 文章
C2 - 35321543
AN - SCOPUS:85127587441
SN - 0013-936X
VL - 56
SP - 5796
EP - 5807
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 9
ER -