超重力强化臭氧高级氧化技术的研究进展

doi:10.16085/j.issn.1000-6613.2020-1039

摘要/Abstract

摘要：

臭氧高级氧化技术因其绿色高效、适用性广、操作简便等优势，成为当前水处理领域前沿技术之一，但臭氧在传统反应器内普遍存在吸收效果差，臭氧利用率低等缺陷。旋转填料床（RPB）利用高速旋转的填料产生超重力场，将液体剪切破碎为细小的液膜、液丝或液滴，其较高的相界面积、不断更新的界面以及内部流体的强制湍动，加快了臭氧的传质与分解，该技术对于传质受限的臭氧高级氧化过程的强化有着突出的优势。本文简述了超重力强化臭氧氧化过程的原理，介绍了RPB与O₃、O₃/H₂O₂、O₃/Fenton、O₃/PS（过硫酸盐）、催化臭氧氧化等高级氧化法耦合应用处理有机废水的研究现状，并对超重力技术的优势及技术突破进行了述评，总结了超重力应用臭氧高级氧化技术的潜在经济效益和环境效益，提出功能化填料及大型RPB的开发需求，以期为超重力技术在废水处理领域的拓展应用提供理论基础和技术参考。

关键词: 超重力, 臭氧, 多相流, 传质, 分解, 废水

Abstract:

Ozone-based advanced oxidation process (AOP) is one of the cutting-edge technologies in wastewater treatments due to its advantages of green-efficiency, wide applicability and simple operation. However, its absorption and utilization efficiency in traditional reactors is low. Rotating packed bed (RPB) applies high-speed rotating packing to generate high-gravity, splitting the liquid into thin film, filaments or small droplets. Hence, the mass transfer and decomposition efficiency of ozone can be significantly enhanced by the high gas-liquid interface area, interface renewal rate, and forced turbulence of internal fluid. This technology has the prominent advantages for the strengthening of ozone-based advanced oxidation process with limited mass transfer. In this study, the principle of enhanced ozonation by high gravity as well as the coupling applications of high gravity with AOPs such as O₃, O₃/H₂O₂, O₃/Fenton, O₃/PS, and catalytic ozonation in organic-based wastewater treatments are introduced. The advantages and technological breakthroughs of high gravity are discussed, and its potential economic and environmental benefits in wastewater treatments are summarized. The development of novel functional packing and large-scale RPB is proposed. This study could provide theoretical and technical implications for the industrial amplifications.

Key words: high gravity, ozone, multiphase flow, mass transfer, decomposition, wastewater

中图分类号:

X703

邵圣娟, 焦纬洲, 刘有智. 超重力强化臭氧高级氧化技术的研究进展[J]. 化工进展, 2020, 39(12): 4798-4811.

Shengjuan SHAO, Weizhou JIAO, Youzhi LIU. Research progress of high gravity enhanced ozone-based advanced oxidation technology[J]. Chemical Industry and Engineering Progress, 2020, 39(12): 4798-4811.

