介质阻挡放电离子源质谱分析

敞开式离子化质谱可对表面样品进行直接快速分析而受到关注,成为质谱分析的热点研究方向.介质阻挡放电离子源是一种基于等离子体放电机理的敞开式离子源,近年来得到了较快的发展.本文着重介绍该离子源的基本原理、性能特征以及应用进展,并对其发展趋势进行了展望.     

基于新型介质阻挡放电离子源的药物快速检测方法研究

本研究将单电极放电技术的DBDI与质谱(MS)联用,快速检测了4种低极性的合成药物,结果表明,4种合成药物主要生成[M+H]+分子离子.此外还利用DBDI-MS对草乌、制草乌切片进行快速分析,在草乌中检测到乌头碱、中乌头碱、脱氧乌头碱的[M+H]+离子,以及[M+H-60]+碎片离子;在制草乌中只检测到乌头碱、中乌头碱、脱氧乌头碱的[M+H-60]+碎片离子.所测草乌中的标志性药效成分主要为双酯类生物碱,制草乌中的标志性药效成分主要为单酯类生物碱.新型DBDI为药物研究提供了一种新的、快速检测方法,具有十分重要的理论和实际应用意义,在药物研究领域具有极大的应用潜力.     

高频介质阻挡放电烟气脱硫研究

采用高频介质阻挡放电的方式产生低温等离子体,研究在不加入NH₃的情况下流动态SO₂的去除情况.实验表明,在输入电压为12 kV,SO₂浓度为5400 mg/m³,气体流量为0.36 m³/h,相对湿度为55%时,脱硫率可达到70%以上;水气的存在对SO₂的去除有较大的促进作用,升高电压和增加O₂量对脱硫率的促进作用有限.对实验结果进行了解释,并提出了反应机理.     

介质阻挡放电-发射光谱测定偏二甲肼

基于气相色谱分离、低温等离子放电与发射光谱技术建立了偏二甲肼（UDMH）的测定方法。以介质阻挡放电（DBD）低温等离子体作为偏二甲肼的发射光谱（OES）激发源、DBD-OES微型发射光谱系统产生的384.94 nm特征光谱为检测信号,电荷耦合检测器（CCD）采集信号。仪器检出限为0.48μg/L;UDMH质量浓度为5μg/L时,相对标准偏差（RSD）为1.3%;环境水样的加标回收率为84%～90%。方法可应用于痕量偏二甲肼的检测和应急监测。     

甲烷二氧化碳介质阻挡放电转化产物分布研究

针对介质阻挡放电甲烷二氧化碳转化实验,分析了反应的产物分布,探讨了进料组成和反应器结构对反应的影响.反应产物包括:高H2/CO摩尔比的合成气、气态烃、高辛烷值的汽油组分、醇和酸等含氧有机物.对所述电极结构,产物的选择性随碳数增加而降低;高的甲烷进料浓度有利于烃的生成,对醇和酸的最佳甲烷进料体积分数范围在67.4％～75.1％;放电间隙越小,原料转化率和烃、酸的选择性越大,大的放电间隙对醇的生成有利.     

介质阻挡放电净化恶臭气体的实验研究

低温等离子体技术是一种新型的污染治理技术,国内外都对其进行了广泛而深入的研究。等离子体是电子,正、负离子,激发态原子、分子,以及自由基混杂的状态,是一种高反应活性的气体,理论上可以引发许多用常规方法难以发生的化学反应,已在废气、废水、固体废物以及放射性废物等方面     

介质阻挡放电引发氮氧化物等离子体化学反应

在523 K介质阻挡放电条件下,研究了不同气体组分体系中NO的转化.实验表明,在无氧体系(NO/N2)中,转化的NO主要分解为N2和O2.在富氧(NO/O2/N2)条件下,由于NO和NO2的生成, NO的转化率最低.体系中加入C2H4(NO/C2H4/N2)时, NO转化率与NO/N2体系几乎一样,与NO相比,生成的O更易与C2H4作用,几乎没有NO2的生成.当C2H4和O2共存时(NO/O2/C2H4/N2),NO主要被氧化为NO2.当能量密度为125 J•L－1时, 与其它体系相比,NO/O2/C2H4/N2体系中NO转化率和NO2生成量最大,转化每个 NO分子能耗最小(61 eV).体系中C2H4主要被氧化为CO.四个体系中N2O的生成量都较少.讨论了介质阻挡放电条件下上述四个体系可能的反应机制.     

