Degradation of AO7 with peroxymonosulfate catalyzed by Co-C-N single atom
XU Jie1,2, WANG Ke-qing1, TIAN Dan1, WU Mei1, LI Si-jia1, BAO Xiu-min1, XU Xiao-yi1
1. School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou 215000, China; 2. Sinosteel Tiancheng Environmental Protection Science & Technology Co., Ltd, Wuhan 430080, China
Abstract：Monoatomic Co-C-N catalyst was synthesized by a template etching method and then was used to activate peroxymonosulfate (PMS) for degradation of decolorize azo dye orange 7 (AO7). The effects of catalyst dosage, PMS concentration, pH value of reaction medium and Cl- commonly exists in dye wastewater on the removal of AO7 in Co-C-N/PMS system were systematically evaluated. The reaction mechanism was inferred, the mineralization ability and the reuse of catalyst were investigated. Experimental results showed that Co-C-N can effectively activate PMS to degrade AO7, and the reaction rate for AO7 removal can be accelerated with an increase in Co-C-N dosage and PMS concentration. AO7 can be removed effectively in the range of pH=3.0 to 9.0. When the concentration of Co-C-N dosage、the PMS and AO7 concentration were 50mg/L、1.0mmol/L and 0.05mmol/L respectively, AO7 can be completely removed within 10min under a neutral condition. SO4·- produced by PMS activation of heterogeneous system was the main active species for the degradation of AO7, and 1O2 produced by C-induced PMS was also involved in the degradation reaction through non-free radical system. The oxidation reaction mainly occurs on the surface of the catalyst. Co-C-N/PMS system has excellent removal ability and strong mineralization effect for AO7. Compared with the single Co-C-N adsorption process of AO7, Co-C-N/PMS system not only can increases the reaction rate, but also greatly improves the recyclability of the catalyst.
徐劼, 王柯晴, 田丹, 吴梅, 李思佳, 鲍秀敏, 许晓毅. 单原子Co-C-N催化过一硫酸盐降解金橙Ⅱ[J]. 中国环境科学, 2021, 41(1): 151-160.
XU Jie, WANG Ke-qing, TIAN Dan, WU Mei, LI Si-jia, BAO Xiu-min, XU Xiao-yi. Degradation of AO7 with peroxymonosulfate catalyzed by Co-C-N single atom. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(1): 151-160.
Meriç S, Kaptan D, Tünay O. Removal of color and cod from a mixture of four reactive azo dyes using fenton oxidation process[J]. Environmental Letters, 2003,38(10):2241-2250.
[2]
Robinson T, Mcmullan G, Marchant R, et al. Remediation of dyes in textile effluent:A critical review on current treatment technologies with a proposed alternative[J]. Bioresource Technology, 2001,77(3):247-255.
[3]
Forgacs E, Cserháti T, Oros G. Removal of synthetic dyes from wastewaters:a review[J]. Environment International, 2004,30(7):953971.
[4]
Yang Q, Choi H, Chen Y, et al. Heterogeneous activation of peroxymonosulfate by supported cobalt catalysts for the degradation of 2,4-dichlorophenol in water:The effect of support, cobalt precursor, and UV radiation[J]. Applied Catalysis B Environmental, 2008, 77(3):300-307.
[5]
周骏,肖九花,方长玲,等.UV/PMS体系硝基氯酚降解动力学及机理研究[J]. 中国环境科学, 2016,36(1):68-75. Zhou J, Xiao J H, Fang C L, et al. Degradation kinetics and mechanisms of chloronitrophenol in UV/PMS system[J]. China Environmental Science, 2016,36(1):66-73.
[6]
Yang S, Wang P, Yang X, et al. Degradation efficiencies of azo dye Acid Orange 7by the interaction of heat, UV and anions with common oxidants:persulfate, peroxymonosulfate and hydrogen peroxide[J]. Journal of Hazardous Materials, 2010,179(1):552-558.
[7]
Chen X Y, Qiao X L, Wang D G, et al. Kinetics of oxidative decolorization and mineralization of Acid Orange 7by dark and photoassisted Co2+ catalyzed peroxymonosulfate system[J]. Chemosphere, 2007,67(4):802-808.
[8]
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.
[9]
Wei C, Zhang J, Zhang Y, et al. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a Co-NiOx catalyst[J]. Water Science & Technology A:Journal of the International Association on Water Pollution Research, 2017,76(6):1436-1446.
[10]
Chen X, Chen J, Qiao X, et al. Performance of nano-Co3O4/peroxymonosulfate system:Kinetics and mechanism study using Acid Orange 7as a model compound[J]. Applied Catalysis B Environmental, 2008,80(1):116-121.
[11]
Sun H Q, Tian H Y, Hardjono Y, et al. Preparation of cobalt/carbon-xerogel for heterogeneous oxidation of phenol[J]. Catalysis Today, 2016,186(1):63-68.
[12]
Yang Y, Banerjee G, Brudvig G W, et al. Oxidation of organic compounds in water by unactivated peroxymonosulfate[J]. Environmental Science & Technology, 2018,52(10):5911-5919.
