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.     

介质阻挡放电降解乙酸异丁酯气体

采用介质阻挡放电(DBD)降解模拟乙酸异丁酯(IA)气体,结果表明:当ρ(IA)为1 788 mg/m3,气体流速为1.8 m/s,外施电压为9.0 kV时,IA去除率达75.3%. 外施电压升高,初始ρ(IA)和气体流速下降,IA去除率升高. 放电间隙对DBD降解IA废气也会产生一定的影响. 能率与气体流速无线性关系,为了得到较高的能率,外施电压应调节至7.5和9.0 kV. 考察了DBD降解实际IA工业废气的效果、费用和可行性,结果表明:废气量为2 000 m3/h,DBD反应管中的气体流速为5.4 m/s,单个DBD电源输入电压为16 kV时,IA去除率达80%以上,单位体积IA废气的处理费用为0.012元/m3. 对DBD降解IA的产物进行了分析,并初步探讨了降解机理.      

介质阻挡放电降解异味物质CS_2研究

采用介质阻挡放电降解二硫化碳(CS2)模拟废气,考察了外加气体空气、氮气(N2)、电源输入功率、初始浓度和停留时间对CS2转化率的影响。结果表明:CS2的去除率呈现空气>N2。在输入功率63 W,停留时间为5.34 s,CS2的初始浓度300 mg/m3,N2氛围下的去除效率为36.9%,而空气氛围下的去除效率可达62.5%。在N2与空气氛围下其产物明显不同,在空气氛围下,主要产物为SO2、COS、CO和CO2;而在N2氛围下其主要产物为大量单质硫、少量CO与CO2。对DBD降解CS2的机理分析表明,在N2条件下主要是高能电子与紫外光的作用;而在有空气条件下,O2的存在促进了CS2的深度氧化。     

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.     

气相中甲苯的臭氧-光催化降解

初步研究了气相中中低浓度(10～80mg/m³)甲苯的臭氧-光催化联合降解,考察甲苯初始浓度、气体流量和湿度对降解效率及去除负荷的影响,并与单一光催化降解进行了比较.结果表明,臭氧-光催化对甲苯的降解效率大大高于光催化的降解效率,在较高浓度时效果更为显著;甲苯浓度在10～40mg/m³范围时,臭氧-光催化降解效率高达90%以上,但随甲苯初始浓度升高而缓慢地线性下降;湿度对甲苯的臭氧-光催化降解稍有影响,但去除率变化不超过2.5%.     

脉冲调制介质阻挡放电和催化联用技术降解甲苯

利用低温等离子体处理挥发性有机化合物(VOCs)废气是目前国内外研究的热点。研究利用脉冲调制介质阻挡放电和催化联用技术降解甲苯,对比分析了连续放电和脉冲调制对去除甲苯的影响;研究了脉冲调制后在有无催化剂的情况下的能量效率,比较了两种情况下的臭氧浓度以及中间产物的不同。结果表明:脉冲调制有效提高了甲苯的降解能效,其能量效率几乎是连续放电时的2倍～3倍;在有催化剂的情况下,能量效率是没催化剂的1.5倍～2倍,臭氧浓度明显降低,结焦产物中含苯环的衍生物的量少于无催化的结焦产物。     

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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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.     

UV254nm+185nm光照降解气态甲苯的实验研究

研究了波长为254nm+185nm紫外光照射下,甲苯初始浓度、停留时间、相对湿度、O2浓度等因素对甲苯光降解效率的影响.通过定量UV254nm+185nm光照下体系中O3的产生浓度变化,以及降解过程中中间产物苯和苯甲醛的变化趋势,讨论了甲苯在UV254nm+185nm照射下降解机理.结果表明,甲苯去除率随着O2含量、停留时间的增加而升高;随着初始浓度的增加而降低.与湿度的关系为先急剧升高然后缓慢增加,而后降低,最佳相对湿度在40%~50%.当甲苯初始浓度为16.1mg/m3,O2含量为20%,相对湿度为40%时,体系对甲苯的降解效率为82.2%,降解速率为0.44mg/(m3·s),产生的O3浓度为131.13mg/m3,中间产物苯和苯甲醛的浓度分别为0.086,0.135mg/m3.在反应体系中,甲苯可吸收185nm波长紫外光直接降解,但主要被体系中产生的自由基氧化降解.     

