氧基氯化铁非均相活化过一硫酸盐降解金橙Ⅱ

王柯晴, 徐劼, 陈家斌, 王澜静, 吴玮

中国环境科学 ›› 2020, Vol. 40 ›› Issue (8) : 3385-3393.

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中国环境科学 ›› 2020, Vol. 40 ›› Issue (8) : 3385-3393.
水污染与控制

氧基氯化铁非均相活化过一硫酸盐降解金橙Ⅱ

  • 王柯晴1, 徐劼1, 陈家斌2, 王澜静1, 吴玮1
作者信息 +

Degradation of AO7 by PMS activated by FeOCl

  • WANG Ke-qing1, XU Jie1, CHEN Jia-bin2, WANG Lan-jing1, WU Wei1
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摘要

采用部分热分解法制备了氧基氯化铁(FeOCl),用于活化过一硫酸盐(PMS)降解难降解偶氮染料金橙Ⅱ(AO7).利用X射线光电子能谱分析(XPS)、扫描电镜(SEM)和X射线衍射光谱(XRD)对其进行了表征;通过实验评估FeOCl/PMS体系对AO7的降解效果并分析了影响AO7去除率的各种因素.结果表明:FeOCl活化PMS降解AO7效果良好,矿化率达44%.在中性条件下,当FeOCl投加量50mg/L、PMS浓度1.0mmol/L、AO7浓度0.05mmol/L时,AO7可在30min内完全降解.随PMS投加量、FeOCl投加量、Cl-浓度和反应初始pH值的增大,AO7的脱色效果提高.FeOCl还具有良好的重复利用性.此外,通过自由基淬灭实验、EPR测试和XPS分析了反应的主要活性物种和反应机理:由PMS活化产生的SO4-·和·OH对污染物进行降解,其中主要活性物种为SO4-·.

Abstract

FeOCl was prepared by the partial thermal decomposition method, and then used to activate PMS to degrade refractory azo dye AO7.The synthesized FeOCl was characterized by XPS, SEM and XRD.The degradation of AO7 was evaluated in the FeOCl/PMS system, and various factors affecting the removal rate of AO7 was investigated. The results showed that AO7 was rapidly degraded in the FeOCl/PMS system, and mineralization rate has reached to 44%. AO7 could be completely degraded in 30min at neutral condition with 50mg/L FeOCl, 1.0mmol/L PMS and 0.05mmol/L AO7. The decolorization of AO7 increased with the increase of PMS concentration, FeOCl dosage, Cl- concentration and the initial pH. FeOCl also exhibited a fine reusability. The main active species and reaction mechanism were verified by the radical quenching experiment, EPR test and XPS analysis. The SO4-· and ·OH produced by the activation of PMS contributed to the degradation of pollutants, and SO4-· played the dominant role.

关键词

过一硫酸盐(PMS) / 活化 / 金橙Ⅱ(AO7) / 硫酸根自由基(SO4-·) / 氧基氯化铁(FeOCl)

Key words

acid orange 7(AO7) / activation / FeOCl / peroxymonosulfate / SO4-·

引用本文

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王柯晴, 徐劼, 陈家斌, 王澜静, 吴玮. 氧基氯化铁非均相活化过一硫酸盐降解金橙Ⅱ[J]. 中国环境科学. 2020, 40(8): 3385-3393
WANG Ke-qing, XU Jie, CHEN Jia-bin, WANG Lan-jing, WU Wei. Degradation of AO7 by PMS activated by FeOCl[J]. China Environmental Science. 2020, 40(8): 3385-3393
中图分类号: X703   

