UV/O<sub>3</sub>/TiO<sub>2</sub>耦合工艺降解2,4,6-三氯苯酚

朱彤; 杨世鹏; 谭伟强; 王凯军

doi:10.13205/j.hjgc.202103002

UV/O₃/TiO₂耦合工艺降解2,4,6-三氯苯酚

doi: 10.13205/j.hjgc.202103002

朱彤^1,2,
杨世鹏²,
谭伟强¹,
王凯军^2, ,

1. 青岛理工大学环境与市政工程学院, 山东青岛 266033;
2. 清华大学环境学院, 北京 100084

基金项目:

国家水体污染控制与治理科技重大专项（2017ZX07103-003）；国家水体污染控制与治理科技重大专项（2018ZX07110）。

详细信息

作者简介:
朱彤(1996-),女,硕士研究生,主要研究方向为废水高级氧化处理技术。zhutong1229@126.com

通讯作者:
王凯军(1960-),男,博士,教授,主要研究方向为厌氧生物发酵及水污染控制。wkj@tsinghua.edu.cn

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出版历程
- 收稿日期: 2020-06-16
- 网络出版日期: 2021-07-19

DEGRADATION OF 2,4,6-TRICHLOROPHENOL BY UV/O₃/TiO₂ COUPLING PROCESS

1. School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266033, China;
2. School of Environment, Tsinghua University, Beijing 100084, China

摘要

摘要: 通过构建UV/O₃/TiO₂耦合工艺反应体系，打破了以臭氧为基础的高级氧化技术臭氧利用率低的技术瓶颈，使用电子自旋共振波谱仪和荧光探针法分析了UV/O₃/TiO₂耦合工艺的反应机理，明确了臭氧链式反应产生的O₂在反应体系内自循环利用是提高臭氧利用率的主要原因。以2，4，6-三氯苯酚为目标污染物，通过分析初始浓度、接触时间、pH、催化剂投加量等影响因素，对比UV/O₃、UV/TiO₂工艺的降解效果，显示出UV/O₃/TiO₂耦合工艺的技术优势。在相同条件下，单独UV/TiO₂光催化体系和UV/O₃体系对2，4，6-三氯苯酚模拟配水的TOC矿化率分别为12.65%和51.54%，反应速率常数分别为0.0058，0.1956 min^-1，而UV/O₃/TiO₂耦合体系的矿化率达到82.97%，反应速率常数为0.2893 min^-1，耦合工艺的臭氧利用率较UV/O₃工艺提高11.7百分点，并且在pH=3~11的较宽范围内有良好的适用性，证明了理论研究结论的正确性。
- UV/O₃/TiO₂ /
- 2,4,6-三氯苯酚 /
- 光催化臭氧化 /
- 羟基自由基
Abstract: This paper broke the technical bottleneck of low ozone utilization of advanced oxidation technology based on ozone, through constructing a reaction system of UV/O₃/TiO₂ coupling process. The reaction mechanism of UV/O₃/TiO₂ coupling process was analyzed by ESR and fluorescence probe method, and it was clear that the self recycling of oxygen produced by ozone chain reaction in the reaction system was the main reason to improve ozone utilization. Taking 2,4,6-trichlorophenol as the target pollutant, through the analysis of initial concentration, contact time, pH, catalyst dosage and other factors, the degradation effect of UV/O₃ and UV/TiO₂ processes was compared, which highlighted the technical advantages of UV/O₃/TiO₂ coupling process. The results showed that the mineralization rate of 2,4,6-trichlorophenol solution by UV/TiO₂ and UV/O₃ was 12.65% and 51.54% in the same condition, and the reaction rate constant was 0.0058 min^-1 and 0.1956 min^-1 respectively. The mineralization rate of 2,4,6-trichlorophenol by UV/O₃/TiO₂ was 82.97% and the reaction rate constant was 0.2893 min^-1. The utilization ratio of ozone was increased by 11.7% in the coupling process with good adaptability in the wide range of pH=3~11. The result could provide data support for theoretical research conclusion.
- UV/O₃/TiO₂ /
- 2,4,6-TCP /
- photocatalytic ozonation /
- hydroxyl radical

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参考文献(30)