参考文献

1	刘浩, 邓慧萍, 刘铮. 臭氧多相催化氧化技术处理水中多环芳烃的进展[J]. 水处理技术, 2010, 36(8): 8-12.
1	LIU Hao, DENG Huiping, LIU Zheng. Analysis of heterogeneous catalytic ozonation for polycyclic aromatic hydrocarbons treatment [J]. Technology of Water Treatment, 2010, 36(8): 8-12.
2	魏兴跃, 吕行, 焦纬洲, 等. 超重力强化非均相催化臭氧矿化苯酚废水的响应面分析与优化[J]. 含能材料, 2020, 28(3): 268-276.
2	WEI Xingyue, Xing LYU, JIAO Weizhou, et al. Response surface analysis and optimization of high gravity-enhanced heterogeneous catalytic ozonation for mineralization of phenol wastewater[J]. Chinese Journal of Energetic Materials, 2020, 28(3): 268-276.
3	周洪政, 刘平, 张静, 等. 微气泡臭氧催化氧化-生化耦合处理难降解含氮杂环芳烃[J]. 中国环境科学, 2017, 37(8): 2978-2985.
3	ZHOU Hongzheng, LIU Ping, ZHANG Jing, et al. Removal of refractory nitrogen-containing heterocyclic aromatics by combination treatment of microbubble catalytic ozonation and biological process[J]. China Environmental Science, 2017, 37(8): 2978-2985.
4	WANG Zhe, CHEN Zhonglin, CHANG Jing, et al. Fabrication of a low-cost cementitious catalytic membrane for p-chloronitrobenzene degradation using a hybrid ozonation-membrane filtration system[J]. Chemical Engineering Journal, 2015, 262: 904-912.
5	SUBBARAMAIAH V, SRIVASTAVA V C, MALL I D. Catalytic oxidation of nitrobenzene by copper loaded activated carbon[J]. Separation & Purification Technology, 2014, 125: 284-290.
6	WANG Jianlong, CHU Libing. Irradiation treatment of pharmaceutical and personal care products (PPCPs) in water and wastewater: an overview[J]. Radiation Physics and Chemistry, 2016, 125: 56-64.
7	WU Chao, LI Pan, XIA Shengji, et al. The role of interface in microbubble ozonation of aromatic compounds[J]. Chemosphere, 2018, 220: 1067-1074.
8	初里冰, 邢新会, 于安峰, 等. 微米气泡强化臭氧氧化的作用机理研究[J]. 环境化学, 2007, 26(5): 622-625.
8	CHU Libing, XING Xinhui, YU Anfeng, et al. Enhancement mechanism of ozonation by micro-bubbles[J]. Environmental Chemistry, 2007, 26(5): 622-625.
9	GRACA C A L, LIMA R B, PEREIRA M F R, et al. Intensification of the ozone-water mass transfer in an oscillatory flow reactor with innovative design of periodic constrictions: optimization and application in ozonation water treatment[J]. Chemical Engineering Journal, 2020, 389: 124412.
10	秦月娇, 焦纬洲, 杨鹏飞, 等. 强化臭氧传质的研究进展[J]. 过程工程学报, 2017, 17(2): 420-426.
10	QIN Yuejiao, JIAO Weizhou, YANG Pengfei, et al. Research progress of enhancement of ozone mass transfer[J]. The Chinese Journal of Process Engineering, 2017, 17(2): 420-426.
11	LIN Chia-Chang, CHAO Chengyu, LIU Meiyun. Removal of ozone from air by absorption in a rotating packed bed[J]. Journal of Industrial and Engineering Chemistry, 2010, 16(1): 140-146.
12	ZENG Zequan, WANG Junfang, LI Zhenhao, et al. The advanced oxidation process of phenol solution by O₃/H₂O₂ in a rotating packed bed[J]. Ozone: Science & Engineering, 2013, 35(2): 101-108.
13	BELTRAN F J. Ozone reaction kinetics for water and wastewater systems[M]. Boca Raton, FL: Lewis Publishers, 2003.
14	BELTRAN F J. Theoretical aspects of the kinetics of competitive ozone reactions in water[J]. Ozone: Science & Engineering, 1995, 17(2): 163-182.
15	GOTTSCHALK C, LIBRA J A, SAUPE A. Ozonation of water and waste water: a practical guide to understanding ozone and its applications[M]. New York: John Wiley & Sons, 2009.
16	ZHAO Zilong, LIU Zekun, WANG Hongjie, et al. Sequential application of Fenton and ozone-based oxidation process for the abatement of Ni-EDTA containing nickel plating effluents[J]. Chemosphere, 2018, 202: 238-245.
17	CHEN Yi-Hung, CHANG Ching-Yuan, SU Weiling, et al. Modeling ozone contacting process in a rotating packed bed[J]. Industrial & Engineering Chemistry Research, 2004, 43(1): 228-236.
18	CHIU Chun-Yu, CHEN Yi-Hung, HUANG Yi-Haw. Removal of naphthalene in Brij30-containing solution by ozonation using rotating packed bed[J]. Journal of Hazardous Materials, 2007, 147(3): 732-737.
19	郭亮. 超重力强化O₃/H₂O₂ 氧化降解含硝基苯废水的研究[D]. 太原: 中北大学, 2015.
19	GUO Liang. Degradation of nitrobenzene-containing wastewater by O₃/H₂O₂ enhanced by high gravity[D]. Taiyuan: North University of China, 2015.
