低温等离子体作用下室内污染物甲醛的光催化去除实验研究
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摘要
甲醛是室内空气污染的主要组成部分,严重危害着人类的健康,而随着装修业的迅速发展,室内空气品质更成为人们关注的焦点。传统的各种空气净化方法都存在着各自的局限性,寻求传统空气净化技术的结合以克服彼此缺点来提高污染物的去除效果对于提高室内空气品质具有十分重要的意义。光催化技术在污染物浓度高,流速低的情况下能够有效地去除污染物,而对于室内污染物浓度低、需要快速达到净化要求的室内空气净化却难以满足;低温等离子体技术产生的高能粒子在可去除污染物的同时,能够激发催化剂,进而产生可与污染物作用的中间官能团,提高污染物的去除效果,但不足之处会有超过国标的臭氧产生。本文将两种净化技术相结合,克服过量臭氧产生的同时提高污染物处理量,为空气净化器的制作提供设计依据。
     本文在分析等离子体产生方式及产生机理的基础上,选择了直流电晕放电方式作为等离子体的产生方法,并根据直流电晕产生要求,制作了线-板、线-线、针-板三种产生等离子体的电极结构。通过实验对比表明线-板电极结构为直流电晕放电等离子体产生的最佳电极结构;
     在总结光催化技术与活性炭吸附技术相结合去除室内污染物研究的基础上,本文将低温等离子体技术与光催化技术和活性炭吸附技术相结合,通过实验探讨了湿度、流速、初始浓度等对单独低温等离子体、单独光催化、及结合作用对污染物甲醛去除的影响,并对比了三者作用时的处理量,结果表明结合技术可有效提高污染物甲醛的去除效果;
     鉴于结合作用对污染物去除量提高的有效性,本文将低温等离子体技术、光催化技术和活性炭吸附技术结合在一起,自制了一台用于小空间空气净化的小型空气净化器,通过实验分析了空气净化器对污染物甲醛的去除效果,结果发现,自制小型空气净化器对甲醛有较好的去除效果;
     由于低温等离子体在产生过程中,会有超过国标规定浓度的臭氧产生,本文通过实验分析了影响臭氧分解的外在因素,实验结果表明,活性炭的存在和纳米TiO_2的存在对于臭氧的分解能够发挥重要作用,对于密封空间会有聚集的过程,但通过在活性炭网上负载对臭氧分解能力更强的催化剂MnO_2即可有效抑制二次污染的产生。
Formaldehyde is the main pollutant in indoor air and seriously endangers human health. As decoration developes rapidly, indoor air quality (IAQ) has attracted lots of attention. Because of many limitations and shortcomings, traditional purification methods can’t be used in practice. Therefore, in order to improve indoor air quality, it becomes so significant to overcome the limitations and enhance pollutant removal efficiency by combining two or more kinds of traditional removal technologies. Photocatalysis technology can effectively remove pollutants while pollutant concentration is higher and flow rate is lower. By contraries, photocatalysis can’t work effectively. High-energy particles resulting from Non-thermal plasma (NTP) technology can removal pollutants and stimulate catalyst, but simultaneously ozone beyond GB will be created. This paper combines phototcatalysis technology and Non-thermal plasma technology to improve the removal efficiency and simultaneously avoid secondary pollution, which will be used as theory to make purifier.
     In this paper, basing on the method and the mechanism of generating plasma, DC corona discharge is chosen as the way to generating plasma. In accordance with the requirements of DC corona discharge, electrode structures of line-plate, line-line, and needle-plate are made. Experimental result shows that the line-plate electrode structure is the optimal structure for DC corona discharge yielding plasma;
     By applying photocatalysis with activated carbon adsorption technology, this paper combines non-thermal plasma technology and photocatalysis with actived carbon technology. Then exploring respectively the influence of humidity, flow rate, initial concentration on the plasma technology, the photocatalytic technology and the combinative technology removing formaldehyde, whts’s more, through contrasting the removal amount it can be concluded combinative technology plays an important role on enhancing the pollutants removal amount.
     In view of the combinative technology being significative, a pint-size purifier combining Non-thermal plasma technology and photocatalysis with actived carbon technology is made for small space. Experimental result shows that the purifier is efficient.
