Promoting multiple reactive oxygen species generation for deep oxidation of VOCs by UV/persulfate/permanganate

被引:3
作者
Xie, Ruijie [1 ,2 ]
Suo, Ziyi [1 ]
Guo, Kaiheng [1 ]
Feng, Fada [2 ]
Lan, Bang [2 ]
Zhang, Tao [1 ]
Li, Guangqin [3 ]
Huang, Haibao [1 ]
机构
[1] Sun Yat Sen Univ, Sch Environm Sci & Engn, Guangzhou 510006, Peoples R China
[2] Jiaying Univ, Sch Chem & Environm, Meizhou 514015, Peoples R China
[3] Sun Yat Sen Univ, Sch Chem, Guangzhou 510006, Peoples R China
基金
中国博士后科学基金;
关键词
Advanced oxidation processes; VOCs; Deep oxidation; ROS; Co-oxidant; PEROXYMONOSULFATE; PERMANGANATE; DEGRADATION; REMEDIATION; COMBINATION; PERFORMANCE; ACTIVATION; CATALYSTS; ABATEMENT; REMOVAL;
D O I
10.1016/j.seppur.2023.124770
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Advanced oxidation processes (AOPs) could effectively remove volatile organic compounds (VOCs) when coupled with wet scrubbing process. However, it still faces challenges in achieving deep oxidation of VOCs due to the limited production of reactive oxygen species (ROS). Herein, we present the utilization of permanganate (KMnO4) as a co-oxidant to enhance VOCs oxidation in UV/persulfate (PDS)/KMnO4 system. The removal efficiency of a targeted VOC, toluene, kept high at above 90% throughout the entire long-term reaction of 4 h, which was much higher than that of UV/PDS and UV/KMnO4. Notably, the in-situ formed manganese oxide (MnOx) acts as a catalyst in UV/MnOx and UV/MnOx/PDS, facilitating the generation of various ROS and thereby enhancing VOCs degradation. Electron paramagnetic resonance (EPR) and quenching experiments indicated that sulfate radical (SO4 & BULL;- ), hydroxyl radical (HO & BULL;), superoxide radical (& BULL;O2  ) and singlet oxygen (1O2) were the main ROS generated in the UV/PDS/KMnO4 system. The overall oxidation process can be divided into three stages: the UV/KMnO4-dominated stage, the UV/MnOx/PDS-dominated stage, and the UV/MnOx-dominated stage. Correspondingly, HO & BULL; played a major role in toluene oxidation in the UV/KMnO4-dominated and UV/MnOx-dominated stages, with the contributions of 48% and 52%, respectively. Meanwhile, SO4 & BULL;� played a more significant role in the UV/MnOx/PDS-dominated stage, with a contribution of 59%. Three main reaction pathways involving electron abstraction, HO & BULL; addition and benzene ring opening were proposed based on the intermediates identified by proton-transfer-reaction mass spectrometry (PTR-MS). This study provided a deep understanding of KMnO4 in improving the oxidation capacity of UV-based AOPs for VOCs degradation, emphasizing the importance of in-situ formed MnOx for promoting multiple ROS generation.
引用
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页数:10
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共 43 条
[1]   Chemical oxidation of benzene and trichloroethylene by a combination of peroxymonosulfate and permanganate linked by in-situ generated colloidal/amorphous MnO2 [J].
Cui, Jiaxin ;
Zhang, Lieyu ;
Xi, Beidou ;
Zhang, Jing ;
Mao, Xuhui .
CHEMICAL ENGINEERING JOURNAL, 2017, 313 :815-825
[2]   Theoretical exploration of VOCs removal mechanism by carbon nanotubes through persulfate-based advanced oxidation processes: Adsorption and catalytic oxidation [J].
Dai, Zhenhua ;
Li, Didi ;
Ao, Zhimin ;
Wang, Shaobin ;
An, Taicheng .
JOURNAL OF HAZARDOUS MATERIALS, 2021, 405
[3]   N-Doping-Induced Nonradical Reaction on Single-Walled Carbon Nanotubes for Catalytic Phenol Oxidation [J].
Duan, Xiaoguang ;
Sun, Hongqi ;
Wang, Yuxian ;
Kang, Jian ;
Wang, Shaobin .
ACS CATALYSIS, 2015, 5 (02) :553-559
[4]   Ultrasound-assisted heterogeneous activation of persulfate and peroxymonosulfate by asphaltenes for the degradation of BTEX in water [J].
Fedorov, Kirill ;
Plata-Gryl, Maksymilian ;
Khan, Javed Ali ;
Boczkaj, Grzegorz .
JOURNAL OF HAZARDOUS MATERIALS, 2020, 397
[5]   Synergetic effect of the mineralization of organic contaminants by a combined use of permanganate and peroxymonosulfate [J].
Gao, Shun ;
Cui, Jiaxin ;
Xiong, Ying ;
Xiao, Wei ;
Wang, Dihua ;
Alshawabkeh, Akram N. ;
Mao, Xuhui .
SEPARATION AND PURIFICATION TECHNOLOGY, 2015, 144 :248-255
[6]   A review of the recent advances on the treatment of industrial wastewaters by Sulfate Radical-based Advanced Oxidation Processes (SR-AOPs) [J].
Giannakis, Stefanos ;
Lin, Kun-Yi Andrew ;
Ghanbari, Farshid .
CHEMICAL ENGINEERING JOURNAL, 2021, 406
[7]   Abatement of Structurally Diverse Micropollutants by the UV/Permanganate Process: Roles of Hydroxyl Radicals and Reactive Manganese Species [J].
Guo, Kaiheng ;
Wei, Wenrui ;
Wu, Sining ;
Song, Weihua ;
Fang, Jingyun .
ACS ES&T WATER, 2022, 2 (04) :593-603
[8]   Ultraviolet Irradiation of Permanganate Enhanced the Oxidation of Micropollutants by Producing HO• and Reactive Manganese Species [J].
Guo, Kaiheng ;
Zhang, Jinsong ;
Li, Ailin ;
Xie, Ruijie ;
Liang, Zhuojian ;
Wang, Anna ;
Ling, Li ;
Li, Xuchun ;
Li, Chuanhao ;
Fang, Jingyun .
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS, 2018, 5 (12) :750-756
[9]   Plasma-induced oxygen vacancies in amorphous MnOx boost catalytic performance for electrochemical CO2 reduction [J].
Han, Hyunsu ;
Jin, Song ;
Park, Seongmin ;
Kim, Yoongon ;
Jang, Daehee ;
Seo, Min Ho ;
Kim, Won Bae .
NANO ENERGY, 2021, 79
[10]   ELECTRONIC-SPECTRA, PHOTOCHEMISTRY, AND AUTOXIDATION MECHANISM OF SULFITE-BISULFITE-PYROSULFITE SYSTEMS - SO2-, SO3-, SO4-, AND SO5- RADICALS [J].
HAYON, E ;
TREININ, A ;
WILF, J .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1972, 94 (01) :47-&