A comparative study on the activity of TiO2 in pulsed plasma under different discharge conditions

In the present study,a combination of pulsed discharge plasma and TiO_2(plasma/TiO_2)has been developed in order to study the activity of TiO_2by varying the discharge conditions of pulsed voltage,discharge mode,air flow rate and solution conductivity.Phenol was used as the chemical probe to characterize the activity of TiO_2in a pulsed discharge system.The experimental results showed that the phenol removal efficiency could be improved by about 10%by increasing the applied voltage.The phenol removal efficiency for three discharge modes in the plasma-discharge-alone system was found to be highest in the spark mode,followed by the spark–streamer mode and finally the streamer mode.In the plasma/TiO_2system,the highest catalytic effect of TiO_2was observed in the spark–streamer discharge mode,which may be attributed to the favorable chemical and physical effects from the spark–streamer discharge mode,such as ultraviolet light,O_3,H_2O_2,pyrolysis,shockwaves and high-energy electrons.Meanwhile,the optimal flow rate and conductivity were 0.05 m~3l~(-1)and 10μS cm~(-1),respectively.The main phenolic intermediates were hydroquinone,catechol,and p-benzoquinone during the discharge treatment process.A different phenol degradation pathway was observed in the plasma/TiO_2system as compared to plasma alone.Analysis of the reaction intermediates demonstrated that p-benzoquinone reduction was selectively catalyzed on the TiO_2surface.The effective decomposition of phenol constant(D_e)increased from 74.11%to 79.16%when TiO_2was added,indicating that higher phenol mineralization was achieved in the plasma/TiO_2system.     

电极结构及填充介质对二氧化碳重整甲烷制合成气的影响

为了考察电极结构及填充介质对放电及二氧化碳重整效果的影响,对线管式介质阻挡放电(DBD)反应装置3种不同电极结构及下的电信号进行了测量,并分析了不同电极结构及不同形貌填充介质下的重整效果。结果表明:反应气体为CH_4和CO_2,DBD反应装置的内电极分别为光滑电极、螺纹电极、线圈电极时,反应装置放电起始电压依次减小。相同电压下,线圈电极下放电功率大于其他2个电极,CH_4和CO_2的转化率也高于其他2个电极所在的反应器,但是CO的选择性明显低于其他2个电极。在放电间隙填充介质后,介质表面形成极化电场,放电区域局部场强增大,促进CH_4和CO_2的分解,活性三氧化二铝小球对CO_2有一定的吸附性,填充三氧化二铝小球下CO_2的转化率高于玻璃珠填充;与球状填充介质相比,填充不规则块状活性三氧化二铝时,放电区域产生的局部电场放电强度增大,CH_4的转化率有明显的提升,但是与无填充相比其对CO_2转化影响很小。     

介质阻挡放电脱色酸性橙Ⅱ废水的动力学及脱色物化效应

气-液两相介质阻挡放电(DBD)等离子体对废水电导率较不敏感,因此电极施加电压和放电气隙成为影响放电强度及废水中污染物降解的两个主要因素。以酸性橙Ⅱ(AO7)废水为对象,考察了电极施加电压、放电气隙等因素对DBD装置放电特性及AO7降解动力学的影响,分析了DBD降解AO7的主要物化效应。结果表明:高压电极引发的丝状放电通道随电压升高、放电气隙减小而增多,且丝状放电通道在接近液面时出现明显的分支现象;AO7降解符合一级反应动力学,施加电压升高、放电气隙减小可提高AO7降解的反应动力学常数。放电气隙为6 mm,峰值电压从15 kV分别升高2 kV和4 kV,反应动力学常数可提高4.45倍和5.67倍;电极施加电压为17 kV,放电气隙从8 mm减小到4 mm和2 mm,AO7降解的反应动力学常数可分别提高3.51倍和6.67倍。废水的pH值对AO7降解也有较大影响,酸性条件和碱性条件下AO7降解的反应动力学常数较大。分析DBD等离子体降解AO7的物理化学效应,臭氧和过氧化氢等反应活性物质是AO7降解的主要原因。     

Evaluation on a double-chamber gas-liquid phase discharge reactor for benzene degradation

A double-chamber gas-liquid phase DBD reactor (GLDR), consisting of a gas-phase discharge chamber and a gas-liquid discharge chamber in series, was designed to enhance the degradation of benzene and the emission of NOx. The performance of the GLDR on discharge characteristics, reactive species production and benzene degradation was compared to that of the single-chamber gas phase DBD reactor (GPDR). The effects of discharge gap, applied voltage, initial benzene concentration, gas flow rate and solution conductivity on the degradation and energy yield of benzene in the GLDR were investigated. The GLDR presents a higher discharge power, higher benzene degradation and higher energy yield than that of the GPDR. NO₂ emission was remarkably inhibited in the GLDR, possibly due to the dissolution of NO₂ in water. The benzene degradation efficiency increased with the applied voltage, but decreased with the initial concentration, gas flow rate, and gas discharge gap, while the solution conductivity presented less influence on benzene degradation. The benzene degradation efficiency and the energy yield reached 61.11% and 1.45 g kWh^–1 at 4 mm total gas discharge gap, 15 kV applied voltage, 200 ppm benzene concentration, 0.2 L min⁻¹ gas flow rate and 721 μS cm⁻¹ water conductivity. The intermediates and byproducts during benzene degradation were detected by FT-IR, GC-MS and LC-MS primarily, and phenols, CO_x, and other aromatic substitutes, O₃, NO_x, etc, were determined as the main intermediates. According to these detected byproducts, a possible benzene degradation mechanism was proposed.     