[13]
Liu W G, Z L L, Liu X, et al. Discriminating Catalytically active FeNx species of atomically dispersed Fe-N-C catalyst for selective oxidation of the C-H bond[J]. Journal of the American Chemical Society, 2017,139(31):10790-10798.
[14]
Xiao M L, Zhu J B, Ma L, et al. Microporous Framework-induced synthesis of single-atom dispersed Fe-N-C acidic orr catalyst and its in-situ reduced Fe-N-C active site identification revealed by X-ray absorption spectroscopy[J]. ACS Catalysis, 2018,8(4):2824-2832.
[15]
Liu W G, Z L L, Yan W S, et al. Single-atom dispersed Co-N-C catalyst:structure identification and performance for hydrogenative coupling of nitroarenes[J]. Chemical Science, 2016,7(9):5758-5964.
[16]
Chen X, Guo H G, Zhang Y L, et al. Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes[J]. Water Research, 2017,113(15):80-88.
[17]
Kim J, Edwards J O. A study of cobalt catalysis and copper modification in the coupled decompositions of hydrogen peroxide and peroxomonosulfate ion[J]. Inorganica Chimica Acta, 1995,235(1):9-13.
[18]
Lu S, G W, S C, et al. Heterogeneous activation of peroxymonosulfate by LaCo1-xCuxO3 perovskites for degradation of organic pollutants[J]. Journal of Hazardous Materials, 2018,353(2):401-409.
[19]
Zhang T, Zhu H, Croué J. Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water:efficiency, stability, and mechanism[J]. Environmental Science & Technology, 2013,47(6):2784-2791.
[20]
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.
[21]
Liu J, Zhou J, Ding Z, et al. Ultrasound irritation enhanced heterogeneous activation of peroxymonosulfate with Fe3O4 for degradation of azo dye[J]. Ultrasonics Sonochemistry, 2017,34:953-959.
[22]
Gong F, Wang L, Li D, et al. An effective heterogeneous iron-based catalyst to activate peroxymonosulfate for organic contaminants removal[J]. Chemical Engineering Journal, 2015,267:102-110.
[23]
Zhang W Q, Zhou S Q, Sun J L, et al. Impact of chloride ions on UV/H2O2 and UV/persulfate advanced oxidation processes[J]. Environmental Science & Technology, 2018,52(13):7380-7389.
[24]
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, Chen 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.
[25]
Wang Z, Yuan R, Guo Y, et al. Effects of chloride ions on bleaching of azo dyes by Co2+/oxone regent:Kinetic analysis[J]. Journal of Hazardous Materials, 2011,190(1):1083-1087.
[26]
Lindsey M E, Tarr M A. Inhibition of hydroxyl radical reaction with aromatics by dissolved natural organic matter[J]. Environmental Science & Technology, 2000,34(3):444-449.
[27]
Yang Z, Jin J, Yuan G, et al. Activation of peroxymonosulfate by benzoquinone:a novel nonradical oxidation process[J]. Environmental Science & Technology, 2015,49(21):12941-12950.
[28]
Yun E T, Lee J H, Kim J, et al. Identifying the nonradical mechanism in the peroxymonosulfate activation process:singlet oxygenation versus mediated electron transfer[J]. Environmental Science & Technology, 2018,52(12):7032-7042.
[29]
Zhang J, Shao X, Shi C, et al. Decolorization of acid orange 7 with peroxymonosulfate oxidation catalyzed by granular activated carbon[J]. Chemical Engineering Journal, 2013,232(10):259-265.
[30]
Liang H Y, Zhang Y Q, Huang S B, et al. Oxidative degradation of p-chloroaniline by copper oxidate activated persulfate[J]. Chemical Engineering Journal, 2013,218(3):384-391.
[31]
Wang Y, Sun H, Ang M, et al. 3D-hierarchically structured MnO2 for catalytic oxidation of phenol solutions by activation of peroxymonosulfate:Structure dependence and mechanism[J]. Applied Catalysis B Environmental, 2015,164:159-167.
[32]
Liang P, Zhang C, Duan X, et al. An insight into metal organic framework derived N-doped graphene for the oxidative degradation of persistent contaminants:formation mechanism and generation of singlet oxygen from peroxymonosulfate[J]. Environmental ence:Nano, 2017,4(2):315-324.
[33]
Wang K, Zhang J, Lou L, et al. UV or visible light induced photodegradation of AO7on TiO2 particles:the influence of inorganic anions[J]. Journal of Photochemistry & Photobiology A Chemistry, 2004,165(30):201-207.
[34]
王柯晴,徐劼,沈芷璇,等. LaCoO3钙钛矿活化过一硫酸盐降解萘普生[J]. 化工学报, 2020,71(3):1326-1334. Wang K Q, Xu J, Shen Z X, et al. Degradation of naproxen by peroxymonosulfate activated with LaCoO3[J]. CIESC Journal, 2020,71(3):1326-1334.