     During the process of generating plasma, there will be ozone beyond GB provisions. This paper analyzes the influence factors of ozone creating and decomposition during experiment. It can be got that the existence of activated carbon and the existence of nano-TiO_2 play an important role on the ozone decomposition. However, the process of aggregation for sealed space will result in ozone exceeding the GB, so it is necessary to utalize MnO_2 to avoid the emergence of secondary pollution. It can be concluded from experimental result that MnO_2 is effective in decomposing O3.
引文
1宋广生编.室内环境质量评价及检测手册[M].北京:机械工业出版社.2002
    2孙纲.室内主要污染物甲醛防治对策研究[J].环境科学与管理,2006.31(4):86-88
    3杨宝庭.大庆市居民室内空气中TVOC污染现状分析[J].环境科学与管理.2007,32(8):76-78
    4刘冬梅.家庭装修中室内环境污染的防治[J].光谱实验室.2006,23(4):869-871
    5曾耀辉.“绿色”室内环境与装潢污染[J].西昌学院学报.自然科学版.2006,20(3):41-43
    6王勇,刘志军.室内环境空气质量现状的分析与改善[J].质量管理与产品认证.2006,24(3):67-69
    7李涛,涂光备等.室内空气品质的改善及净化技术的应用[J].洁净与空调技术.2004,(3):7-11
    8张晓明,黄碧纯等.低温等离子体光催化净化空气污染物技术研究进展[J].化工进展.2005,24(9):964-967
    9 Holzer.F,Roland.U,F.-D.Kopinke.Combination of non-thermal plasma and heterogeneous catalysis for oxidation of volatile organic compounds [J].Applied Catalysis B:Environmental.2002,(38):163–181
    10 Huang Chen,Soo Wohn Lee,Tae Ho Kim Bo,et al.Photocatalytic decomposition of benzene with plasma sprayed TiO_2-based coatings on formed aluminum [J]. Journal of European Ceramic Society.2006,(26):2231-2239
    11余刚,姜效勤等.低温等离子体催化协同脱硝技术中若干问题探讨[J].洁净煤燃烧与发电技术.2004,(1):3-6
    12都基峻,季学李.低温等离子体处理气态污染物[J].污染防治技术.2000,13(1):33-34
    13吴碧君,刘晓勤.挥发性有机物污染控制技术研究进展[J].电力环境保护.2005,21(4):42-45
    14李文彩.用于光催化空气净化的催化剂成膜实验研究[D].北京:北京工业大学环境与能源工程学院.2006
    15盛建平.室内污染物甲醛、苯及苯系物的光催化去除实验研究[D].北京:北京工业大学环境与能源工程学院.2007
    16鹿院卫,李文彩,王伟等.活性炭与TiO_2相结合去除室内污染物甲醛的实验研究(I)[J].太阳能学报.2008,29(1):115-118
    17鹿院卫,李文彩,王伟等.活性炭与TiO_2相结合去除室内污染物甲醛的实验研究(II)[J].太阳能学报.2008,29(5):550-554
    18 Xingwang Zhang,Lecheng Lei,Jianling Zhang],et al. A novel CdS/S-TiO_2 nanotubes photocatalyst with high visible light activity [J].Separation and PurificationTechnology.2009,(66):417–421
    19 Yang Yang,Haiying Wang,Xiang Li,et al. Electrospun mesoporous W6+doped TiO_2 thin films for efficient visible-light photocatalysis[J].Materials Letters. 2009 (63):331–333
    20 Romana Khan,Tae-Jeong Kim.Preparation and application of visible-light- responsive Ni-doped and SnO_2-coupled TiO_2 nanocomposite photocatalysts[J].Journal of Hazardous Materials 2009. (163):1179–1184
    21 C.H.Ao,S.C.Lee.Enhancement effect of TiO_2 immobilized on activated carbon filter for the photodegradation of pollutants at typical indoor air level [J] . Applied CatalysisB: Environmental.2003,(44):191-205
    22 C.H.Ao,S.C.Lee.Combination effect of activated carbon with TiO_2 for the photodegradation of binary pollutants at typical indoor air level[J].Journal of photochemistry and photobiology,A:Chemistry.2004,(161):131-140
    23于竹芹,李坚,金毓峑.活性炭纤维负载TiO_2光催化降解甲醛研究[J].工业催化.2008,16(7):71-74