参考文献

[1] Fu Y, Viraraghavan T. Fungal decolorization of dye wastewaters:a review[J]. Bioresource Technology, 2001,79(3):251-262.
[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] Peralta-Zamora P, Kunz A, de Moraes S G, et al. Degradation of reactive dyes I. A comparative study of ozonation, enzymatic and photochemical processes[J]. Chemosphere, 1999,38(4):852.
[4] Ji Y, Dong C, Kong D, et al. Heat-activated persulfate oxidation of atrazine:Implications for remediation of groundwater contaminated by herbicides[J]. Chemical Engineering Journal, 2015,263:45-54.
[5] Lominchar M A, Santos A, De M E, et al. Remediation of aged diesel contaminated soil by alkaline activated persulfate[J]. Science of the Total Environment, 2017,622-623:41-48.
[6] 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):66-73. 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.
[7] Cai C, Zhang H, Zhong X, et al. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe-Co/SBA-15catalyst for the degradation of Orange II in water[J]. Journal of Hazardous Materials, 2015,283:70-79.
[8] Chen L, Hu X, Yin Y, et al. Degradation of atrazine and structurally related s-triazine herbicides in soils by ferrous-activated persulfate:Kinetics, mechanisms and soil-types effects[J]. Chemical Engineering Journal, 2018,351:523-531.
[9] Tugba O H, Idil A A. Comparison of sulfate and hydroxyl radical based advanced oxidation of phenol[J]. Chemical Engineering Journal, 2013,224(1):10-16.
[10] 毕文龙,郝茜华,刘奋武,等.硫酸根自由基对活性炭吸附刚果红的影响[J].中国环境科学, 2020,40(1):190-197. Bi W L, Hao Q H, Liu F W, et al. Effect of sulfate radical on adsorption of Congo red by activated carbon[J]. China Environmental Science, 2020,40(1):190-197.
[11] Pang X, Yang G, Zhang Y, et al. LaCoO3 perovskite oxide activation of peroxymonosulfate for aqueous 2-phenyl-5-sulfobenzimidazole degradation:Effect of synthetic method and the reaction mechanism[J]. Chemical Engineering Journal, 2016,304:897-907.
[12] Yan J, Lei M, Zhu L, et al. Degradation of sulfamonomethoxine with Fe3O4 magnetic nanoparticles as heterogeneous activator of persulfate[J]. Journal of Hazardous Materials, 2011,186(2/3):1398-1404.
[13] Mian M M, Liu G. Sewage sludge-derived TiO2/Fe/Fe3C-biochar composite as an efficient heterogeneous catalyst for degradation of methylene blue[J]. Chemosphere, 2019,215:101-114.
[14] Wu J, Gao H, Yao S, et al. Degradation of Crystal Violet by catalytic ozonation using Fe/activated carbon catalyst[J]. Separation & Purification Technology, 2015,147:179-185.
[15] Elizarova G L, Zhidomirov G M, Parmon V N. Hydroxides of transition metals as artificial catalysts for oxidation of water to dioxygen[J]. Catalysis Today, 2000,58(2/3):71-88.
[16] Sagua A, Rivera A, León C, et al. High ionic conductivity of hydrated Li0.5FeOCl[J]. Solid State Ionics, 2006,177(11/12):1099-1104.
[17] 徐西蒙. FeOCl催化剂用于非均相Fenton体系催化降解水中微量有机物[D].上海:华东理工大学, 2013. Xu X M, FeOCl catalysts for the heterogeneous fenton degradation of trace organic contaminants[D]. Shanghai:East China University of Science and Technology, 2013.
[18] Liang C, Huang C F, Mohanty N, et al. A rapid spectrophotometric determination of persulfate anion in ISCO[J]. Chemosphere, 2008,73(9):1540-1543.
[19] Dai Y D, Yu Z, He Y, et al. Mössbauer studies on the spiral antiferromagnetic coupling in iron oxychloride[J]. Chemical Physics Letters, 2002,358(5):473-478.
[20] Betterton E A, Hoffmann M R. Kinetics and mechanism of the oxidation of aqueous hydrogen sulfide by peroxymonosulfate[J]. Environmental Science & Technology, 1990,24(12):1819-1824.
[21] George P A, Dionysios D D. Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt[J]. Environmental Science & Technology, 2003,37(20):4790.
[22] Guan Y H, Ma J, Ren Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Research, 2013,47(14):5431-5438.
[23] Wang Y, Zhang H, Zhu Y, et al. Au-NP-Decorated crystalline FeOCl nanosheet:Facile synthesis by laser ablation in liquid and its exclusive gas sensing response to HCl at room temperature[J]. Advanced Materials Interfaces, 2016,3(9):1500801.
[24] Jie L, Zhao Z, Shao P, et al. Activation of peroxymonosulfate with magnetic Fe3O4-MnO2 core-shell nanocomposites for 4-chlorophenol degradation[J]. Chemical Engineering Journal, 2015,262(9):854-861.
[25] Duan X, O'Donnell K, Sun H, et al. Sulfur and nitrogen Co-doped graphene for metal-free catalytic oxidation reactions[J]. Small, 2015, 11(25):3036-3044.
[26] Mezohegyi G, Gonçalves F, órfão J J M, et al. Tailored activated carbons as catalysts in biodecolourisation of textile azo dyes[J]. Applied Catalysis B Environmental, 2010,94(1):179-185.
[27] 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.
[28] Guan Y H, Ma J, Li X C, et al. Influence of pH on the formation of sulfate and hydroxyl radicals in the UV/peroxymonosulfate system[J]. Environmental Science & Technology, 2011,45(21):9308-9314.
[29] 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.
[30] Abdullah M, Low G K C, Matthews R W. Effects of common inorganic anions on rates of photocatalytic oxidation of organic carbon over illuminated titanium dioxide[J]. Journal of Physical Chemistry, 1990,94(17):6820-6825.
[31] 邵子纯,卢建,高仕谦,等.共价三嗪骨架活化过一硫酸盐降解磺胺甲恶唑[J].中国环境科学, 2020,40(1):135-142. Shao Z C, Lu J, Gao S Q, et al. Covalent triazine-based framework activates peroxymonosulfate to degrade sulfamethoxazole[J]. China Environmental Science, 2020,40(1):135-142.
[32] 王萍.过硫酸盐高级氧化技术活化方法研究[D].青岛:中国海洋大学, 2010. Wang P, Activation mothods of advanced persulfate oxidation[D]. Qingdao:Ocean University of China, 2010.
[33] Latifoglu A, Gurol M D. The effect of humic acids on nitrobenzene oxidation by ozonation and O3/UV processes[J]. Water Research, 2003,37(8):1889.
[34] Furman O S, Teel A L, Ahmad M, et al. Effect of basicity on persulfate reactivity[J]. Journal of Environmental Engineering, 2011, 137(4):241-247.
[35] Yan J, Lei M, Zhu L, et al. Degradation of sulfamonomethoxine with Fe3O4 magnetic nanoparticles as heterogeneous activator of persulfate[J]. Journal of Hazardous Materials, 2011,186(2/3):1398-1404.
[36] 戴慧旺,陈建新,苗笑增,等.醇类对UV-Fenton体系羟基自由基淬灭效率的影响[J].中国环境科学, 2018,38(1):202-209. Dai H W, Chen J X, Miao X Z, et al. Effect of alcohols on scavenging efficiencies to hydroxyl radical in UV-Fenton system[J]. China Environmental Science, 2018,38(1):202-209.
[37] 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.

基金

水体污染控制与治理科技重大专项(No.2017ZX07201001);国家自然科学基金资助项目(51778391)

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