介质阻挡放电脱除甲醛的化学动力学模拟

对大气压介质阻挡放电脱除甲醛进行了化学动力学模拟, 建立了时空平均化的模型, 并对相关的结果进行了实验验证. 分析了各主要物种的浓度随放电时间的变化, 在模拟空气气氛下, HCHO主要由O·和OH·自由基脱除, 其中, OH·自由基的作用更为突出. 强调了氮分子的第一电子激发态N2(A3∑+u)的作用, 它与O2、H2O 分子的碰撞增加了O·和OH·自由基的浓度,在氮气气氛中, N2(A3∑+u)态是使HCHO脱除的主要物种.讨论了HCHO初始浓度、气体流量对HCHO 脱除比能耗和产物中CO2/CO 摩尔比值的影响, HCHO 初始浓度较高时, 甲醛脱除的比能耗较低, 在输入能量密度<60 J·L-1, HCHO 初始浓度较低时, 产物中nCO2 /nCO值较高.     

单电极介质阻挡放电离子源的消电子技术研究

基于电场绝缘屏蔽技术的单电极介质阻挡放电离子源(DBDI),具有放电均匀、稳定、离子化能量高等优点,可实现对更大极性范围样品的快速检测。较高的离子化能量也增大了质谱图的背景噪声水平,对部分弱极性、低沸点样品的检测信噪比不高。本研究发展了基于单电极DBDI体系的外置电极消电子技术,探讨了外置针电极和外置金属网的消电子机理及其检测效果。结果表明,外置金属网消电子技术显著提高了部分弱极性样品的检测信噪比,异丙威、全氟辛酸、苏丹红Ⅲ的信噪比提升了5~6倍。基于该技术测定辣椒粉中苏丹红Ⅲ,回收率为83.7%~94.6%,相对标准偏差(RSD)为5.6%~9.0%,检出限为23 mg/kg,满足辣椒粉中苏丹红Ⅲ添加剂检测分析的要求。外置金属网消电子技术进一步提高了单电极DBDI对弱极性、低沸点、复杂样品的检测能力。     

基于大气压下介质阻挡放电抑制LA-ICP-MS分析中元素分馏效应研究

采用自制的大气压下介质阻挡放电装置串联在激光剥蚀池与ICP炬管之间, 对激光剥蚀产生的气溶胶进行预电离. 结果表明, 元素瞬时信号轮廓的平滑度得以改善, 元素分析信号精密度(RSD, n=3)可提高2.55％. 在ArF准分子激光(193 nm)和Nd∶YAG 固体激光(213 nm)两种不同波长的激光剥蚀系统中, 元素分馏因子均比常规模式下更接近于1, 表明采用介质阻挡放电对气溶胶预电离后元素分馏效应得以有效抑制. 相比两种不同波长的激光剥蚀系统, 介质阻挡放电对213 nm固体激光的元素分馏效应改善作用明显.     

A Brief Catalyst Study on Direct Methane Conversion Using a Dielectric Barrier Discharge

A series of metal catalysts was used for methane conversion to higher hydrocarbons and hydrogen in a dielectric barrier discharge. The main goal of this study is to identify the metal catalyst components which can influence the reactions in room‐temperature plasma conditions. The catalysts supported by γ‐Al₂O₃ and zeolite (ZSM 5x) were prepared by the incipient wetness method with solutions containing the metal ions of the second component. Among the catalysts tested, only Pt and Fe catalysts showed a unique result of catalytic reaction in a reactor bed packed with glass beads.     

