Enhanced degradation of tetracycline hydrochloride by cobalt-manganese sulfide activated peroxymonosulfate
XIE Jin-ling1, PU Jia-xing1, LI Si-yu1, HUANG Li1, GONG Xiao-bo1,2
1. College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610066, China; 2. Key Laboratory of Special Waste Water Treatment, Sichuan Province Higher Education System, Chengdu 610066, China
Abstract：Manganese and cobalt bimetallic sulfide (MnCo2S4) was prepared by a simple two-step method. The morphology, crystal structure and composition of MnCo2S4 were analyzed by scanning electron microscope, X-ray diffraction and X-ray photoelectron spectroscopy, respectively. Degradation efficiency and pathways of tetracycline hydrochloride in MnCo2S4/PMS system were explored. The degradation efficiency of TC reached 88% in 30min when concentrations of MnCo2S4 and PMS were both 0.1g/L. The degradation efficiency of TC remained high in wide pH value range (3~9), which was attributed to the continuous supply of metal active sites of Mn2+ and Co2+ in MnCo2S4 and the synergistic effect of cobalt and manganese. Quenching experiment and electron paramagnetic resonance (EPR) technology provided that SO4•-, •OH and 1O2 were the main active species in MnCo2S4/PMS system. This research gives a new strategy for bimetallic sulfide catalyst construction to activate PMS and treat refractory pollutants.
张春华,赵晓波,李跃军,等.(BiO)2CO3-Bi-TiO2复合纳米纤维制备及其光催化降解抗生素 [J]. 应用化学, 2021,38(1):99-106. Zhang C, Zhao X, Li Y, et al. Preparation of (Bio)2CO3-Bi-TiO2 composite nanofiber and its photocatalytic degradation of antibiotics [J]. Chinese Journal of Applied Chemistry, 2021,38(1):99-106.
[2]
Duan P J, Liu X N, Liu B H, et al. Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism [J]. Applied Catalysis B: Environmental, 2021,298:120532.
[3]
张凌星,肖鹏飞.活化过硫酸盐氧化处理抗生素废水的研究进展 [J]. 工业水处理, 2021,41(5):29-35. Zhang L, Xiao P. Research progress on treatment of antibiotic wastewater by activated persulfate oxidation [J]. Industrial Water Treatment, 2021,41(5):29-35.
[4]
Ahn Y Y, Choi J, Kim M, et al. Chloride-mediated enhancement in heat-Induced activation of peroxymonosulfate: New reaction pathways for oxidizing radical production [J]. Environmental Science & Technology, 2021,55(8):5382-5392.
[5]
Qi C, Liu X, Ma J, et al. Activation of peroxymonosulfate by base: Implications for the degradation of organic pollutants [J]. Chemosphere, 2016,151:280-288.
[6]
Guan Y, Chen J, Chen L, et al. Comparison of UV/H2O2, UV/PMS, and UV/PDS in destruction of different reactivity compounds and formation of bromate and chlorate [J]. Frontiers in Chemistry, 2020, 8:581198.
[7]
Yang H, Zhou J, Yang E, et al. Magnetic Fe3O4-N-doped carbon sphere composite for tetracycline degradation by enhancing catalytic activity for peroxymonosulfate: A dominant non-radical mechanism [J]. Chemosphere, 2021,263:128011.
[8]
郭枭杰,方志勇,周鑫,等.NC-PC锚定微量Fe活化PMS降解水中2,4-二氯苯氧乙酸 [J]. 中国环境科学, 2021,41(7):3238-3246. Guo X, Fang Z, Zhou X, et al. NC-PC anchors trace Fe to activate PMS to degrade 2,4-dichlorophenoxyacetic acid in water [J]. China Environmental Science, 2021,41(7):3238-3246.
[9]
Cheng C, Shao J, Wei P, et al. Nitrogen and boron Co-doped carbon spheres for carbon dioxide electroreduction [J]. Chem. Nano. Mat., 2021,7(6):635-640.
[10]
Huang J, Zhang H. Mn-based catalysts for sulfate radical-based advanced oxidation processes: A review [J]. Environment International, 2019,133:105141.
[11]
徐睿,杨威,杨哲,等.膨胀石墨负载氧化铜活化过硫酸盐用于降解盐酸四环素 [J]. 环境工程, 2020,38(2):48-54,47. Xu R, Yang W, Yang Z, et al. High-efficient removal of tetracycline hydrochloride based on peroxymonosulfate activated by CuO/ expanded graphite composite [J]. Environmental Engineering, 2020, 38(2):48-54,47.
[12]
Kohantorabi M, Giannakis S, Moussavi G, et al. An innovative, highly stable Ag/ZIF-67@GO nanocomposite with exceptional peroxymonosulfate (PMS) activation efficacy, for the destruction of chemical and microbiological contaminants under visible light [J]. Journal of Hazardous Materials, 2021,413:125308.
[13]
李强,唐海,张昊楠,等.α-Fe2O3砂芯微球制备及紫外辅助下活化PMS降解AO7 [J]. 中国环境科学, 2019,39(9):3832-3839. Li Q, Tang H, Zhang H, et al. Preparation of α-Fe2O3 sand core microspheres for the activation of UV-assisted peroxymonosulfate on the degradation of AO7 [J]. China Environmental Science, 2019,39(9): 3832-3839.
