苯醌对聚合硅酸铁多相UV-Fenton体系的增效机制

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摘要通过构建苯醌增效聚合硅酸铁多相UV-Fenton体系，讨论了体系中橙Ⅱ的脱色和降解途径.在研究苯醌浓度对聚合硅酸铁铁离子的释放、Fe²⁺与Fe³⁺之间的转化、H₂O₂分解和·OH生成影响的基础上，提出了苯醌对聚合硅酸铁多相UV-Fenton体系的增效机制.结果表明，随苯醌浓度的增加，其紫外光下光解还原聚合硅酸铁并释放Fe²⁺的程度增大、H₂O₂分解速度加快、产生·OH浓度峰值增高且出现的时间提前；苯醌增效体系释放于溶液中的Fe²⁺可以通过Fenton反应转化成Fe³⁺，反应结束后聚合硅酸铁能重新吸附Fe³⁺并使其浓度降低，避免了增效体系铁离子的二次污染.本研究将为多相催化剂催化过程的调控提供新的视角，为多相光助-芬顿反应在有机废水资源化中的应用提供理论依据和技术支持.

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	姜自立
	李献众
	刘治庆
	刘力章
	陈建新

关键词 ：多相UV-Fenton体系, 橙Ⅱ, 聚合硅酸铁, 苯醌, 羟基自由基

Abstract：The decoloration and degradation pathway of Orange II were discussed in BQ enhanced heterogeneous UV-Fenton system with PSF as catalyst. Based on the study of BQ concentration's effects on the release of iron ions from PSF, the changes between Fe²⁺ and Fe³⁺, the decomposition of hydrogen peroxide and the generation of·OH, an enhanced mechanism of benzoquinone (BQ) on Poly-Silicate-Ferric (PSF) in heterogeneous UV-Fenton system was proposed. The results showed that with the increase of BQ concentration, the degree of Fe²⁺ released from PSF by photolysis reduction under UV light increased, the decomposition of hydrogen peroxide accelerated, and the peak of hydroxyl radical concentration increased and appeared earlier. The Fe²⁺ released from PSF would convert into Fe³⁺ through Fenton reaction in BQ enhanced heterogeneous UV-Fenton system. After treatment, the concentration of Fe³⁺ could be significantly decreased by adsorption on PSF, avoiding secondary pollution of iron ions. This study will provide a new perspective for the regulation of heterogeneous catalysts, and provide theoretical basis and technical support for the application of heterogeneous UV-Fenton reaction in the recycling of organic wastewater.

Key words： heterogeneous UV-Fenton system OrangeⅡ PSF benzoquinone hydroxyl radical

收稿日期: 2019-11-30

PACS:

X503

基金资助:国家自然科学基金资助项目（21966021，21367021）；广东省科技计划资助项目（2017B030314175）；江西省教育厅基金资助项目（GJJ13072）

通讯作者: 陈建新,副教授,jxchen@ncu.edu.cn E-mail: jxchen@ncu.edu.cn

作者简介: 姜自立(1996-),男,江西南昌人,南昌大学硕士研究生,主要从事水污染控制研究.

引用本文:

姜自立, 李献众, 刘治庆, 刘力章, 陈建新. 苯醌对聚合硅酸铁多相UV-Fenton体系的增效机制[J]. 中国环境科学, 2020, 40(7): 2943-2951. JIANG Zi-li, LI Xian-zhong, LIU Zhi-qing, LIU Li-zhang, CHEN Jian-xin. The enhanced mechanism of benzoquinone(BQ) on poly-silicate-ferric(PSF) in heterogeneous UV-Fenton system. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(7): 2943-2951.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2020/V40/I7/2943

