Research on the degradation mechanism of pyridine in drinking water by dielectric barrier discharge

Pyridine, an important chemical raw material, is widely used in industry, for example in textiles,leather, printing, dyeing, etc. In this research, a dielectric barrier discharge(DBD) system was developed to remove pyridine, as a representative type of nitrogen heterocyclic compound in drinking water. First, the influence of the active species inhibitors tertiary butanol alcohol(TBA),HCO_3~-, and CO_3~(2-)on the degradation rate of pyridine was investigated to verify the existence of active species produced by the strong ionization discharge in the system. The intermediate and final products generated in the degradation process of pyridine were confirmed and analyzed through a series of analytical techniques, including liquid chromatography–mass spectrometry(LC–MS), high performance liquid chromatography(HPLC), ion chromatography(IC), total organic carbon(TOC) analysis, ultraviolet(UV) spectroscopy, etc. The results showed that the degradation of pyridine was mainly due to the strong oxidizing power of ozone and hydroxyl radical produced by the DBD system. Several intermediate products including 3-hydroxyl pyridine, fumaric acid, 2, 3-dihydroxypyridine, and oxalic acid were detected. Nitrogen was removed from the pyridine molecule to form nitrate. Through analysis of the degradation mechanism of pyridine, the oxidation pathway was deduced. The study provided a theoretical and experimental basis for the application of DBD strong ionization discharge in treatment of nitrogen heterocyclic compounds in drinking water.     

Toluene removal characteristics by a superimposed wire-plate dielectric barrier discharge plasma reactor

A superimposed wire-plate dielectric barrier discharge reactor was used to remove toluene in this study. The effects of oxygen content, gas flow rate, gas initial concentration and with/without catalyst on toluene decomposition were investigated. It was found that an optimal toluene removal was achieved when the oxygen content was about 5%. Under this condition, the highest toluene removal efficiency of 80.8% was achieved when the gas concentration was 80 mg/m^3. The toluene removal efficiency decreased with the increase of the gas flow rate and the initial concentration of toluene. In addition, the ozone concentration decreased with the increase of the initial concentration of toluene. It suggested that combining DBD （dielectric barrier discharge） with Co3O4/Al2O3/foam nickel catalyst in-situ could improve the toluene removal efficiency and suppress ozone formation. Products analysis showed that the main products were CO and CO2 when oxygen was more than 5%.     

介质阻挡放电联合催化臭氧化降解甲苯

采用介质阻挡放电区后结合MnOx/Al2O3/发泡镍去除甲苯,考察甲苯进气方式、臭氧产生方法及湿度对甲苯与O3同时去除的影响。结果表明,O3是等离子体区后催化降解甲苯的主要物种,介质阻挡放电联合催化臭氧化可实现甲苯及O3的同时高效去除。输入电压为9.0 kV时,甲苯的去除效率达92.8%,在80 min内O3的去除效率维持在99%以上。水蒸气对催化剂催化分解臭氧的活性没有直接的影响,O3浓度较高时湿度对甲苯降解效率的影响很小。GC-MS分析结果表明,甲苯降解的主要气相副产物有烷烃、酸、酮和含苯环有机物,提出了甲苯的降解途径。     

反应气耦合等离子体降解沙林模拟剂

采用水蒸气、氨气、过氧化氢气雾和臭氧4种气体对沙林模拟剂氟磷酸二异丙酯(DFP)进行降解研究,发现臭氧对DFP具有较好的降解作用,在流量200 L/h,DFP初始浓度50 mg/m3时,降解率最高可达56.1%。对高浓度DFP(大于80 mg/m3)进行降解研究时,等离子体单独作用最高降解率为89%,而添加臭氧后的降解率都在95%以上。计算得到臭氧作用的能量利用率为0.05 mg/(W·h),等离子体的能量利用率为0.55 mg/(W·h),而添加臭氧后的等离子体能量利用率为0.68 mg/(W·h)明显高于臭氧和等离子体能量利用率之和,因此对高浓度DFP进行处理时,臭氧与等离子体存在耦合作用。对等离子体和臭氧耦合等离子体降解DFP反应进行了产物分析,发现主要的降解产物基本一致,但是臭氧的存在能使降解更加彻底。     

等离子体固态可燃物液化反应动力学分析

本文利用介质阻挡放电等离子体技术,对以煤和生物质为代表的固态可燃物液化反应机理进行研究,以期探索能源利用新途径.借助碰撞理论和Boltzman方程,对高能电子碰撞引发多种离解反应的速率常数进行数值模拟,计算结果和实验曲线对比,证明模型具有一定的适用性和可靠性.在一定的电子温度下,通过不同离解反应速率常数的对比,可以判断...     