介质阻挡放电降解苯乙烯的研究

研究了介质阻挡放电(DBD)常压下降解流动态苯乙烯时,不同电压、流速、初始浓度及湿度下苯乙烯的降解情况.结果表明,DBD降解苯乙烯15~20min即可达稳定,产物主要为CO、CO₂和H₂O;电压4800V时有少量带苯环的气态及固态物质产生,且随电压的升高而减少,到7500V时红外光谱已无法检测到;高电压下放电可以取得90%左右的降解率,产生带苯环的气态物质和结焦物质较少.流速在1.5cm/s,浓度为3000mg/m³,相对湿度为20%左右时,降解效果最好.     

介质阻挡放电去除NO的实验研究

设计了一套高压电源和同轴圆柱 -筒介质阻挡放电反应器装置 ,进行了冷等离子体去除NO的实验研究 ,结果表明该方法是有效的 .研究了气体流量、NO初始浓度、放电电压、O2 含量以及中心电极尺寸对NO去除效率的影响 .当流量较小或NO初始浓度较低时 ,有较高的去除率 ;流量变大和NO初始浓度增加时 ,NO的去除率将下降 .放电电压升高 ,NO去除率将增大 .O2 的存在会降低NO的去除率 .放电管其它特征尺寸给定条件下 ,中心电极存在一个最佳直径 ,使得NO的去除效果最为理想 .     

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.     

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.     

类芬顿试剂液相氧化法脱硝的实验研究

以类芬顿试剂(H2O2/Fe3+/UV)液相氧化法脱硝,探讨了液相催化和类芬顿脱硝反应的机理及其关系.研究了H2O2浓度、[H2O2]/[Fe3+]、初始pH值、气体流量、紫外光和H2O2投加方式对NO去除率的影响.结果表明,脱硝效率随H2O2浓度增加而升高;H2O2浓度一定时,Fe3+浓度的增加有利于NO的脱除,[H2O2]/[Fe3+]=6时,脱硝效率最高;当初始pH值3时,pH值升高,脱硝效率下降,初始pH值为3时脱硝效果最好;NO去除率随气体流量的增加而下降;紫外光的照射能提高脱硝效率;分3次等量投加H2O2可以使脱硝效率维持在80%左右.     

针-板式介质阻挡放电降解土壤中对硝基苯酚研究

采用针-板式介质阻挡放电(DBD)产生低温等离子体降解土壤中对硝基苯酚(PNP),考察了放电电压、载气气量、土壤含水率以及土壤pH值对土壤中PNP降解效果的影响。结果表明:针-板式DBD对土壤中PNP有良好的降解效果。在PNP初始浓度400mg/kg,放电电压18 kV条件下,放电处理60 min,PNP降解率达到87.3%。增加放电电压和含水率均能提高降解率。不通入载气,也有较好的降解效果。碱性条件有利于PNP降解。     

介质阻挡等离子体放电与催化联用技术分解苯

采用介质阻挡等离子体放电与催化剂MnO₂联用技术对苯去除进行了研究.结果表明,加入MnO₂可充分利用O₂和产生于介质阻挡等离子放电区的O₃,能够增加苯氧化分解为CO₂的程度,且苯去除的能量效率是不用催化剂时的2倍.催化剂MnO₂苯去除率有显著影响.当能量密度低于564J/L时,MnO₂离放电区的距离越近,苯的去除效果越好;当能量密度高于1051J/L时,苯的去除效果与MnO₂离放电区的距离有关并有一个最佳值.阐述了苯在等离子体放电区以及MnO₂上的氧化机理.     