20	LIU Taoran, WANG Dan, WANG Wei, et al. Study on the efficient production of ozone water by a rotating packed bed[J]. Industrial & Engineering Chemistry Research, 2019, 58(17): 7227-7232.
21	CHEN Yi-Hung, CHANG Ching-Yuan, SU Weiling, et al. Ozonation of CI Reactive Black 5 using rotating packed bed and stirred tank reactor[J]. Journal of Chemical Technology & Biotechnology, 2005, 80(1): 68-75.
22	WANG Dan, LIU Taoran, MA Lei, et al. Modeling and experimental studies on ozone absorption into phenolic solution in a rotating packed bed[J]. Industrial & Engineering Chemistry Research, 2019, 58(17): 7052-7062.
23	SOTELO J L, BELTRAN F J, BENITEZ F J, et al. Henry's law constant for the ozone-water system[J]. Water Research, 1989, 23(10): 1239-1246.
24	YANG Peizhen, LUO Shuai, LIU Hongyan, et al. Aqueous ozone decomposition kinetics in a rotating packed bed[J]. Journal of the Taiwan Institute of Chemical Engineers, 2019, 96: 11-17.
25	沈慧芳, 张心亚, 刘晓鸿, 等. 臭氧在鼓泡塔中吸收与反应过程的模拟[J]. 华南理工大学学报(自然科学版), 2004, 32(5): 67-70.
25	SHEN Huifang, ZHANG Xinya, LIU Xiaohong, et al. Simulation of the absorption and reaction processes of ozone in bubble columns[J]. Journal of South China University of Technology (Natural Science Edition), 2004, 32(5): 67-70.
26	陈英, 李艳莉, 张浩, 等. 水中臭氧的分解动力学研究[J]. 高校化学工程学报, 2001, 15(5): 500-504.
26	CHEN Ying, LI Yanli, ZHANG Hao, et al. Studies on kinetics of ozone decomposition in water[J]. Journal of Chemical Engineering of Chinese Universities, 2001, 15(5): 500-504.
27	ZHAO Lei, MA Weichao, MA Jun, et al. Relationship between acceleration of hydroxyl radical initiation and increase of multiple-ultrasonic field amount in the process of ultrasound catalytic ozonation for degradation of nitrobenzene in aqueous solution[J]. Ultrasonics Sonochemistry, 2015, 22: 198-204.
28	XU Yin, ZHONG Xin, ZHANG Hui. Absorption and decomposition of ozone in a three-phase split-rectangular airlift reactor under ultrasonic irradiation[J]. Water Science & Technology, 2016, 73(8): 1796.
29	GUO Yang, ZHAO Erzhuo, WANG Jun, et al. Comparison of emerging contaminant abatement by conventional ozonation, catalytic ozonation, O₃/H₂O₂ and electro-peroxone processes[J]. Journal of Hazardous Materials, 2019, 389: 121829.
30	LIN Chia-Chang, LIU Wen-Tzong. Ozone oxidation in a rotating packed bed[J]. Journal of Chemical Technology & Biotechnology, 2003, 78(2/3): 138-141.
31	CHEN Yi-Hung, CHIU Chun-Yu, CHANG Ching-Yuan, et al. Modeling ozonation process with pollutant in a rotating packed bed[J]. Industrial & Engineering Chemistry Research, 2005, 44(1): 21-29.
32	刁金祥. 旋转填料床中O₃和O₃/H₂O₂氧化处理TNT红水的研究[D]. 太原: 中北大学, 2007.
32	DIAO Jinxiang. O₃ and O₃/H2O₂ oxidative treatment of TNT red-water in a rotating packed bed[D]. Taiyuan: North University of China, 2007.
33	JIAO Weizhou, LUO Shuai, HE Zhen, et al. Applications of high gravity technologies for wastewater treatment: a review[J]. Chemical Engineering Journal, 2017, 313: 912-927.
34	郭亮, 焦纬洲, 刘有智, 等. 不同臭氧组合工艺处理含硝基苯类化合物废水的实验研究[J]. 含能材料, 2014, 22(5): 702-708.
34	GUO Liang, JIAO Weizhou, LIU Youzhi, et al. Treatment of Nitrobenzene-containing wastewater using different combined processes with ozone[J]. Chinese Journal of Energetic Materials, 2014, 22(5): 702-708.
35	JIAO Weizhou, YU Lisheng, FENG Zhirong, et al. Optimization of nitrobenzene wastewater treatment with O₃/H₂O₂ in a rotating packed bed using response surface methodology[J]. Desalination and Water Treatment, 2016, 57(42): 19996-20004.
36	AROWO M. 超重力强化技术在基于臭氧氧化工艺处理邻苯二胺废水中的应用[D]. 北京: 北京化工大学, 2017.
36	AROWO M. Higee process intensification and application in treatment of o-phenylenediamine by ozone-based oxidation processes[D]. Beijing: Beijing University of Chemical Technology, 2017.
37	JIAO Weizhou, LIU Youzhi, LIU Wenli, et al. Degradation of nitrobenzene-containing wastewater with O₃ and H₂O₂ by high gravity technology[J]. China Petroleum Processing & Petrochemical Technology, 2013, 15(1): 85-94.
38	梁晓贤. 超重力均相催化臭氧法处理黑索今废水的研究[D]. 太原: 中北大学, 2013.