沿面型介质阻挡放电中高压电极配置对放电特性及臭氧产量的影响

为了提高沿面型介质阻挡放电反应器的放电性能及臭氧产量,以螺环型沿面放电作为研究对象,探讨了不同外加条件、电极结构对沿面放电功率和臭氧产量的影响,并通过分析不同条件下的Lissajous图形探讨了各项因素的影响程度。实验测试了5种不同管径d的反应器,其d分别为7.5、16.7、24.7、35.0、56.0 mm。实验结果表明:外加电压U相同时,采用50 Hz工频电源,管径d为56.0 mm时的放电功率P最大为43.3 W,臭氧产量Q也达到最大值753.0 mg/h;而单位体积的放电功率PV及单位体积的臭氧产量QV的考察结果与之相反,在d为7.5mm时取得最大值;单位功率臭氧产量QW则是在d为16.7 mm时存在一个最佳值;随着高压弹簧电极线径l和螺距s的增大,相应的P和Q也有不同程度的增加,但其影响都不是单方面的;沿面放电中d是对P和Q影响最大的因素,壁厚d′次之,l与s影响最小。Lissajous图形的分析结果也表明:d的变化对气隙等效电容有更大的影响,因此其对P的影响也最大。     

Performance of Dielectric Barrier Discharge Reactors on Elemental Mercury Oxidation in the Coal-Fired Flue Gas

The oxidation of elemental mercury （Hg~） by dielectric barrier discharge reactors was studied at room temperature, where concentric cylinder discharge reactor （CCDR） and surface discharge plasma reactor （SDPR） were employed. The parameters （e.g. Hg^0 oxidation efficiency, energy constant, energy yield, energy consumption, and O3 concentration） were discussed. From comparison of the two reactors, higher Hg^0 oxidation efficiency and energy constant in the SDPR system were obtained by using lower specific energy density. At the same applied voltage, energy yield in the SDPR system was larger than that in the CCDR system, and energy consumption in the SDPR system was much less. Additionally, more 03 was generated in the SDPR system. The experimental results showed that 98% of Hg^0 oxidation efficiency, 0.6 J·L^-1 of energy constant, 13.7 μg·J^-1 of energy yield, 15.1 eV·molecule^-1 of energy consumption, and 12.7 μg·J^-1 of O3 concentration were achieved in the SDPR system. The study reveals an alternative and economical technology for Hg^0 oxidation in the coal-fired flue gas.     

Electrical Characteristics of Pulsed Corona Discharge Plasmas in Chitosan Solution

Pulsed discharge plasma has exhibited active potential to prepare low molecular weight chitosan. In the present study, the viscosity of ehitosan solution was decreased noticeably after treated with pulsed corona discharge plasma. An experimental investigation on electrical characteristics of pulsed corona discharge plasma in chitosan solution was conducted with a view toward getting insight into discharge process. Factors affecting I-V curve, single pulse injec- tion energy and pulse width were studied. Experimental results showed positive effect of pulsed peak voltage on discharge plasma in chitosan solution. Pulse-forming capacitor greatly influenced the discharge form, and 4 nF was observed as a suitable value for efficiently generating stable discharge plasmas. As the electrode distance was larger than 10 ram, it had slight impact on dis- charge plasma due to the excellent conductive-property of chitosan solution. The injection energy significantly increased with air flow rate, while the pulse width hardly changed as the air flow rate increased from 0.5 m^3/h to 1.0 m^3/h. This study is expected to provide reference for promoting the application of pulsed corona discharge plasma to ehitosan solution treatment.     

用气相沿面放电生成臭氧方式降解偶氮染料废水的影响因素分析

为提高臭氧降解和脱色染料废水的效果,通过沿面放电臭氧生成-废水处理一体化反应器降解偶氮染料废水研究了供电电源类型、放电电压、放电反应器内注入的气体组分及流量、废水电导率、催化剂等因素对染料降解的影响。研究结果表明:同50Hz工频电源相比,在相同的输入功率下,高频电源降解偶氮染料效果更快;沿面放电反应器内注入的气体成分影响染料降解率,注入氧气时,甲基红降解率最高,注入氮气时,甲基红几乎没有降解;注入气体流量影响气相和液相臭氧浓度及染料废水的湍流度,进而影响甲基红的降解率;废水电导率对甲基红降解影响不大;二氧化钛添加量影响甲基红的降解,染料降解初期,适量的二氧化钛有利于甲基红的降解。     

The structure optimization of gas-phase surface discharge and its application for dye degradation

A gas-phase surface discharge (GSD) was employed to optimize the discharge reactor structure and investigate the dye degradation. A dye mixture of methylene blue, acid orange and methyl orange was used as a model pollutant. The results indicated that the reactor structure of the GSD system with the ratio of tube inner surface area and volume of 2.48, screw pitch between a high-voltage electrode of 9.7 mm, high-voltage electrode wire diameter of 0.8 mm, dielectric tube thickness of 2.0 mm and tube inner diameter of 16.13 mm presented a better ozone (O3) generation efficiency. Furthermore, a larger screw pitch and smaller wire diameter enhanced the O3 generation. After the dye mixture degradation by the optimized GSD system, 73.21％ and 50.74％ of the chemical oxygen demand (COD) and total organic carbon removal rate were achieved within 20 min, respectively,and the biochemical oxygen demand (BOD) and biodegradability (BOD/COD) improved.