非平衡等离子体联合技术降解甲苯气体

采用了自制的纳米钛酸钡基介电材料作为催化剂,以电工陶瓷拉西环作为载体,利用介质阻挡放电产生的非平衡态等离子体对常压下流动态含甲苯的空气进行处理,研究了电场强度、流速、初始浓度及不同填料情况下甲苯的降解及臭氧产生情况,初步探讨了等离子体催化降解甲苯的机理,并进行了产物分析.实验结果表明,电场强度小于13kV·cm-1时,甲苯降解率和臭氧产生浓度随电场强度的提高而上升,随气速和初始浓度的增加而降低;不同填料下降解率及臭氧浓度由大到小排序为有催化剂填料、普通填料、无填料,有催化剂存在时(电场强度为14kV·cm-1,流速为0.3 m3·h-1,甲苯浓度为600 mg·L-1),甲苯降解率最高可达95%.当电场强度>13kV·cm-1时,臭氧浓度因受到过量的高能电子攻击而发生分解.表现为臭氧浓度随电场强度的继续增加而降低.因此,电场强度为13kV·cm-1时,产生的臭氧浓度最高.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NOx) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition, NOx was suppressed with the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NOx suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NO_x) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition,NO_xwas suppressedwith the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NO_x suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

外置式联合等离子体光解技术去除苯乙烯气体

开发了用一个高压电源同时产生等离子体和KrI* 准分子紫外辐射的外置式联合等离子体光解(Outer Combined Plasma Photolysis, OCPP)技术,并用于降解模拟流动态苯乙烯气体. 结果表明:在Kr和I₂充入量分别为26.60 kPa和6 mg, 气体流速为3.26 m3/h, 初始ρ(苯乙烯)为1 265 mg/m3,外施电压为9.0 kV的条件下,苯乙烯的去除率达84.4%;与介质阻挡放电技术相比,苯乙烯的去除率提高了20.6%,能率提高了5.7 g/(kW·h). 同时,研究了OCPP技术降解苯乙烯的影响因素,包括Kr和I₂的充入量、石英材质、气体流速、初始ρ(苯乙烯)及反应器结构. 采用红外光谱仪和气质联用仪分析了结焦产物,探讨了OCPP技术降解苯乙烯的机理.      

介质阻挡放电等离子协同TiO_2-GAC降解甲基橙的研究

采用介质阻挡放电(DBD)等离子协同颗粒活性炭负载TiO2(TiO2-GAC)对甲基橙进行降解,研究了该体系的协同处理效果,探讨了放电电压、初始pH、初始电导率、初始浓度和TiO2-GAC投加量等操作参数的影响,并建立了协同体系的表观反应动力学模型.实验结果表明,DBD与TiO2-GAC联合处理表现出明显的协同效应,处理25min后,协同体系对甲基橙的降解率和COD去除率分别为96.2%和90%,与单独DBD体系相比,分别提高了52.7%和50.4%;协同体系降解甲基橙的过程符合表观反应动力学模型,模型值与实验值吻合良好,总级数为2.352;体系中H2O2、O3浓度测定结果表明,与单独DBD体系对比,协同体系的H2O2浓度增高,而O3浓度降低,说明TiO2-GAC起到了催化作用;TiO2-GAC在DBD体系中获得了原位再生,五次再生循环后再生率达80%.     

Decomposition of gaseous CF2CIBr by cold plasma method

The paper presented the results regarding the decomposition of gaseous CF₂ClBr by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF₂ClBr pure and 2660 Pa CF₂ClBr plus 7980 Pa O₂ reached 60% and 80%,respectively.The paper also studied the cold plasma gas phase chemistry reaction mechanism of CF₂ClBr at low pressure,and the pressure effects of CF₂ClBr and added gas(He,N₂,O₂ and dry air)on the CF₂ClBr decomposition respectively by cold plasma method.These studies will be helpful to application of cold plasma method in the treatment of hazardous gaseous wastes.     