    24 M.E. Rinco′n,M.E.Trujillo-Camacho,A.K. Cuentas-Gallegos,etal.Surface characterization of nanostructured TiO_2 and carbon blackscomposites by dye adsorption and photoelectrochemical studies[J].Applied Catalysis B:Environmental.2006,(69):65–74
    25 Seoung-Hyun Kim,Huu Hao Ngo,H.K. Shon,etal.Adsorption and photocatalysis kinetics of herbicide onto titanium oxide and powdered activated carbon.Separation and Purification Technology.2008,(58):335–342
    26 Rusheng Yuan,Rongbo Guan,Jingtang Zheng.Effect of the pore size of TiO_2-loaded activated carbon fiber on its photocatalytic activity[J].Scripta Materialia.2005,(52): 1329–1334
    27 Pengyi Zhang,Fuyan Liang,Qing Chen,et al.A comparative study on decomposition of gaseous toluene by O3/UV,TiO_2/UV and O3/TiO_2/UV [J].Journal of photochemistry and photochemistry and photobiology A: Chemistry. 2003,(156) :189-194
    28 Kuo-Pin Yu,Grace W.M. Lee.Decomposition of gas-phase toluene by the combination of ozone and photocatalytic oxidation process (TiO_2/UV, TiO_2/UV/O_3,and UV/O3) [J].Applied Catalysis B: Environmental.2007,(75) :29–38
    29 Hong QI,De-zhi SUN,Guo-qing CHI.Formaldehyde degradation by UV/TiO_2/O_3 process using continuous ?ow mode [J].Journal of Environmental Sciences.2007 ,(19): 1136-1140
    30 Nobuya Hayashi,Tsutomu Yamakawaa,Seiji Baba.Effect of additive gases on synthesis of organic compounds from carbon dioxide using non-thermal plasma produced by atmospheric surface discharges[J].Vacuum.2006,(80) :1299–1304
    31 Subrahmanyam.Ch,Magureanu.M,Renken.A,et al.Catalytic abatement of volatile organiccompounds assisted by non-thermal plasma,Part 1.A novel dielectric barrier discharge reactor containing catalytic electrode[J].Applied Catalysis B: Environmental.2006,(65):150–156
    32 Subrahmanyam .Ch,Renken.A,Kiwi-Minsker.L,et al.Catalytic abatement of volatile organic compounds assisted by non-thermal plasma,Part II.Optimized catalytic electrode and operating conditions[J].Applied Catalysis B: Environmental.2006,(65):157–162
    33 Mista.W, Kacprzyk.R.Decomposition of toluene using non-thermal plasma reactor at room temperature [J].Catalysis Today.2008,(137) 345–349
    34胡平,孙春宝,丁德玲.脉冲电晕法去除甲苯废气的研究[J].安全与环境工程.2007,14(2):68-71
    35梁文俊,李坚等.低温等离子体法处理甲醛气体[J].环境污染治理技术与设备.2005,6(4):50-52
    36 Toshiaki Yamamoto,Kumar Ramanathan,Phil A. Lawless,et al.Control of volatile organic compounds by an ac energized ferroelectric pellet reactor and a pulse corona reactor.IEEE Transactions on Industry Applications.1992,28(3):528-534
    37梁文俊,李坚等.低温等离子体法去除苯和甲苯废气性能研究[J].环境污染治理技术与设备.2005,6(5):50-55
    38 Atsushi Ogata,Daisuke Ito,et al.Removal of Dilute Benzene Using a Zeolite-Hybrid Plasma Reactor [J].Transactions on Industry Applications.2001,37(4):959-964
    39 Atsushi Ogata,Kazushi Yamanouchi,et al.Decomposition of Benzene Using Alumina-Hybrid and Catalyst-Hybrid Plasma Reactors[J].Transactions on Industry Applications.1999,36(4):1289-1295
