TY - JOUR
T1 - Mechanism insight into oxygen vacancy-dependent effect in Fe1/TiO2 single-atom catalyst for highly enhanced photo-Fenton mineralization of phenol
AU - Yang, Man
AU - Li, Haibo
AU - Liu, Fenli
AU - Sun, Shaodong
AU - Mei, Jing
AU - Jiao, Yuxiang
AU - Cui, Jie
AU - Xu, Yang
AU - Song, Hailiang
AU - Duan, Zongfan
AU - Liu, Wengang
AU - Ren, Yujing
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2024/10/5
Y1 - 2024/10/5
N2 - This study develops a highly efficient Fe1/TiO2-OV single-atom catalyst to explore the synergistic effect in the photo-Fenton mineralization of phenol. Via using diverse in-situ spectroscopies and density functional theory calculations, the catalytic mechanism is unraveled. That is, oxygen vacancies can significantly accelerate photogenerated charge separation and oriented delivery to Fe1 single atoms for fast generation of reactive oxygen species, as well as promote the selective adsorption/activation of phenol. As a result, the C-H bonds on phenol were deeply oxidized (conversion: > 91%), accompanied by the mineralization of the benzene ring, with CO2 and H2O as end products (mineralization rate: 66%). Such concerted catalysis between Fe single atoms and oxygen vacancies results in a high reactivity for phenol photo-Fenton mineralization, which is superior to most reported transition-metal-based catalysts. Our finding is expected to provide guidance for designing high-efficiency heterogeneous catalysts in the photo-Fenton catalytic process.
AB - This study develops a highly efficient Fe1/TiO2-OV single-atom catalyst to explore the synergistic effect in the photo-Fenton mineralization of phenol. Via using diverse in-situ spectroscopies and density functional theory calculations, the catalytic mechanism is unraveled. That is, oxygen vacancies can significantly accelerate photogenerated charge separation and oriented delivery to Fe1 single atoms for fast generation of reactive oxygen species, as well as promote the selective adsorption/activation of phenol. As a result, the C-H bonds on phenol were deeply oxidized (conversion: > 91%), accompanied by the mineralization of the benzene ring, with CO2 and H2O as end products (mineralization rate: 66%). Such concerted catalysis between Fe single atoms and oxygen vacancies results in a high reactivity for phenol photo-Fenton mineralization, which is superior to most reported transition-metal-based catalysts. Our finding is expected to provide guidance for designing high-efficiency heterogeneous catalysts in the photo-Fenton catalytic process.
KW - Oxygen vacancy
KW - Phenol oxidation
KW - Photo-Fenton reaction
KW - Single-atom catalyst
KW - Surface catalytic mechanism
UR - http://www.scopus.com/inward/record.url?scp=85191156646&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2024.124071
DO - 10.1016/j.apcatb.2024.124071
M3 - 文章
AN - SCOPUS:85191156646
SN - 0926-3373
VL - 354
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 124071
ER -