Destruction of VOCs by combination of corona discharge and catalysis techniques

The catalytic effect of alumina on the destruction of toluene, benzene, acetone and methanol, in DC pulsed corona discharge reactor was studied. In the presence of alumina the inlet concentration of the VOCs was varied from 5 x 10-6 mol/L to 80% x 10-6 mol/L, and their decomposition efficiency (conversion %) was found to be 99%-80% for toluene, 99%-97% for benzene, 95%-92% for acetone, and 72%-85% for methanol. Corresponding decomposition in the absence of alumina was 90%-38% for toluene, 89%-57% forbenzene, 42%-30% for acetone, and 47%-19% for methanol. Feed gas flow rate was 400 cm3/min and power reading from DC source was 7.4 W in all of the experiments. Alumina also shifted the CO/CO2 ratio in the by-products in favor of CO2. Ozone concentration at the reactor outlet was higher in the presence of alumina. Enhancement in VOCs decomposition by alumina was explained on the basis of higher concentration of ozone and its precursor atomic oxygen [O].Decomposition efficiency (conversion %) for individual compounds was found to be inversely proportional to the ionization potential of the compound, under identical conditions. Double DC high voltage sources pulse generator was tested and found to improve VOCs decomposition compared with the conventional single DC high voltage source.     

Destruction of VOCs by combination of corona discharge and catalysis techniques

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Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide(NOx) by-products were investigated in a dielectric barrier discharge(DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide(Mn Ox), iron oxide(Fe Ox), cobalt oxide(Co Ox) and copper oxide(Cu O), supported on Al2O3/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO2 selectivity. In addition, NOx was suppressed with the decrease of specific energy density(SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the Cu O catalyst showed the best performance in NOx suppression. The Mn Ox catalyst exhibited the lowest concentration of O3 and highest CO2 selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Decomposition of CF3CI by corona discharge

In this paper pulsed corona discharge is shown to be effective for the decomposition of CF₃Cl(Freon-13).The pressure of CF₃Cl was 2.67×10³Pa,after discharged for 2 min,39.5% of CF₃Cl was decomposed.The products were mainly CF₄,Cl₂ and CF₂Cl₂.The yield increased by adding O₂ or air.Under the same conditions,more than 94% decomposition yield was obtained if 5.32×10³Pa O₂ or air was added.The composition of products became CF₂O,Cl₂ and CF₄.While the partial pressure of O₂ or air reached 1 arm,the decomposition yield decreased to 54.5% and 48. 5% respectively.     

CF2ClBr的火花等离子体降解

对用等离子体降解ＣＦ２ＣｌＢｒ进行了初步研究,产物主要用气相色谱分析。在ＣＦ２ＣｌＢｒ的强为２．６７×１０＾３Ｐａ时获得了９０％左右的解离率,主要降解产为ＣＦ３Ｃｌ,Ｂｒ２,ＣＦ４,ＣＦ２Ｃｌ２。另外,从热力学上对产物进行了解释,得出了产总是朝使体系更稳定的方向生成的结论。     

低温等离子体降解哈隆类物质中的竞争反应

利用低温等离子体技术对哈隆类物质 CF₂ClBr和 CF₃Br进行了降解反应研究 ,发现无氧条件下某些降解产物的量随放电时间不同而出现波动 ,表明降解过程中存在竞争反应 ;而氧气过量条件下不存在竞争反应 ,其主要产物为 CF₂O等 .对低气压下 CF₂ClBr和 CF₃Br在低温等离子体空间中的气相反应机理进行讨论 ,为实现低温等离子体降解污染物提供了理论依据 .     