[1]	Yuan D, Zhang C, Tang S, et al. Enhancing CaO2 fenton-like process by Fe(II)-oxalic acid complexation for organic wastewater treatment[J]. Water Research, 2019,163:1-11.
[2]	郝思宇,张艾,刘亚男.臭氧与过氧化钙协同降解甲基红废水[J]. 中国环境科学, 2019,39(2):591-597. Hao S Y, Zhang A, Liu Y N. Removal of methyl red in aqueous by O3/CaO2 treatment:influencing factors and synergetic effects[J]. China Environmental Science, 2019,39(2):591-597.
[3]	Zhao Q, Lu D, Ma J, et al. Peroxymonosulfate-based cleaning technology for metal oxide-coated ceramic ultrafiltration membrane polluted by Alcian Blue 8GX dye:Radical and non-radical oxidation cleaning mechanism[J]. Journal of Membrane Science, 2019,573:210-217.
[4]	Law J C, Leung K S. Redox mediators and irradiation improve fenton degradation of acesulfame[J]. Chemosphere, 2019,217:374-382.
[5]	徐淑英,陈建新,王琳,等.不同晶型铁氧化Fenton和UV-Fenton降解橙Ⅱ的催化性能[J]. 安全与环境学报, 2017,17(4):1448-1453. Xu S Y, Chen J X, Wang L, et al. Catalytic features of iron oxides with different crystal forms during Orange Ⅱ degradation in Fenton and UV-Fenton systems[J]. Journal of Safety and Environment, 2017,17(4):1448-1453.
[6]	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.
[7]	苗笑增,戴慧旺,陈建新,等.草酸根对α-FeOOH多相UV-Fenton催化能力的增效实验[J]. 环境科学, 2018,39(3):1202-1211. Miao X Z, Dai H W, Chen J X, et al. Experiment to enhance catalytic activity of α-FeOOH in heterogeneous UV-Fenton system by addition of oxalate[J]. Environmental Science, 2018,39(3):1202-1211.
[8]	Gao J, Liu Y, Xia X, et al. Mechanisms for photo assisted Fenton of synthesized pyrrhotite at neutral pH[J]. Applied Surface Science, 2019,463:863-871.
[9]	Zeng L, Gong J, Dan J, et al. Novel visible light enhanced Pyrite-Fenton system toward ultrarapid oxidation of p-nitrophenol:Catalytic activity, characterization andme-chanism[J]. Chemosphere, 2019,228:232-240.
[10]	冯勇,吴德礼,马鲁铭.黄铁矿催化类Fenton反应处理阳离子红X-GRL废水[J]. 中国环境科学, 2012,32(6):1011-1017. Fang Y, Wu D L, Ma L M. Treatment of cationic Red X-GRL wastewater by pyrite catalyzed Fenton-like reaction[J]. China Environmental Science, 2012,32(6):1011-1017.
[11]	Choe Y J, Byun J Y, Kim S H, et al. Fe3S4/Fe7S8-promoted degradation of phenol via heterogeneous, catalytic H2O2 scission mediated by S-modified surface Fe2+ species[J]. Applied Catalysis B:Environmental, 2018,233:272-280.
[12]	Li Y J, Ning P, Tian S L. Ferrocene-catalyzed heterogeneous Fenton-like degradation mechanisms and pathways of antibiotics under simulated sunlight:A case study of sulfamethoxazole[J]. Journal of Hazardous Materials, 2018,353:26-34.
[13]	张彪军,田森林,李英杰,等.光助-二茂铁/H2O2非均相体系降解磺胺二甲基嘧啶[J]. 环境科学, 2018,39(11):5043-5050. Zhang B J, Tian S L, Li Y J, et al. Photo-assisted degradation of sulfamethazine by ferrocene-catalyzed heterogeneous Fenton-like system[J]. Environmental Science, 2018,39(11):5043-5050.
[14]	李志丽,张潇逸,杨萍,等.基于小角度激光光散射的聚硅酸铁絮体特性研究[J]. 中国给水排水, 2017,33(11):91-96. Li Z L, Zhang X Y, Yang P, et al. Flocs characteristics of poly-silicic-ferric coagulant based on small-angle laser light scattering[J]. China Water & Wastewater, 2017,33(11):91-96.
[15]	Liu Y, Shen J, Chen Z. Effects of amorphous-zinc-silicate-catalyzed ozonation on the degradation of p-chloronitr obenzene in drinking water[J]. Applied Catalysis A:General, 2011,403:112-118.
[16]	Liu Y, Shen J, Chen Z. Degradation of p-chloronitrobenzene in drinking water by manganese silicate catalyzed ozonation[J]. Desalination, 2011,279:219-224.
[17]	刘玥,陈忠林,杨磊,等.聚合硅酸铁催化臭氧氧化硝基氯苯的效能[J]. 哈尔滨工业大学学报, 2010,42:914-918. Liu Y, Chen Z L, Yang L, et al. Iron silicate polymer catalyzed ozonation for removing chloronitrobenzenes in drinking water[J]. Journal of Harbin Institute of Technology, 2010,42:914-918.
