Magnetic covalent triazine-based frameworks (MCTF) were prepared by microwave-assisted synthesis. The morphology and surface groups of MCTF were characterized and analyzed by SEM, TEM and FTIR. The microscopic mesoporous structure and saturation magnetization were measured, which was used to the degradation of sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). The main significant factors of degradation of SMX in MCTF/PMS system were studied, including dosage of MCTF, PMS concentration, pH, inorganic ions. The results showed that the 100% degradation occurred for 0.05mmol/L SMX after 30min treatment by 0.3g/L MCTF and 1.50mmol/L PMS. The degradation rate of SMX decreased with the increase of pH. SO42- and HCO3- had inhibitory effects on SMX degradation, while Cl- had dual effects on SMX degradation. Cyclic test proved that MCTF had good recycling performance. In the reaction process, the active substances degrading SMX were mainly generated reaction on the catalyst surface by sulfate radical (SO4-·) and hydroxyl radical (·OH). The pathways and potential products of SMX was analyzed by UHPLC-MS/MS.
Xu M J, LI J, Yan Y, et al. Catalytic degradation of sulfamethoxazole through peroxymonosulfate activated with expanded graphite loaded CoFe2O4 particles[J]. Chemical Engineering Journal, 2019,369(1):403-413.
[2]
Cui C Z, Jin L, Jiang L, et al. Removal of trace level amounts of twelve sulfonamides from drinking water by UV-activated peroxymonosulfate[J]. Science of the Total Environment, 2016,572(1):244-251.
[3]
Rodríguez J, García C, Lepistö R, et al. Intensification of UV-C tertiary treatment:disinfection and removal of micropollutants by sulfate radical based advanced oxidation processes[J]. Journal of Hazardous Materials, 2018,372(15):94-102.
[4]
Ma J, Ding Y, Chi L P, et al. Degradation of benzotriazole by sulfate radical-based advanced oxidation process[J]. Environmental Technology, 2019.DOI:10.1080/09593330.2019.1625959.
[5]
Zhao D Y, Wang H L, Qi H P, et al. Facile synthesis of mesoporous Co3O4 with excellent performance for activation of PMS[J]. Materials Research Express, 2019,6(7):1-13.
[6]
Sun H Q, Liu S Z, Zhou G L, et al. Reduced Graphene oxide for catalytic oxidation of aqueous organic pollutants[J]. ACS Applied Materials & Interfaces, 2012,4(10):5466-5471.
[7]
于小龙.氮掺杂碳纳米孔材料催化过硫酸盐氧化直接红23染料废水[D]. 长春:吉林大学, 2017. Yu X L. Nitrogen-doped carbon material a catalyst for Direct Red23 oxidation in persulfate-containing aqueous solutions[D]. Changchun:Jilin university, 2017.
[8]
Li N, Du J J, Di W, et al. Recent advances in facile synthesis and applications of covalent organic framework materials as superior adsorbents in sample pretreatment[J]. Trends in Analytical Chemistry, 2018,108:154-166.
[9]
Guo B X, Wu C G, Su Q, et al. A Zn-salen based covalent triazine framework as a promising candidate for CO2 capture[J]. Materials Letters, 2018,221(15):236-239.
[10]
Li J, Zhang L H, Liu X T, et al. Pd nanoparticles supported on covalent triazine-based framework material:An efficient and high chemosel-ective catalyst for the reduction of nitroarenes[J]. New Journal of Chemistry, 2018,42(12):9684-9689
[11]
Wan S, Guo J, Kim J et a1. A belt-shaped, blue Luminescent, and semiconducting covalent organic framework[J]. Angewandte Chemie, 2009,121(18):3234-3253.
[12]
Kuhn P, Antonietti M, Thomas A, et a1. Porous, covalent triazine-based frameworks prepared by ionothermal synthesis[J]. Angewandte Chemie, 2008,47(18):3450-3453.
[13]
Xiong Y H, Su L J, He X C, et al. Colorimetric determination of copper ions based on regulation of the enzyme-mimicking activity of covalent triazine frameworks[J]. Sensors and Actuators B:Chemical, 2017,253:384-391.
[14]
Zheng X F, Ruan Q Q, Jiang Q, et al. Integrated adsorption and catalytic degradation of safranine T by a porous covalent triazine-based framework[J]. Journal of Colloid and Interface Science, 2018, 532(15):1-11.
[15]
Wang R H, Zhong H, Hong Z X, et al. A covalent triazine-based framework consisting of donor-acceptor dyads for visible-light-driven photocatalytic CO2reduction[J]. Chem Sus Chem, 2019,12(19):4493-4499.
[16]
Chen L, He Y T, Lei Z X, et al. Preparation of core-shell structured magnetic covalent organic framework nanocomposites for magnetic solid-phase extraction of bisphenols from human serum sample[J]. Talanta, 2018,181(1):296-304.
[17]
王忠明,陈家斌,张黎明,等.活性炭负载Co3O4活化过一硫酸盐降解金橙G[J]. 环境科学, 2016,37(7):2591-2600. Wang Z M, Cheng J B, Zhang L M, et al. Activated carbon supported Co3O4 catalysts to activate peroxymonosulfate for orange G degradation[J]. Environmental Science, 2016,37(7):2591-2600.