Efficient degradation of chlorobenzene in a non-thermal plasma catalytic reactor supported on CeO2/HZSM-5 catalysts

Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO₂/HZSM-5 catalysts. The performance of catalysts was evaluated in terms of removal and energy efficiency. The decomposition products of chlorobenzene were analyzed. The results show that CeO₂/HZSM-5 exhibited a good catalytic activity, which resulted in enhancements of chlorobenzene removal, energy efficiency, and the formation of lower amounts of by-products. With regards to CO₂ selectivity, the presence of catalysts favors the oxidation of by-products, leading to a higher CO₂ selectivity. With respect to ozone, which is considered as an unavoidable by-product in air plasma reactors, a noticeable decrease in its concentration was observed in the presence of catalysts. Furthermore, the stability of the catalyst was investigated by analyzing the evolution of conversion in time. The experiment results indicated that CeO₂/HZSM-5 catalysts have excellent stability: chlorobenzene conversion only decreased from 78% to 60% after 75 hr, which means that the CeO₂/HZSM-5 suffered a slight deactivation. Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared (FT-IR) spectroscopy, scanning electron microscope (SEM) and energy dispersive X-ray spectroscopy (EDS) analyses of the catalyst before and after the reaction, revealing the cause of catalyst deactivation.     

Synergistic effects of non-thermal plasma-assisted catalyst and ultrasound on toluene removal

A wire-mesh catalyst coated by La_0.8Sr_0.2MnO₃ was combined with a dielectric barrier discharge (DBD) reactor for toluene removal at atmospheric pressure. It was found that toluene removal efficiency and carbon dioxide selectivity were enhanced in the catalytic packed-bed reactor. In addition, ozone and nitrogen monoxide from the gas effluent byproducts decreased. This is the first time that ultrasound combined with plasma has been used for toluene removal. A synergistic effect on toluene removal was observed in the plasma-assisted ultrasound system. At the same time, the system increased toluene conversion and reduced ozone emission.     

介质阻挡放电处理水中3,4-二氯苯胺机理研究

采用介质阻挡放电产生低温等离子体来处理水中3,4-二氯苯胺(3,4-DCA),考察了放电功率、空气流量、金属离子(Fe2+、Cu2+)浓度、光催化剂二氧化钛对3,4-DCA去除率的影响,并分析了降解产物及可能的降解机理.实验结果表明,介质阻挡放电方法对3,4-DCA有良好的去除效果,在3,4-DCA初始浓度为30mg·L-1,放电功率为80W,空气流量为1L·min-1时,放电处理6min后3,4-DCA的去除率可达92.5%.增加空气流量能显著地提高3,4-DCA的去除率,添加亚铁离子(Fe2+)浓度和光催化剂TiO2均能提高3,4-DCA的去除率,且存在最佳添加量值.介质阻挡放电方法对3,4-DCA的降解去除反应符合一级反应动力学.通过气质联用仪(GC-MS)分析检测发现,反应主要为脱氯、脱氨基和苯环开环反应,二氯乙烯为其主要的降解产物.     

Non-thermal plasma treatment of Radix aconiti wastewater generated by traditional Chinese medicine processing

The wastewater effluent from Radix aconiti processing, an important step in the production processes of traditional Chinese medicine (TCM), is a type of toxic wastewater and difficult to treat. Plasma oxidation methods have emerged as feasible techniques for effective decomposition of toxic organic pollutants. This study examined the performance of a plasma reactor operated in a dielectric barrier discharge (DBD) to degrade the effluent from R. aconiti processing. The effects of treatment time, discharge voltage, initial pH value and the feeding gas for the reactor on the degradation of this TCM wastewater were investigated. A bacterium bioluminescence assay was adopted in this study to test the toxicity of the TCM wastewater after non-thermal plasma treatment. The degradation ratio of the main toxic component was 87.77% after 60 min treatment with oxygen used as feed gas and it was 99.59% when the initial pH value was 8.0. High discharge voltage and alkaline solution environment were beneficial for improving the degradation ratio. The treatment process was found to be capable of reducing the toxicity of the wastewater to a low level or even render it non-toxic. These experimental results suggested that the DBD plasma method may be a competitive technology for primary decomposition of biologically undegradable toxic organic pollutants in TCM wastewater.     