    40 Shigeru Futamura,Zhang Aihua,Hisahiro Einaga,etal.Involvement of catalyst materials in non-thermal plasma chemical processing of hazardous air pollutants [J] . Catalysis Today.2002,(7):259-265
    41 Shigeru Futamura.Synergistic effect of silent discharge plasma and catalysts on benzene decomposition [J].Catalysis Today.2004 (89):89-95
    42 Misook Kang,Bum-JoonKim,Sung M C,et al.Decomposition of toluene using an atmospheric pressure plasma/TiO_2 catalytic system[J].Journal of Molecular Catalysis Chemical.2002,(180):125-132
    43赵雷,周中平.低温等离子体技术净化空气中的甲苯[J].环境科学研究.2006,19(4):70-72
    44王惠敏,刘博.低温等离子体发生片替代纳米TiO_2催化光源的实验分析[J].青岛大学学报.2003,18(4):51-54
    45 Duan Li,Daisuke Yakushiji,Seiji Kanazawa,et al.Decomposition of Toluene by Using a Streamer Discharge Reactor Combined with Catalysts [J].Journal of Electrostatics.2002,(55):311-319
    46 BruceR Locke,Atsufumi Ichihashi,et al.Diesel Engine Exhaust Treatment with a PulsedStreamer Corona Reactor Equipped with Reticulated Vitreous Carbon Electrodes [J].Transactions on Industry Applications.2001,37(3):715-723
    47徐荣,王珊,梅凯.低温等离子体催化降解甲醛的实验研究[J].高电压技术.2007,33(2):178-181
    48王伟.光催化技术在室内污染控制中的应用研究[D].北京工业大学.2004
    49林跃宾.纳米TiO_2/ATP复合体的合成及其光催化去除有机污染物的研究[D].江苏大学.2007,5
    50林云琴,林和健,王德汉.低温等离子体技术及其在VOCs处理中的应用[J].城市环境与城市生态.2005,18(5):26-29
    51 Jim Van Durme,Jo Dewulf,Christophe Leys,etal.Combining non-thermal plasma with heterogeneous catalysis in waste gas treatment:A review[J].Applied Catalysis B:Environmental.2008,(78):324–33
    52张国兰,耿世彬,杜雁霞.低温等离子体去除室内空气污染物研究现状.建筑热能通风空调.2004,23(1):44-47
    53 Urashima.K,J S Chang.Removal of volatile organic compounds from airstreams and industrial flue gas by non-thermal plasma technology[J].IEEE Trans. Dielectr. Insult.2000,(7):602-614
    54 Thevenet.F,Guaitella.O,Puzenat.E,et al.Oxidation of acetylene by photocatalysis coupled with dielectric barrier discharge[J].Catalysis Today.2007 (122):186-194
    55 Hyun-Ha Kim,Hitomi Kobara,Atsushi Ogata,et al.Comparative Assessment of Different Nonthermal Plasma Reactions on Energy Efficiency and Aerosol Formation From the Decomposition of Gas-Phase Benzene[J].Transactions on industry applications.2005,41(1):206-214
    56蔡忆昔,刘志楠,赵卫东等.介质阻挡放电特性及其影响因素[J].江苏大学学报.2005,26(6):476-479
    57常净宜.纳米TiO_2催化剂协同非平衡等离子体去除室内空气中苯的实验研TiO_2[D].重庆大学城市建设与环境工程学院.2007
    58周泽存沈其工方瑜等编.高压电技术[M].中国电力出版社.2007
    59彭国贤编著.气体放电——等离子体物理的应用[M].知识出版社.1988
    60沈丽,白敏的,白希尧.强电离放电产生高浓度臭氧的实验研究[J].大连海事大学学报.2001,27(1):67-70
    61 Young Sun Mok,In-Sik Nam.Modeling of pulsed corona discharge process for the removal of nitric oxide and sulfur dioxide[J].Chemical Engineering Journal.2002,(85): 87–97
    62张元赏.直流电晕自由基簇射脱除室内污染物的试验研究[D].浙江大学.2006
    63 Hui-Xian Ding,Ai-Min Zhu,Xue-Feng Yang,et al.Removal of formaldehyde from gasstreams via packed-bed dielectric barrier discharge plasmas [J].Journal of physics D:Applied physics.2005,(38):4160–4167
    64 Andrei.A,Kulikovsky,Member.Production of Chemically Active Species in the Air by a Single Positive Streamer in a Nonuniform Field[J].Trans on Plasma Science.1997,25(3):439-446