Destruction of Styrene in an Air Stream by Packed Dielectric Barrier Discharge Reactors

This study presents the decomposition rates of styrene vapors with non-packed and packed bed dielectric barrier discharge reactors. The concentrations of intermediate byproducts at various plasma operation conditions were evaluated. The results showed that although styrene vapors could be almost completely removed at low styrene inlet concentration of 132 ppm, the selectivity of CO₂ as the major product was rather low in a non-packed bed reactor. It was found that solid carbon containing compound was the major byproduct. An increase in the styrene inlet concentration tended to reduce the styrene removal efficiency, it also led to increase in the solid byproduct. The reactors that packed with glass, Al₂O₃ or Pt–Pd /Al₂O₃ pellets could improve the styrene decomposition efficiency and reduce the formation of intermediate products, of which the best oxidation of styrene to CO₂ could be achieved with a Pt–Pd /Al₂O₃ packed bed reactor. The carbon byproducts could also be reduced if the rector length was increased. The concentrations of ozone formed during the plasma process were also evaluated for the non-packed and packed bed reactors. The plasma reactor that packed with Pt–Pd /Al₂O₃ pellets was proved to have the lowest O₃ concentration.     

Humidity Effect on Toluene Decomposition in a Wire-plate Dielectric Barrier Discharge Reactor

Laboratory-scale experiments were performed to evaluate the humidity effect on toluene decomposition by using a wire-plate dielectric barrier discharge (DBD) reactor at room temperature and atmospheric pressure. The toluene decomposition efficiency as well as the carbon dioxide selectivity with/without water in a gas stream of N₂ with 5% O₂ was investigated. Under the optimal humidity of 0.2% the characteristics of toluene decomposition in various background gas, including air, N₂ with 500 ppm O₂, and N₂ with 5% O₂ were observed. In addition, the influence of a catalyst on the decomposition was studied at selected humidities. It was found that the optimum toluene removal efficiency was achieved by the gas stream containing 0.2% H₂O, since the presence of water enhanced the CO₂ selectivity. In addition, the toluene removal efficiency increased significantly in a dry gas stream but decreased with an increase in the humidity when the Co₃O₄/Al₂O₃/nickel foam catalyst was introduced into the discharge area.     

Chlorinated Organic Compounds Decomposition in a Dielectric Barrier Discharge

The decomposition of chlorinated volatile organic compounds by non-thermal plasma generated in a dielectric barrier discharge was investigated. As model compounds trichloroethylene (TCE) and 1,2-dichloroethane (DCE) were chosen. It was found that TCE removal exceeds 95% for input energy densities above 0.2 eV/molecule, regardless of the initial concentration of TCE, in the range 100–750 ppm. On the other hand, DCE was more difficult to decompose, the removal rate reached a maximum of 60% at the highest input energy used. For both investigated compounds the selectivity towards carbon dioxide was significantly influenced by their initial concentration, increasing when low concentrations were used. The gas flow rate had also an effect on CO₂ selectivity, which is higher at low flow rate, due to the higher residence time of the gas in the plasma. The best values obtained in these experiments were around 80%.     

介质阻挡放电中OH自由基对甲醛脱除的影响

对管线式介质阻挡放电中的甲醛脱除进行了实验研究, 测量了介质阻挡放电产生的OH (A²Σ→X ²Π, 0-0)自由基发射光谱. 研究了在一个大气压下不同放电峰值电压、放电频率、添加氩气和氧气时甲醛脱除率与OH自由基发射光谱强度的变化关系. 实验结果表明: 在氮气含甲醛体系中, 提高放电峰值电压、放电频率和增大氩气含量时, 甲醛脱除率随OH (A²Σ→X ²Π, 0-0)自由基发射光谱强度的增强而提高; 当在氮气含甲醛体系中增大氧气含量时, 甲醛脱除率随OH (A²Σ→X ²Π, 0-0)自由基发射光谱强度的减弱而降低. 在11.5 kV放电峰值电压和9 kHz放电频率下, 氮气含甲醛体系中甲醛脱除率达93.8%.     