38	LIANG Xiaoxian. Study on RDX-containing wastewater treatment by homogeneous catalytic ozonation in rotating packed bed[D]. Taiyuan: North University of China, 2013.
39	QIN Yuejiao, LUO Shuai, GENG Shuo, et al. Degradation and mineralization of aniline by O₃/Fenton process enhanced using high-gravity technology[J]. Chinese Journal of Chemical Engineering, 2018, 26(7): 8-14.
40	ZENG Zequan, ZOU Haikui, LI Xin, et al. Degradation of phenol by ozone in the presence of Fenton reagent in a rotating packed bed[J]. Chemical Engineering Journal, 2013, 229: 404-411.
41	WEI Qing, QIAO Shufeng, SUN Baochang, et al. Study on the treatment of simulated coking wastewater by O₃ and O₃/Fenton processes in a rotating packed bed[J]. RSC Advances, 2015, 5(113): 93386-93393.
42	李振兴, 刘有智, 焦纬洲, 等. 旋转填料床强化Fenton试剂处理DNT废水实验研究[J]. 火工品, 2012(1): 48-52.
42	LI Zhenxing, LIU Youzhi, JIAO Weizhou, et al. Experimental study on Fenton reagent treating DNT wastewater intensified by rotating packed bed[J]. Initiators & Pyrotechnics, 2012(1): 48-52.
43	王丹. 超重力强化高级氧化法处理实际废水的研究[D]. 北京: 北京化工大学, 2017.
43	WANG Dan. Reserch on treatment of effluents with advanced oxidation processes intensified by rotating packed bed[D]. Beijing: Beijing University of Chemical Technology, 2017.
44	王永红. 超重力均相催化臭氧化降解酸性硝基苯废水[D]. 太原: 中北大学, 2017.
44	WANG Yonghong. Homogeneous catalytic ozonation for degradation of acid nitrobenzene wastewater in rotating packed bed[D]. Taiyuan: North University of China, 2017.
45	冯杰. 超重力强化高铁酸盐与臭氧协同处理有机废水[D]. 北京: 北京化工大学, 2015.
45	FENG Jie. Treatment of organic wastewater by Fe(Ⅵ) and ozone with the process intensified by high gravity technology[D]. Beijing: Beijing University of Chemical Technology, 2015.
46	杨鹏飞, 刘瑛, 焦纬洲, 等. 超重力环境下O₃/Fenton法处理含硝基苯废水[J]. 过程工程学报, 2018, 18(4): 728-734.
46	YANG Pengfei, LIU Ying, JIAO Weizhou, et al. Treatment of nitrobenzene-containing wastewater by O₃/Fenton in high gravity[J]. The Chinese Journal of Process Engineering, 2018, 18(4): 728-734.
47	LI Mo, ZENG Zequan, LI Yingwen, et al. Treatment of amoxicillin by O₃/Fenton process in a rotating packed bed[J]. Journal of Environmental Management, 2015, 150: 404-411.
48	邢天辰. 超重力环境下利用高级氧化技术处理酸性黄23印染废水的研究[D]. 北京: 北京化工大学, 2016.
48	XING Tianchen. Study on degradation of simulated dyeing wastewater with advanced oxidation processes intensified by rotating packed bed[D]. Beijing: Beijing University of Chemical Technology, 2016.
49	田力剑, 邢天辰, 陈建峰, 等. 旋转填充床中O₃/Fenton工艺处理聚丙烯酰胺污水的研究[J]. 化学反应工程与工艺, 2016, 32(1): 83-88.
49	TIAN Lijian, XING Tianchen, CHEN Jianfeng, et al. Treatment of polyacrylamide wastewater by O₃/Fenton process in a rotating packed bed[J]. Chemical Reaction Engineering and Technology, 2016, 32(1): 83-88.
50	AMR S S A, AZIZ H A, ADLAN M N, et al. Pretreatment of stabilized leachate using ozone/persulfate oxidation process[J]. Chemical Engineering Journal, 2013, 221: 492-499.
51	QIAO Jingjuan, LUO Shuai, YANG Peizhen, et al. Degradation of nitrobenzene-containing wastewater by ozone/persulfate oxidation process in a rotating packed bed[J]. Journal of the Taiwan Institute of Chemical Engineers, 2019, 99: 1-8.
52	GE Deming, ZENG Zequan, AROWO M, et al. Degradation of methyl orange by ozone in the presence of ferrous and persulfate ions in a rotating packed bed[J]. Chemosphere, 2016, 146: 413-418.
53	CHANG Chia-Chi, CHIU Chun-Yu, CHANG Ching-Yuan, et al. Pt-catalyzed ozonation of aqueous phenol solution using high-gravity rotating packed bed[J]. Journal of Hazardous Materials, 2009, 168(2/3): 649-655.
54	CHANG Chia-Chi, CHIU Chun-Yu, CHANG Ching-Yuan, et al. Combined photolysis and catalytic ozonation of dimethyl phthalate in a high-gravity rotating packed bed[J]. Journal of Hazardous Materials, 2009, 161(1): 287-293.
55	WEI Xingyue, SHAO Shengjuan, DING Xin, et al. Degradation of phenol with heterogeneous catalytic ozonation enhanced by high gravity technology[J]. Journal of Cleaner Production, 2020, 248: 119179.
56	刘有智. 超重力化工过程与技术[M]. 北京: 国防工业出版社, 2009.
56	LIU Youzhi. Chemical engineering process and technology in high gravity[M]. Beijing: National Defense Industry Press, 2009.