[18]
Sui N, Duan Y Z, Jiao X L, et al. Large-scale preparation and catalytic properties of one-dimensional α/β-MnO2 nanostructures[J]. The Journal of Physical Chemistry C, 2009,113(20):8560-8565.
[19]
Xu L, Xu C, Zhao M R, et al. Oxidative removal of aqueous steroid estrogens by manganese oxides[J]. Water Research, 2008,42(20):5038-5044.
[20]
Deng J, Feng S F, Ma X Y, et al. Heterogeneous degradation of orange II with peroxymonosulfate activated by ordered mesoporous MnFe2O4[J]. Separation & Purification Technology, 2016,167(14):181-189.
[21]
田凯勋,杨超,肖泉,等.超声强化零价铁/过硫酸钾体系降解2,4,6-三氯苯酚废水[J]. 中国环境科学, 2017,37(10):3729-3734. Tian K X, Yang C, Xiao Q, et al. Degradation of 2,4,6-TCP in an ultrasound-enhanced zero-valent iron/potassium persuifate system[J]. China Environmental Science, 2017,37(10):3729-3734.
[22]
Yan Z J, He M, Chen B B, et al. Magnetic covalent triazine framework for rapid extraction of phthalate esters in plastic packaging materials followed by gas chromatography-flame ionization detection[J]. Journal of Chromatography A, 2017,1525(24):32-41.
[23]
Feng Y, Liu J H, Wu D L, et al. Efficient degradation of sulfamethazine with CuCo2O4 spinel nanocatalysts for peroxymonosulfate activation[J]. Chemical Engineering Journal, 2015,280(15):514-524.
[24]
Fan Y, Ji Y F, Zheng G Y, et al. Degradation of atrazine in heterogeneous Co3O4 activated peroxymonosulfate oxidation process:Kinetics, mechanisms, and reaction pathways[J]. Chemical Engineering Journal, 2017,330(15):831-839.
[25]
张黎明,陈家斌,房聪,等. Cl-对碳纳米管/过一硫酸盐体系降解金橙G的影响[J]. 中国环境科学, 2016,36(12):3591-3600. Zhang L M, Cheng J B, Fang C, et al. Effect of chloride ions on degradation of orange G with peroxymonosulfate activated by carbon nanotubes[J]. China Environmental Science, 2016,36(12):3591-3600.
[26]
Ao X W, Liu W J. Degradation of sulfamethoxazole by medium pressure UV and oxidants:Peroxymonosulfate, persulfate, and hydrogen peroxide[J]. Chemical Engineering Journal, 2017,313(1):629-637.
[27]
Zhang X L, Feng M B, Qu R J, et al. Catalytic degradation of diethyl phthalate in aqueous solution by persulfate activated with nano-scaled magnetic CuFe2O4/MWCNTs[J]. Chemical Engineering Journal, 2016, (1),301:1-11.
[28]
Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants[J]. Environmental Science & Technology, 2004,38(13):3705-3712.
[29]
夏文君,刘锋,郝尚斌,等.石墨烯负载铁锰氧化物活化过一硫酸盐降解金橙G[J]. 环境科学, 2018,39(5):2202-2210. Xia W J, Liu F, Hao S B, et al. Degradation of OG with peroxymonosulfate activated by a MnFe2O4-graphene hybrid[J]. Environmental Science, 2018,39(5):2202-2210.
[30]
Yang S Y, Yang X, Shao X T, et al. Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7at ambient temperature[J]. Journal of Hazardous Materials, 2011,186(1):659-666.
[31]
卢建,黄天寅,徐劼,等.抗坏血酸对三价铁/过氧化钙体系降解头孢氨苄的影响[J]. 环境工程学报, 2018,12(10):2758-2767. Lu J, Huang T Y, Xu J, et al. Effect of ascorbic acid on the cefalexin degradation in Fe3+/calcium peroxide system[J]. Chinese Journal of Environmental Engineering, 2018,12(10):2758-2767.
[32]
桑稳姣,李志轩,黄明杰.羟胺强化过渡金属活化过硫酸盐降解磺胺甲恶唑[J]. 环境科学学报, 2019,39(6):1772-1780. Sang W J, Li Z X, Huang M J, et al. Enhanced transition metal oxide based persulfate activation by hydroxylamine for the degradation of sulfamethoxazole[J]. Acta Scientiae Circumstantiae, 2019,39(6):1772-1780.
[33]
李翔,王安杰,柳广厦,等.芳香杂环含硫化合物C-S键断裂方式[J]. 石油学报(石油加工), 2017,33(6):1039-1052. Li X, Wang A J, Liu G X, et al. Mechanisms of the cleavage of C-S bonds in polyaromatic sulfur-containing compounds[J]. Acta Petrolei Sinica (Petroleum Processing Section), 2017,33(6):1039-1052.
[34]
Wang H Z, Guo W Q, Yin R L, et al. Biochar-induced Fe(III) reduction for persulfate activation in sulfamethoxazole degradation:Insight into the electron transfer, radical oxidation and degradation pathways[J]. Chemical Engineering Journal, 2019,362(15):561-569.