[1]	LIU B, CHEN B, ZHANG B Y, et al. Photocatalytic degradation of polycyclic aromatic hydrocarbons in offshore produced water:effects of water matrix[J]. Journal of Environmental Engineering, 2016, 142(11):04016054.
[2]	LIU B, CHEN B, LEE K, et al. Removal of naphthalene from offshore produced water through immobilized nano-TiO₂ aided photo-oxidation[J]. Water Quality Research Journal of Canada, 2016, 51(3):246-255.
[3]	李贞燕, 陈冰. 纳米二氧化钛光催化氧化油田采出水中萘和芴的影响因素分析[J]. 环境工程学报, 2015, 9(5):2106-2112.
[4]	李贞燕, 陈冰. 油田采出水中萘和芴的紫外光催化和·OH氧化降解过程影响因素与条件优化分析[J]. 环境工程, 2015, 33(10):31-34.
[5]	LIU B, CHEN B, ZHANG B Y. Oily wastewater treatment by nano-TiO₂-induced photocatalysis:seeking more efficient and feasible solutions[J]. IEEE Nanotechnology Magazine, 2017, 11(3):4-15.
[6]	GOMES J F, BEDNARCZYK K, GMUREK M, et al. Noble metal-TiO₂, supported catalysts for the catalytic ozonation of parabens mixtures[J]. Process Safety & Environmental Protection, 2017, 111:148-159.
[7]	MARTINS R C, QUINTA-FERREIRA R M. Screening of ceria-based and commercial ceramic catalysts for catalytic ozonation of simulated olive mill wastewaters[J]. Industrial & Engineering Chemistry Research, 2009, 48(3):1196-1202.
[8]	CENTI G, PERATHONER S. Advanced Oxidation Processes in Water Treatment[M]. Handbook of Advanced Methods and Processes in Oxidation Catalysis:from Laboratory to Industry, 2014:251-290.
[9]	OFIARSKA A, PIECZYŃSKA A, FISZKA B A, et al. Pt-TiO₂-assisted photocatalytic degradation of the cytostatic drugs ifosfamide and cyclophosphamide under artificial sunlight[J]. Chemical Engineering Journal, 2016, 285:417-427.
[10]	VELEGRAKI T, HAPESHI E, FATTAKASSINOS D, et al. Solar-induced heterogeneous photocatalytic degradation of methyl-paraben[J]. Applied Catalysis B:Environmental, 2015,178:2-11.
[11]	LIN Y, FERRONATO C, DENG N, et al. Study of benzylparaben photocatalytic degradation by TiO₂[J]. Applied Catalysis B Environmental, 2011, 104(3/4):353-360.
[12]	HUANG H, LI W. Destruction of toluene by ozone-enhanced photocatalysis:performance and mechanism[J]. Applied Catalysis B:Environmental, 2011, 102(3/4):449-453.
[13]	CHONG M N, JIN B, CHOW C W K, et al. Recent developments in photocatalytic water treatment technology:A review[J]. Water Research, 2010, 44(10):2997-3027.
[14]	SALIMI M, ESRAFILI A, GHOLAMI M, et al. Contaminants of emerging concern:a review of new approach in AOP technologies[J]. Environmental Monitoring and Assessment, 2017, 189(8):414.
[15]	余丽琴, 赵高峰, 冯敏, 等. 典型氯酚类化合物对水生生物的毒性研究进展[J].生态毒理学报,2013,8(5):658-670.
[16]	贺强礼, 关向杰, 黄水娥, 等. 典型酚类废水的微生物处理研究现状及其进展[J]. 环境工程, 2014,32(3):6-9.
[17]	宋瀚文, 王东红, 徐雄, 等. 我国24个典型饮用水源地中14种酚类化合物浓度分布特征[J]. 环境科学学报, 2014, 34(2):355-362.
[18]	赵德明,李敏,张建庭,等.微波强化臭氧氧化降解苯酚水溶液[J]. 化工学报,2009,60(12):3137-3141.
[19]	YAN G L, CHEN J, HUA Z Z. Roles of H₂O₂ and OH radical in bactericidal action of immobilized TiO₂ thin-film reactor:an ESR study[J]. Journal of Photochemistry and Photobiology A:Chemistry, 2009, 207(2/3):153-159.
[20]	GOMES J F, LEAL I, BEDNARCZYK K, et al. Photocatalytic ozonation using doped TiO₂ catalysts for the removal of parabens in water[J]. Science of the Total Environment, 2017, 609:329-340.
[21]	MEHRJOUEI M, MVLLER S, MÖLLER D. A review on photocatalytic ozonation used for the treatment of water and wastewater[J]. Chemical Engineering Journal, 2015, 263:209-219.
[22]	MERENYI G, LIND J, NAUMO V S, et al. Reaction of ozone with hydrogen peroxide (peroxone process):a revision of current mechanistic concepts based on thermokinetic and quantum-chemical considerations[J]. Environmental Science & Technology, 2010, 44(9):3505-3507.
[23]	MOREIRA N F F, ORGE C A, RIBEIRO A R, et al. Fast mineralization and detoxification of amoxicillin and diclofenac by photocatalytic ozonation and application to an urban wastewater[J]. Water Research, 2015, 87:87-96.
[24]	李志健, 马兰, 景立明, 等. 2,4,6-三氯苯酚臭氧氧化特性研究[J]. 纸和造纸, 2015, 34(11):69-73.
[25]	CHONG M N, JIN B, CHOW C W K, et al. Recent developments in photocatalytic water treatment technology:a review[J]. Water Research, 2010, 44(10):2997-3027.
[26]	王欣, 王金翠, 殷晓梅, 等. 乙酰甲胺磷UV-TiO₂/类Fenton光催化降解过程的响应面法优化[J]. 应用化工, 2013, 42(1):33-40.
[27]	AGUSTINA T E, ANG H M, VAREEK V K. A review of synergistic effect of photocatalysis and ozonation on wastewater treatment[J]. Journal of Photochemistry and Photobiology C:Photochemistry Reviews, 2005, 6(4):264-273.
[28]	刘茜, 唐飏, 李越, 等. 可见光下F-TiO₂催化剂对2,4,6-三氯苯酚光催化活性研究[J].化学研究与应用,2017,29(6):761-767.
[29]	殷晓梅, 王欣, 王金翠, 等. 纳米TiO₂-UV光催化降解乙酰甲胺磷影响因素的研究[J]. 应用化工, 2012, 41(9):1508-1512.
[30]	王旭东, 唐婧, 王磊, 等. 纳米TiO₂光催化-超滤法处理模拟二级出水[J]. 环境工程学报, 2016,10(4):1615-1620.