[1]	王云飞, 秦蕊, 郑利军, 李焱, 李清平. 旋转填充床CFD模拟研究进展[J]. 化工进展, 2023, 42(S1): 1-9.
[2]	盛维武, 程永攀, 陈强, 李小婷, 魏嘉, 李琳鸽, 陈险峰. 微气泡和微液滴双强化脱硫反应器操作分析[J]. 化工进展, 2023, 42(S1): 142-147.
[3]	黄益平, 李婷, 郑龙云, 戚傲, 陈政霖, 史天昊, 张新宇, 郭凯, 胡猛, 倪泽雨, 刘辉, 夏苗, 主凯, 刘春江. 三级环流反应器中气液流动与传质规律[J]. 化工进展, 2023, 42(S1): 175-188.
[4]	杨寒月, 孔令真, 陈家庆, 孙欢, 宋家恺, 王思诚, 孔标. 微气泡型下向流管式气液接触器脱碳性能[J]. 化工进展, 2023, 42(S1): 197-204.
[5]	陈匡胤, 李蕊兰, 童杨, 沈建华. 质子交换膜燃料电池气体扩散层结构与设计研究进展[J]. 化工进展, 2023, 42(S1): 246-259.
[6]	高雨飞, 鲁金凤. 非均相催化臭氧氧化作用机理研究进展[J]. 化工进展, 2023, 42(S1): 430-438.
[7]	许春树, 姚庆达, 梁永贤, 周华龙. 共价有机框架材料功能化策略及其对Hg(Ⅱ)和Cr(Ⅵ)的吸附性能研究进展[J]. 化工进展, 2023, 42(S1): 461-478.
[8]	赵景超, 谭明. 表面活性剂对电渗析减量化工业含盐废水的影响[J]. 化工进展, 2023, 42(S1): 529-535.
[9]	邵博识, 谭宏博. 锯齿波纹板对挥发性有机物低温脱除过程强化模拟分析[J]. 化工进展, 2023, 42(S1): 84-93.
[10]	王晨, 白浩良, 康雪. 大功率UV-LED散热与纳米TiO₂光催化酸性红26耦合系统性能[J]. 化工进展, 2023, 42(9): 4905-4916.
[11]	白志华, 张军. 二乙烯三胺五亚甲基膦酸/Fenton体系氧化脱除NO[J]. 化工进展, 2023, 42(9): 4967-4973.
[12]	王琦, 寇丽红, 王冠宇, 王吉坤, 刘敏, 李兰廷, 王昊. 焦化废水生物出水中可溶解性有机物的分子识别[J]. 化工进展, 2023, 42(9): 4984-4993.
[13]	史天茜, 石永辉, 武新颖, 张益豪, 秦哲, 赵春霞, 路达. Fe²⁺对厌氧氨氧化EGSB反应器运行性能的影响[J]. 化工进展, 2023, 42(9): 5003-5010.
[14]	张智琛, 朱云峰, 成卫戍, 马守涛, 姜杰, 孙冰, 周子辰, 徐伟. 高压聚乙烯失控分解研究进展：反应机理、引发体系与模型[J]. 化工进展, 2023, 42(8): 3979-3989.
[15]	李洞, 王倩倩, 张亮, 李俊, 付乾, 朱恂, 廖强. 非水系纳米流体热再生液流电池串联堆性能特性[J]. 化工进展, 2023, 42(8): 4238-4246.