A New Approach to Metal Surface Nitriding Using Dielectric Barrier Discharge at Atmospheric Pressure

A new approach to metal surface nitriding using dielectric barrier discharge (DBD) plasma at atmospheric pressure is presented in this paper. Results of the study show that the plasma nitriding at atmospheric pressure using DBDs is realizable. Harder and thicker compound layer and diffusion layer on the treated surface has been formed in shorter treatment time comparing with the conventional vacuum plasma nitriding, Increasing the applied voltage will facilitate the formation of a thicker nitrided layer using the DBD. The nitrided layer acquired by this new approach is mainly composed of ɛ phase and γ′ phase, and the crystal grains of the ɛ phase is fine and has high dislocations density.     

Application of Dielectric Barrier Discharge Reactor Immersed in Wastewater to the Oxidative Degradation of Organic Contaminant

Dielectric barrier discharge (DBD) is an effective method available for the production of ozone and ultraviolet light. The wastewater treatment system of this study was designed to utilize both ozone and ultraviolet light produced in the DBD reactor for the degradation of organic contaminant. The DBD reactor consisted of a quartz cylinder and a coaxial ceramic tube inside of which a steel rod was placed. The DBD reactor was immersed in the wastewater that was grounded. In this case, the wastewater acted not only as an electrode but also as the cooling medium for the DBD reactor. An azo dye, Acid Red 27, was used as the organic contaminant. In this system, the organic contaminant was degraded by two oxidation pathways induced by ozone and ultraviolet light. The concentration of ozone, the ultraviolet radiation intensity and the degradation efficiency of the organic contaminant were measured by varying the discharge. The results showed that the present system was very effective for the degradation of the organic contaminant. The energy requirement for the degradation was found to be 0.654 kJ/mg, which is much smaller value than those obtained with an ultraviolet/photocatalytic process.     

低温等离子体原子化器-原子荧光光谱法测定碲

基于介质阻挡放电(DBD)原理和结构,建立了适用于原子荧光光谱仪(AFS)的低温等离子体小型原子化器(Atomizer),并研究了氢化物发生-低温等离子体原子化器-原子荧光光谱(HG-DBDAtomizer-AFS)测定环境样品中痕量碲(Te)的分析方法。DBD等离子体原子化器具有小型、低温等优点。对DBD放电结构和放电功率、载气气体流速,氢化物发生过程中的酸度、KBH4浓度,以及观测高度等实验条件进行了详细的考察并优化。本系统测定Te的检出限(3σ)为0.08μg/L;线性范围为0.5～80μg/L;测定精密度为2.1%(n=7);加标回收率为90%～103%。对国家级标准样品(GBW07404,GBW07405,GBW07406)进行测定,测定结果与标准值一致,证明本方法准确可行。     

A Study of Two-Dimensional Microdischarge Pattern Formation in Dielectric Barrier Discharges

Although microdischarges in dielectric-barrier discharges (DBDs) have been studied for the past century, their mutual interaction was explained only recently. This interaction is responsible for the formation of microdischarge patterns reminiscent of two-dimensional crystals. Depending on the application, microdischarge patterns may have a significant influence on DBD performance, particularly when spatial uniformity is desired. This paper presents the results of study of regular microdischarge pattern formation in DBD in air at atmospheric pressure. Experimental images of DBD (Lichtenberg figures) were obtained using photostimulable phosphors. A new method for analysis of microdischarge patterns that allow measuring the degree of pattern regularity was developed. Simulated and experimental patterns were compared using the newly developed method and comparison indicates the presence of interaction between microdischarges. Analysis of microdischarge patterns shows that regularity of the patterns increases with the number of excitation cycles used to produce the pattern.