等离子体场内CeO2催化降解甲醇的表面活性氧物种来源与作用研究

利用水热法制备了3种不同形貌(纳米棒、纳米颗粒、纳米立方体)的CeO_2催化剂,并通过比表面积测试(BET)、扫描电子显微镜(SEM)、拉曼光谱分析(Raman)、O_2程序升温脱附(O_2-TPD)手段表征其物理化学性质,结果发现,CeO_2纳米棒的表面氧空位和氧物种最多.等离子体与催化协同降解甲醇性能评价实验结果显示,CeO_2纳米棒展现出最好的催化性能.进一步设计实验(甲醇-TPD、不同气氛常温催化、催化剂内后置比较、O_3催化氧化)推测在等离子体场内CeO_2表面活性氧物种来源及其作用.结果表明:①在等离子体场内参与CeO_2表面催化反应的活性氧物种有两个来源,一是催化剂本身存在的表面氧物种,二是等离子体区域产生的短寿命物种及长寿命物种(主要是O_3),其中,O_3分解产生的活性氧物种是提高催化性能的主要因素.②不同形貌CeO_2由于表面氧空位含量不同,导致O_3在催化剂上分解产生的活性氧物种的量不同,最终影响等离子体催化性能.     

外加气体对等离子体降解CF2ClBr的影响

用等离子体处理难降解大气污染是近国内外产活跃的领域,选用化学方法难解的ＣＦ２ＣｌＢｒ为对象,研究了Ｈｅ,Ｎ２,Ｏ２及空气对等离子体降解ＣＦ２ＣｌＢｒ的影响,实现了ＣＦ２ＣｌＢｒ的常压降解,外加气体为Ｈｅ,Ｎ２时ＣＦ２ＣｌＢｒ的降解情况与纯ＣＦ２ＣｌＢｒ的降解基本相同,外加气体为Ｏ２,空气时的主要降解产物为ＣＦ２Ｏ,Ｂｒ２,Ｃｌ２,外加气体对降糖的影响大小Ｈｅ〈Ｎ２〈Ｏ２空气。     

介质阻挡放电降解流动态二甲基二硫废气

采用介质阻挡放电等离子体技术(Dielectric Barrier Discharge,DBD)处理常压下流动态气体中的有机硫恶臭气体二甲基二硫(Dimethyl Disulfide,DMDS).研究了不同停留时间、进气浓度及外施电压条件下DMDS的转化,推导了DBD处理DMDS的动力学模型,并根据傅立叶红外(FT-IR)产物分析探讨了反应机理.研究结果表明,DMDS降解产物主要为CO2、SO2和H2O.在停留时间0.067 s、外施电压7500 V、进气量8.4m3·h-1的条件下,进气浓度为80 mg·m-3 DMDS的降解率达到64.3%,体积降解比量为2.26×10-2L·s-1·W-1,绝对处理量达到430 mg·h-1.     

脉冲电晕法藕合Ca(OH)2固体吸收处理四氯乙烯废气研究

采用线-筒式脉冲电晕反应器对四氯乙烯去除效果进行了研究.结果表明,四氯乙烯去除率随电压的增大而增大.在氮气中加入氧气,四氯乙烯降解效果低于纯氮气下的降解效果.四氯乙烯在氮气下的主要气相产物为Cl_2和少量的CCl_4.当氧气加入后,四氯乙烯主要降解为CO_2、CO、COCl_2、O_3和C_2Cl_4O.为了去除有害中间产物,在反应器中加入Ca(OH)_2固体吸收剂,这明显提高了有害中间产物的去除,存在水汽及含Ca(OH)_2固体吸收剂时并未检测到COCl_2、O_3和有害中间产物C_2Cl_4O,但水汽不利于四氯乙烯去除.