Enhanced photocatalytic degradation of sulfamethoxazole using MIL-101 (Fe) supported Mo single-atom with oxygen vacancies under visible light activation of peroxymonosulfate

被引:4
作者
Kong, Weitao [1 ]
Liu, Zhongmou [1 ]
Wu, Jinghui [1 ,2 ,3 ]
Wen, Chenying [1 ]
Yan, Juncheng [1 ]
Gao, Yidi [2 ]
Li, Guanqiao [2 ]
Wang, Xianze [1 ,2 ]
Huo, Mingxin [2 ]
机构
[1] Jilin Jianzhu Univ, Key Lab Songliao Aquat Environm, Minist Educ, Changchun 130118, Peoples R China
[2] Northeast Normal Univ, Sci & Technol Innovat Ctr Municipal Wastewater Tre, Changchun 130117, Peoples R China
[3] Northeast Normal Univ, Engn Res Ctr Low Carbon Treatment & Green Dev Poll, Sch Environm, Minist Educ, Changchun 130117, Peoples R China
基金
中国国家自然科学基金;
关键词
Photocatalysis; Mo single-atom; Oxygen vacancies; Peroxymonosulfate; Singlet oxygen; Metal-organic frameworks; SULFONAMIDE ANTIBIOTICS; OXIDATION; TETRACYCLINE;
D O I
10.1016/j.psep.2025.106778
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study investigates the degradation of sulfamethoxazole (SMX), a widely detected and persistent antibiotic in the environment, using a novel photocatalytic system based on MIL-101(Fe) supported Mo single-atom with oxygen vacancies (Mo/Ov-MOF). Anchoring Mo single-atoms into the MOF structure enhances catalytic activity by effectively improving charge separation and reducing electron-hole recombination. The Mo/Ov-MOF efficiently activates peroxymonosulfate (PMS) under visible light, generating singlet oxygen (1O2) as a primary reactive species responsible for SMX degradation. Degradation experiments demonstrated that the degradation efficiency reached 96.8 % in the presence of PMS and visible light. Through quenching and trapping experiments on active species, an in-depth investigation into the source of 1O2 was performed, demonstrating the crucial role of holes in the rapid and selective generation of 1O2 under visible light. Additionally, the reusability of the Mo/ Ov-MOF catalyst was confirmed, maintaining over 70 % degradation efficiency after five cycles. Toxicity assessments indicated that the degradation by-products exhibited significantly lower toxicity than the parent compound SMX, thus mitigating potential ecological risks. The mechanistic insights reveal that oxygen vacancies and Mo single-atom enhance electron transport and facilitate efficient PMS activation, ultimately leading to effective pollutant degradation. The findings underscore the potential of the Mo/Ov-MOF photocatalytic system for practical applications in wastewater treatment, particularly for removing persistent organic pollutants from aquatic environments.
引用
收藏
页数:13
相关论文
共 42 条
[1]   Synergistic Hydrogenation over Palladium through the Assembly of MIL-101(Fe) MOF over Palladium Nanocubes [J].
Bakuru, Vasudeva Rao ;
Kalidindi, Suresh Babu .
CHEMISTRY-A EUROPEAN JOURNAL, 2017, 23 (65) :16456-16459
[2]   Visible light enhanced persulfate activation for degradation of tetracycline via boosting adsorption of persulfate by ligand-deficient MIL-101 (Fe) icosahedron [J].
Cheng, Gangya ;
Yuan, Chen ;
Ruan, Wansheng ;
Ma, Ben ;
Zhang, Xinyu ;
Yuan, Xinjing ;
Li, Zhihui ;
Wang, Dan ;
Teng, Fei .
CHEMOSPHERE, 2023, 317
[3]   Photocatalytic performance and mechanism of AgI/Ag/ZnO composites as catalysts for the visible-light-driven degradation of naproxen [J].
Ding, Chao ;
Fu, Kun ;
Wu, Minhui ;
Gong, Sicheng ;
Liu, Jia ;
Shi, Jun ;
Deng, Huiping .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2021, 414
[4]   Superoxide radicals dominated visible light driven peroxymonosulfate activation using molybdenum selenide (MoSe2) for boosting catalytic degradation of pharmaceuticals and personal care products [J].
Dong, Chencheng ;
Wang, Zhiqiang ;
Ye, Zhichao ;
He, Juhua ;
Zheng, Zexiao ;
Gong, Xueqing ;
Zhang, Jinlong ;
Lo, Irene M. C. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 296
[5]   Occurrence and ecotoxicity of sulfonamides in the aquatic environment: A review [J].
Duan, Weiyan ;
Cui, Hongwu ;
Jia, Xinyu ;
Huang, Xiao .
SCIENCE OF THE TOTAL ENVIRONMENT, 2022, 820
[6]   Synthesis and characterization of Bi2MoO6/MIL-101(Fe) as a novel composite with enhanced photocatalytic performance: Effect of water matrix and reaction mechanism [J].
Hajiali, Mahboube ;
Farhadian, Mehrdad ;
Tangestaninejad, Shahram ;
Khosravi, Mohsen .
ADVANCED POWDER TECHNOLOGY, 2022, 33 (05)
[7]   Enhanced photocatalysis degradation of organophosphorus flame retardant using MIL-101(Fe)/persulfate: Effect of irradiation wavelength and real water matrixes [J].
Hu, Han ;
Zhang, Haixuan ;
Chen, Ya ;
Chen, Yujia ;
Zhuang, Li ;
Ou, Huase .
CHEMICAL ENGINEERING JOURNAL, 2019, 368 :273-284
[8]   Occurrence and removal of sulfonamide antibiotics and antibiotic resistance genes in conventional and advanced drinking water treatment processes [J].
Hu, Yaru ;
Jiang, Lei ;
Zhang, Tianyang ;
Jin, Lei ;
Han, Qi ;
Zhang, Dong ;
Lin, Kuangfei ;
Cui, Changzheng .
JOURNAL OF HAZARDOUS MATERIALS, 2018, 360 :364-372
[9]   Defects on CoS2-x: Tuning Redox Reactions for Sustainable Degradation of Organic Pollutants [J].
Ji, Jiahui ;
Yan, Qingyun ;
Yin, Pengcheng ;
Mine, Shinya ;
Matsuoka, Masaya ;
Xing, Mingyang .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (06) :2903-2908
[10]   Efficient wastewater disinfection by raised 1O2 yield through enhanced electron transfer and intersystem crossing via photocatalysis of peroxymonosulfate with CuS quantum dots modified MIL-101(Fe) [J].
Jiang, Yanni ;
Gao, Binyang ;
Wang, Zhongjuan ;
Li, Jie ;
Du, Ye ;
He, Chuanshu ;
Liu, Yang ;
Yao, Gang ;
Lai, Bo .
WATER RESEARCH, 2023, 229