    65王运武,《有机化学》[M].高等教育出版社.1993
    66周飞,杨学昌,高得力.等离子体TiO_2催化空气净化试验研究[J].清华大学学报(自然科学版).2007,47(4):10-13
    67 GB/T18883-2002,室内空气质量标准.国家卫生部.2002.
    68陈烈贤.室内空气净化技术及其性能评价方法[J].中国环境卫生,2002,5(1):219-233
    69 Ru-Bao Sun,Zhu-Ge Xi.Decomposition of low-concentration gas-phase toluene using plasma-driven photocatalyst reactor[J].Atmospheric environmental 2007,(41):6853-6859
    70 Mista.W, Kacprzyk.R.Decomposition of toluene using non-thermal plasma reactor at room temperature[J].Catalysis Today.2008,(137):345–349
    71徐雪成.空气相对湿度对高压电机线圈电晕起始电压的影响的试验研究[J].大电机技术.1994,(8):27-31
    72 Obee T N,Hay S O.Effects of Moisture and Temperature on the Photooxidation of Ethylene on Titania[J].Sci.Technol.1997,(31):2034-2038
    73 Noguchi.T,Fujishima.A,Sawunytama.P,et al.Photocatalytic Degradation of Gaseous Formaldehyde Using TiO_2 Film[J] . Environmental Science and Technology . 1998 ,(32):3831-3833
    74李玉华,王琨,赵庆良等.球载纳米TiO_2光催化氧化低质量浓度甲醛[J].化学工程.2009,37(1):37-40
    75杨瑞.纳米光催化降解VOCs研究[D].清华大学.2005
    76朱孟府,王海燕,宿红波等.便携式臭氧空气净化器的研制[J].医疗卫生装备.2008,29(1):9-10
    77李靖平,王磊,陈敬润等.臭氧在循环冷却水处理中的杀菌作用[J].腐蚀与防护.2008, 29(12):768-773
    78 Hisahiro Einaga, Atsushi Ogata.Benzene oxidation with ozone over supported manganese oxide catalysts: Effect of catalyst support and reaction conditions[J].Journal of Hazardous Materials].2009, (164):1236–1241
    79朱小平,张勤.一种用于电晕放电式臭氧发生器时高压直流开关电源设计[J].电源技术.2006,(2):69-70
    80姚河清,朱天宇,卞新高等.电晕放电式臭氧发生器工作原理的探讨[J].高压电器.2002,38(6):28-30
    81 Li R.N,Liu.X.Main fundamental gas reaction in renitrification and desulfurization from flue gas by non-thermal plasmas[J].Chemical Engineering Science.2000,(55):2491-2506
    82 Kim J G.Ozone as antimicrobial agent in minimally processed food [D].Columbus,Ohio:Ohio State University.1998
    83石志平,王文生.相对湿度变化对臭氧分解速率的影响[J].前沿科技.2004,(6):24-25
    84谈智,顾健,徐燕.相对湿度对空气臭氧消毒效果影响的试验观察[J].中国消毒学杂志.1999,16(4):240-241
    85钟理,张浩,陈英等.臭氧在水中的自分解动力学及反应机理[J].华南理工大学学报.2002,30(2):83-86
    86印红玲,谢家理,杨庆良等.臭氧在金属氧化物上的分解机理[J].化学研究与应用.2003,15(1):1-5
    87周国富,王富生,谢超.一种智能型电梯纳米光催化空气净化器的设计[J].机电工程技术.2008,37(7):54-55
    88张妍,李振海.室内空气净化器性能指标的探讨[J].环境与健康杂志.2007,24(6): 453-455
    89 GB/T18801-2002空气净化器[S].国家质量监督检验检疫总局.2003
    90 ANSI—AHAM AC-1-2000. Association of home appliance manufacture method for measuring perforance of portable household electric cord—connected room air cleaners [S]
    91张华山,李官贤,刘焕亮等.低温等离子体净化器产生的O3及其变化规律[J].中国公共卫生.2005,21(3):307-308
    92 GB/T18883-2002室内空气质量标准[S].国家质量监督检验检疫总局.2003
    93 Van Durme.J,Dewulf.J,Demeestere.K,et al. Post-plasma catalytic technology for the removal of toluene from indoor air:Effect of humidity.Applied Catalysis B: Environmental.2009,(87):78–83

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