TY - JOUR
T1 - Oxygen vacancies in Z-scheme r-MIL-88A/OV-BiOBr heterojunctions enhance photo-Fenton degradation of chloroquine phosphate
T2 - Mechanisms insight, DFT calculations, degradation pathways and toxicity assessment
AU - Heng, Shiliang
AU - Lu, Xueqin
AU - Song, Yenan
AU - Liu, Zhaobin
AU - Hu, Lingtian
AU - Liu, Yisheng
AU - Liu, Jing
AU - Cai, Teng
AU - Zhen, Guangyin
N1 - Publisher Copyright:
© 2024
PY - 2024/8/10
Y1 - 2024/8/10
N2 - A low cycle of Fe2+/Fe3+, additional H2O2 use, and low mineralization efficiency have limited the wide application of Fe-MOFs. Herein, a novel Z-scheme r-MIL-88A/OV-BiOBr composites (OV-BM) with oxygen vacancies (OV) were fabricated by polyvinylpyrrolidone/ethylene glycol solvothermal method. The optimal OV-BM-25 showed the highest degradation efficiency of 97.8 % for chloroquine phosphate (CQ) by initiating H2O2 under LED visible light irradiation within 60 min. The presence of oxygen vacancies enhanced the electron/hole separation in OV-BM composites and the electron transfer from OV-BiOBr to r-MIL-88A, driving Fe2+/Fe3+ cycling and in-situ H2O2 generation. Quenching experiments and EPR analysis demonstrated that O2–, 1O2, and e– were the main active species, inducing deamination, decarbonization, and cleavage of ring structures in CQ. The possible decomposition pathways of CQ and the ecotoxicity of intermediates were evaluated through UPLC-MS and QSAR analysis. This study provides a theoretical basis for developing Fe-MOFs-based heterojunctions photocatalysts in a Z-scheme photo-Fenton system to treat CQ-bearing organic wastewater.
AB - A low cycle of Fe2+/Fe3+, additional H2O2 use, and low mineralization efficiency have limited the wide application of Fe-MOFs. Herein, a novel Z-scheme r-MIL-88A/OV-BiOBr composites (OV-BM) with oxygen vacancies (OV) were fabricated by polyvinylpyrrolidone/ethylene glycol solvothermal method. The optimal OV-BM-25 showed the highest degradation efficiency of 97.8 % for chloroquine phosphate (CQ) by initiating H2O2 under LED visible light irradiation within 60 min. The presence of oxygen vacancies enhanced the electron/hole separation in OV-BM composites and the electron transfer from OV-BiOBr to r-MIL-88A, driving Fe2+/Fe3+ cycling and in-situ H2O2 generation. Quenching experiments and EPR analysis demonstrated that O2–, 1O2, and e– were the main active species, inducing deamination, decarbonization, and cleavage of ring structures in CQ. The possible decomposition pathways of CQ and the ecotoxicity of intermediates were evaluated through UPLC-MS and QSAR analysis. This study provides a theoretical basis for developing Fe-MOFs-based heterojunctions photocatalysts in a Z-scheme photo-Fenton system to treat CQ-bearing organic wastewater.
KW - Chloroquine phosphate
KW - MIL-88A(Fe)
KW - Oxygen vacancies
KW - Photo-Fenton system
KW - Reactive oxidation species
UR - https://www.scopus.com/pages/publications/85184023451
U2 - 10.1016/j.jmst.2023.11.036
DO - 10.1016/j.jmst.2023.11.036
M3 - 文章
AN - SCOPUS:85184023451
SN - 1005-0302
VL - 190
SP - 172
EP - 187
JO - Journal of Materials Science and Technology
JF - Journal of Materials Science and Technology
ER -