Enhanced Permanganate Activation under UVA-LED Irradiation: Unraveled Mechanism Involving Manganese Species and Hydroxyl Radical

被引:25
作者
Yang, Tao [1 ]
Mai, Jiamin [1 ]
Zhu, Mengyang [1 ]
Peng, Qiqi [1 ]
Huang, Cui [1 ]
Wu, Sisi [1 ]
Tan, Qinying [1 ]
Jia, Jianbo [1 ]
Fang, Jingyun [2 ]
Ma, Jun [3 ]
机构
[1] Wuyi Univ, Sch Biotechnol & Hlth Sci, Jiangmen 529020, Guangdong, Peoples R China
[2] Sun Yat Sen Univ, Sch Environm Sci & Engn, Guangdong Prov Key Lab Environm Pollut Control & R, Guangzhou 510275, Peoples R China
[3] Harbin Inst Technol, Sch Environm, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
基金
中国国家自然科学基金;
关键词
UVA-LED; Mn(VII); micropollutant; degradation mechanism; LIGHT-EMITTING-DIODES; PHOTOCATALYTIC DEGRADATION; ORGANIC CONTAMINANTS; REACTION-KINETICS; HUMIC-ACID; OXIDATION; WATER; ION; TRANSFORMATION; DISINFECTION;
D O I
10.1021/acs.est.2c06290
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Permanganate [Mn(VII)] has gained broad attention in water treatment. However, its limited reactivity toward some refractory micropollutants hinders its application for micropollutant degradation. Herein, we introduced UVA-LED photolysis of Mn(VII) (UVA-LED/Mn(VII)) to degrade micropollutants (diclofenac (DCF), 4-chlorophenol (4 -CP), atrazine, and nitrobenzene) by selecting DCF and 4-CP as target micropollutants. The effects of operating conditions (e.g., light intensity, radiation wavelengths, pH, and water constituents) on DCF and 4-CP degradation as well as the underlying mechanisms were systematically studied. The degradation rates of DCF and 4-CP linearly decreased with increasing radiation wavelengths (from 365 to 405 nm), likely due to the decreased molar absorption coefficients and quantum yields of Mn(VII). Reactive manganese species (RMnS), including Mn(V), Mn(III), and HO center dot, were generated in the UVA-LED/Mn(VII) process. Mn(V) and HO center dot were responsible for DCF degradation, while Mn(III), HO center dot, and likely Mn(V) accounted for 4-CP degradation. Competitive kinetic results revealed that contributions of RMnS and HO center dot decreased with increasing radiation wavelengths, wherein RMnS played the dominant role. Increasing pH displayed opposite effects on DCF and 4-CP degradation with higher degradation efficiency obtained at acidic pH for the former one but alkaline pH for the latter one. The presence of water background ions (e.g., Cl-, HCO3 -, and Ca2+) barely influenced DCF and 4-CP degradation. Finally, in comparison with Mn(VII) alone, enhanced degradation of DCF and 4-CP by UVA-LED/Mn(VII) was observed in real waters. This work advances the understanding of the photochemistry of manganese species in micropollutant degradation and facilitates Mn(VII) oxidation in practical application.
引用
收藏
页码:17720 / 17731
页数:12
相关论文
共 59 条
[1]   Degradation of diclofenac by pyrite catalyzed Fenton oxidation [J].
Bae, Sungjun ;
Kim, Dongwook ;
Lee, Woojin .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 134 :93-102
[2]   STRUCTURE AND REACTIVITY OF THE OXYANIONS OF TRANSITION METALS .8. ACIDITIES AND SPECTRA OF PROTONATED OXYANIONS [J].
BAILEY, N ;
CARRINGTON, A ;
LOTT, KAK ;
SYMONS, MCR .
JOURNAL OF THE CHEMICAL SOCIETY, 1960, (JAN) :290-297
[3]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[4]   Synthesis and characterization of high photocatalytic activity and stable Ag3PO4/TiO2 fibers for photocatalytic degradation of black liquor [J].
Cai, Li ;
Long, Qiyi ;
Yin, Chao .
APPLIED SURFACE SCIENCE, 2014, 319 :60-67
[5]   Oxidation of PCE with a UV LED photocatalytic reactor [J].
Chen, DH ;
Ye, XJ ;
Li, KY .
CHEMICAL ENGINEERING & TECHNOLOGY, 2005, 28 (01) :95-97
[6]   Unraveling the Role of Mn(VI) and Mn(V) Species in Contaminant Abatement by Permanganate [J].
Chen, Jie ;
Sun, Bo ;
Zhu, Yating ;
Yang, Youqiang ;
Guan, Xiaohong .
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS, 2022, 9 (05) :446-451
[7]   The role of active manganese species and free radicals in permanganate/bisulfite process [J].
Chen, Jie ;
Rao, Dandan ;
Dong, Hongyu ;
Sun, Bo ;
Shao, Binbin ;
Cao, Guomin ;
Guan, Xiaohong .
JOURNAL OF HAZARDOUS MATERIALS, 2020, 388
[8]   Selective interfacial oxidation of organic pollutants in Fenton-like system mediated by Fe(III)-adsorbed carbon nanotubes [J].
Chen, Lei ;
Wang, Shu ;
Yang, Zhichao ;
Qian, Jieshu ;
Pan, Bingcai .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 292 (292)
[9]   Accurate identification of radicals by in-situ electron paramagnetic resonance in ultraviolet-based homogenous advanced oxidation processes [J].
Chen, Long ;
Duan, Jun ;
Du, Penghui ;
Sun, Weiliang ;
Lai, Bo ;
Liu, Wen .
WATER RESEARCH, 2022, 221
[10]   Permanganate oxidation of diclofenac: The pH-dependent reaction kinetics and a ring-opening mechanism [J].
Cheng, Hanyang ;
Song, Dean ;
Liu, Huijuan ;
Qu, Jiuhui .
CHEMOSPHERE, 2015, 136 :297-304