[14]
王莹,魏成耀,黄天寅,等.氮掺杂碳纳米管活化过一硫酸盐降解酸性橙AO7 [J]. 中国环境科学, 2017,37(7):2583-2590. Wang Y, Wei C, Huang T. et al. Activation of peroxymonosulfate by nitrogen-doped carbon nanotubes to decolorize acid orange 7 [J]. China Environmental Science, 2017,37(7):2583-2590.
[15]
Lu Y, Zhang W, Yang F, et al. Tailored oxygen defect coupling composition engineering Co Mn2O4 spinel hollow nanofiber enables improved Bisphenol A catalytic degradation [J]. Separation and Purification Technology, 2022,282:120051.
[16]
Nie W, Mao Q, Ding Y, et al. Highly efficient catalysis of chalcopyrite with surface bonded ferrous species for activation of peroxymonosulfate toward degradation of bisphenol A: A mechanism study [J]. Journal of Hazardous Materials, 2019,364:59-68.
[17]
Xu H, Wang D, Ma J, et al. A superior active and stable spinel sulfide for catalytic peroxymonosulfate oxidation of bisphenol S [J]. Applied Catalysis B: Environmental, 2018,238:557-567.
[18]
Li C, Zhao T, Feng X, et al. Construction of hierarchical honeycomb-like MnCo2S4 nanosheets as integrated cathodes for hybrid supercapacitors [J]. Journal of Alloys and Compounds, 2021,859: 157815.
[19]
Zhang F, Cho M, Eom T, et al. Facile synthesis of manganese cobalt sulfide nanoparticles as high-performance supercapacitor electrode [J]. Ceramics International, 2019,45(16):20972-20976.
[20]
Elshahawy A M, Li X, Zhang H, et al. Controllable MnCo2S4 nanostructures for high performance hybrid supercapacitors [J]. Journal of Materials Chemistry A, 2017,5(16):7494-7506.
[21]
Song Y, Sun D, Jiang X, et al. Enhanced activation of peroxymonosulfate by bimetallic spinel sulfides CoNi2S4 for organic dye degradation [J]. Journal of Environmental Chemical Engineering, 2021,9(6):106889.
[22]
蒋海燕,段 毅,刘宇琪,等.煅烧高岭土活化过一硫酸盐去除废水中的四环素 [J]. 环境工程学报, 2020,14(9):2494-2505. Jang H, Duan Y, Liu Y, et al. Removal of tetracycline from wastewater by activating persulfate with calcined kaolin [J]. Chinese Journal of Environmental Engineering, 2020,14(9):2494-2505.
[23]
Xie J, Chen L, Luo X, et al. Degradation of tetracycline hydrochloride through efficient peroxymonosulfate activation by B, N co-doped porous carbon materials derived from metal-organic frameworks: Nonradical pathway mechanism [J]. Separation and Purification Technology, 2022,281:119887.
[24]
杨珂,唐琪,杨晓丹,等.铁酸铜非均相活化过硫酸盐降解罗丹明B [J]. 中国环境科学, 2019,39(9):3761-3769. Yang K, Tang Q, Yang X, et al. Degradation of rhodamine B by heterogeneous activation of persulfate with copper ferrate [J]. China Environmental Science, 2019,39(9):3761-3769.
[25]
Fan J, Zhao Z, Ding Z, et al. Synthesis of different crystallographic FeOOH catalysts for peroxymonosulfate activation towards organic matter degradation [J]. RSC Advances, 2018,8(13):7269-7279.
[26]
Guo Y, Yan L, Li X, et al. Goethite/biochar-activated peroxymonosulfate enhances tetracycline degradation: Inherent roles of radical and non-radical processes [J]. Science of the Total Environment, 2021,783: 147102.
[27]
Gao Y, Zhao Q, Li Y, et al. Degradation of sulfamethoxazole by peroxymonosulfate activated by waste eggshell supported Ag2O-Ag nano-particles [J]. Chemical Engineering Journal, 2021,405:126719.
[28]
Ge L, Dong Q, Halsall C, et al. Aqueous multivariate phototransformation kinetics of dissociated tetracycline: Implications for the photochemical fate in surface waters [J]. Environmental Science and Pollution Research, 2018,25(16):15726-15732.
[29]
葛勇建,蔡显威,林 翰,等.碱活化过一硫酸盐降解水中环丙沙星 [J]. 环境科学, 2017,38(12):5116-5123. Ge Y, Cai X, Lin H, et al. Base activation of peroxymonosulfate for the degradation of ciprofloxacin in water [J]. Environmental Science, 2017,38(12):5116-5123.
[30]
Ma W, Wang N, Du Y, et al. Human-hair-derived N, S-doped porous carbon: An enrichment and degradation system for wastewater remediation in the presence of peroxymonosulfate [J]. ACS Sustainable Chemistry & Engineering, 2018,7:2718-2727.
[31]
Fu H, Zhao P, Xu S, et al. Fabrication of Fe3O4 and graphitized porous biochar composites for activating peroxymonosulfate to degrade p-hydroxybenzoic acid: Insights on the mechanism [J]. Chemical Engineering Journal, 2019,375:121980.
[32]
Xie J, Luo X, Chen L, et al. ZIF-8derived boron, nitrogen co-doped porous carbon as metal-free peroxymonosulfate activator for tetracycline hydrochloride degradation: Performance, mechanism and biotoxicity [J]. Chemical Engineering Journal, 2022,440:135760.