[18]	Gao G, Kang J, Shen J, et al. Catalytic ozonation of sulfamet hoxazole by composite iron-manganese silicate oxide:cooperation mechanism between adsorption and catalytic reaction[J]. Environmental Science and Pollution Research, 2016,23:21360-21368.
[19]	侯炳江,沈吉敏,李太平,等.硅酸铁催化臭氧去除水中的阿特拉津和硝基苯[J]. 黑龙江大学自然科学学报, 2015,32:223-228. Hou B J, Shen J M, Li T P, et al. Removal of atrazine and nitrobenzene in water by iron silicate catalized ozonation[J]. Journal of Natural Science of Heilongjiang University, 2015,32:223-228.
[20]	叶国杰,王一显,韦朝海,等.水处理高级氧化法活性物种生成机制及其技术特征分析[J/OL]. 环境工程, http://kns.cnki.net/kcms/detail/11.2097.X.20191011.0858.002.html. Ye G J, Wang Y X, Wei C H, et al. Formation mechanism of active species in advanced oxidation technologies and analysis on its technical characteristics in water treatment[J]. Environmental Engineering, http://kns.cnki.net/kcms/detail/11.2097.X.20191011.0858.002.html.
[21]	贺俊梅,孔令娜,梁倩,等.苯醌类与苯醌亚胺类在光/Fenton体系中的光敏性[J]. 中国环境科学, 2016,36(9):2638-2644. He J M, Kong L N, Liang Q, et al. Photosensitivity of benzoquinones and benzoquinoneimines in the sunlight/fenton system[J]. China Environmental Science, 2016,36(9):2638-2644.
[22]	顾佳.紫外光解苯酚及对苯醌水溶液产生水合电子的机理研究[D]. 哈尔滨:哈尔滨工业大学, 2018:49-50. Gu J. Mechanism of hydrated electron generation by UV photolysis of phenol and p-benzoquinone in aqueous solution[D]. Harbin:Harbin Institute of Technology, 2018:49-50.
[23]	Lenoble V, Laclautre C, Deluchat V, et al. Arsenic removal by adsorption on iron(III) phosphate[J]. Journal of Hazardous Materials, 2005,B123:262-268.
[24]	Zhong X, Royer S, Zhang H, et al. Mesoporous silica iron-doped as stable and efficient heterogeneous catalyst for the degradation of C.I. Acid Orange 7using sono-photo-Fenton process[J]. Separation and Purification Technology, 2011,80:163-171.
[25]	Li H, Gong Y, Huang Q, et al. Degradation of Orange II by UV-Assisted advanced Fenton process:Response surface approach, degradation pathway, and biodegradability[J]. Industrial & Engineering Chemistry Research. 2013,52:15560-15567.
[26]	Jiang T, PoyrazA S, Iyer A,et al. Synthesis of mesoporous iron oxides by an inverse micelle method and their application in the degradation of Orange II under visible light at neutral pH[J]. The Journal of Physical Chemistry C, 2015,119:10454-10468.
[27]	Hel Golrner. Photoprocesses of p-benzoquinones in aqueous solution[J]. The Journal of Physical Chemistry C, 2003,107:11587-11595.
[28]	Sonntag J V, Mvula E, Hildenbrand K, et al. Photohydroxylation of 1,4-benzoquinone in aqueous solution revisited[J]. Chemistry-A European Journal, 2004,10:440-451.
[29]	刘强,孙英平,汪小熊,等.对苯二酚强化多相类Fenton过程降解活性艳红MX-5B的效能与机理[J]. 环境科学学报, 2012,32(7):1589-1595. Liu Q, Sun Y P, Wang X X, et al. The efficiency and mechanisms of the enhancement of hydroquinone on the degradation of reactive red MX-5B by heterogeneous Fenton-like reaction[J]. Acta Scientiae Circumstantiae, 2012,32(7):1589-1595.
[30]	严梅,张青,谢慧芳,等.纳米Fe3O4负载聚苯胺对染料的协同催化降解[J]. 中国环境科学, 2017,37(4):1394-1400. Yan M, Zhang Q, Xie H F, et al. Load of PANI on nano-Fe3O4 and synergy catalytic degradation of dyes[J]. China Environmental Science, 2017,37(4):1394-1400.
[31]	穆毅,贾法龙,张礼知,等.纳米零价铁活化分子氧原理及降解有机污染物性能增强策略[J]. 化学学报, 2017,75:538-543. Mu Y, Jia F L, Zhang L Z, et al. Molecular oxygen activation with nano zero-valent iron for aerobic degradation of organic contaminantsand the performance enhancement[J]. Acta Chimica Sinica, 2017,75:538-543.