低温等离子体降解污染土壤热脱附尾气中DDTs

为优化低温等离子体技术对污染土壤热脱附尾气的处理效果,采用脉冲电晕放电等离子体处理含DDTs（滴滴涕）的热脱附尾气,控制进气中的ρ（DDTs）为2.873 mg/m3,考察了载气φ（O₂）、等离子体温度、载气湿度和脉冲电压对DDTs降解效果的影响,分析了O₃在降解过程中的作用.结果表明:①当氮气/氧气混合载气中φ（O₂）分别为0、3%、6%、10%、21%和100%时,DDTs降解率分别为80.1%、76.5%、78.4%、81.1%、88.8%和94.6%,ρ（O₃）分别为0、0.20、0.25、0.40、0.99和1.93 mg/L.随着φ（O₂）的增加,ρ（O₃）逐渐增大,除氮气气氛外,DDTs降解率均逐渐增大,当φ（O₂）超过10%时,DDTs降解率较氮气气氛下更高.p,p'-DDD降解率均为100%,p,p'-DDE和o,p'-DDT的降解率随φ（O₂）的增加而增大.氮气气氛下p,p'-DDT降解率高于低浓度氧气气氛,除氮气气氛外,p,p'-DDT降解率随φ（O₂）的增加而增大.②当等离子体温度分别为80、100和150 ℃时,DDTs降解率分别为88.8%、83.2%和56.3%,ρ（O₃）分别为0.99、0.65和0.35 mg/L.当载气湿度为0、1.0、2.7和20.5 g/m3时,DDTs降解率分别为88.8%、81.6%、68.6%和30.0%,ρ（O₃）分别为0.99、0.73、0.56和0.32 mg/L.随着等离子体温度升高、载气湿度增大,反应器内ρ（O₃）逐渐减小,DDTs降解率也随之降低.③DDTs降解率随脉冲电压的升高而增大,当脉冲电压为24 kV、脉冲频率为50 Hz、等离子体温度为80 ℃、气体在反应器中的停留时间为10 s时,DDTs降解率达86.9%.研究显示,脉冲电晕放电等离子体能够快速、有效地去除热脱附尾气中的DDTs.      

介质阻挡放电脱除模拟工业苯系物的可行性

采用介质阻挡放电(DBD)技术降解流动态"三苯"(苯、甲苯和二甲苯)模拟废气,分析了浓度、气体流速对其降解的影响.对混合"三苯"废气进行单级和串联运行中试放大试验研究,结果显示,DBD串联可以在一定程度上提高"三苯"的去除率.三级申联时三种气体去除率都达到89%以上,对"三苯"混合废气单位体积处理费用进行了估算,结果表明,单级运行时1000m3废气处理费用只需1～3元.最后指出,要真正实现DBD降解苯系物工业化,首先要解决的还是管壁结焦和出流气体中的气溶胶粒子问题.     

Formaldehyde degradation by UV/TiO2/O3process using continuous flow mode

The degradation of formaldehyde gas was studied using UV/TiO2/O3 process under the condition of continuous flow mode. The effects of humidity, initial formaldehyde concentration, residence time and ozone adding amount on degradation of formaldehyde gas were investigated. The experimental results indicated that the combination of ozonation with photocatalytic oxidation on the degradation of formaldehyde showed a synergetic action, e.g,, it could considerably increase decomposing of formaldehyde. The degradation efficiency of formaldehyde was between 73.6% and 79.4% while the initial concentration in the range of 1.84--24 mg/m^3 by O3/TiO2flJV process. The optimal humidity was about 50% in UV/TiO2/O3 processs and degradation of formaldehyde increases from 39.0% to 94.1% when the ozone content increased from 0 to 141 mg/m^3. Furthermore, the kinetics of formaldehyde degradation reaction could be described by Langmuir-Hinshelwood model. The rate constant k of 46.72 mg/（m^3.min） and Langmuir adsorption coefficient K of 0.0268 m^3/mg were obtained.