CuSnZr三元催化剂应用于NTP强化催化脱硫过程的特性

为高效地在低温下处理大量低浓度电解铝烟气, 采用浸渍法制备了Sn Zr型金属氧化物并添加Cu作为助剂的催化剂, 并首次测试了它在低温等离子体(NTP)技术上的脱硫效果, 结果表明负载了20wt% Cu老化温度为40℃的催化剂表现出最佳的脱硫性能.并对强化之后的催化剂进行了表征, 与新鲜的催化剂对比, X射线衍射分析(XRD)结果表明放电对催化剂晶型基本不产生影响; 扫描电子显微镜(SEM), 氮吸附和脱吸(BET)表明放电会使催化剂的吸附脱附能力与孔道结构有较大提升; X射线光电子光谱(XPS)也表明放电会使催化剂表面元素价态变化, 从而使其氧化还原性能改变, 反应路径发生偏向; 催化剂性能理论计算表明铜含量的上升会导致催化剂能带结构改变, 更好利用于激发气体.     

阻挡放电联合金属氧化物催化降解H2S的研究

采用介质阻挡放电联合金属氧化物催化降解气态H2S,考察了单组分及复合金属氧化物催化剂、催化剂与低温等离子体结合方式对H2S及副产物O3去除性能的影响,分析了等离子体联合Mn复合金属氧化物催化降解H2S机理。结果表明,金属负载量相同条件下,电压低于22kV时,Mn复合金属氧化物对H2S的催化活性高于单组分Mn金属氧化物,催化活性及对O3的分解能力从大到小依次为:Ag+Mn、Cu+Mn、Fe+Mn、Mn。当电压为18 kV时,Ag+Mn、Cu+Mn、Fe+Mn复合催化剂分别比单组分Mn催化剂对H2S的去除效率提高了近10%、6%、4%。等离子体后催化区域中Mn催化剂催化氧化H2S的效率明显低于等离子体催化区域。Mn催化剂在等离子体后催化区域中能有效催化分解O3。随着电压的升高,Mn金属氧化物在等离子体后催化区域对H2S催化作用逐渐增强。在电压22 kV时,等离子体联合后催化比单独等离子体作用时,H2S去除效率提高了近11%。     

介质特性对DBD降解苯的影响

为了提高介质阻挡放电(dielectric barrier discharge,DBD)等离子体的处理效率,研究了内外介质组成分别为:(1)石英 石英;(2)陶瓷 石英;(3)陶瓷 陶瓷这3种情况下苯的降解情况.试验结果表明,在处理低浓度含苯废气时,陶瓷 陶瓷效果最好;陶瓷(内管) 石英(外管)在处理高浓度含苯废气时显示出优势.通过对气相产物和固相结焦产物的分析验证了DBD能有效降解苯,降解产物不会带来新的污染.进一步分析了实验条件和介质材料的变化对DBD降解苯的影响机理.     

介质阻挡放电等离子体分解CO_2

温室效应导致全球变暖已成为全球性的环境问题之一.采用放电等离子体法转化CO2,不仅可消纳温室气体,缓解全球变暖的巨大影响,还可制备化工原料CO和O2.充分利用了C1(含1个碳原子的化合物分子)资源,对高频同轴式介质阻挡放电等离子体分解纯CO2进行了研究.结果发现:在采用不锈钢光滑内电极,放电间隙为2.0mm,注入功率为180W,气体流量为170mL/min的条件下,CO2转化率可达18.2%,CO和O2产率分别为10.1%和4.7%;增大注入功率,减小气体流量、选择合适的放电间隙和内电极形式,均有利于提高CO2转化率,获得更多的CO和O2.     

DBD反应器关键操作参数对2,4-二氯酚去除的影响

采用同轴喷雾式介质阻挡放电(DBD)反应器处理2,4-二氯酚(2,4-DCP)模拟废水,考察了水质、废水流量、载气流量、放电频率等关键操作参数对2,4-DCP去除的影响。自来水中的CO₃^2-/HCO₃^-能够中和生成的硝酸/亚硝酸(载气含N₂),同时也能清除放电过程中产生的自由基,因而不利于2,4-DCP的去除。在DBD反应器的操作参数中,载气流量对于活性组分的产生及气相到液相的传质有显著影响,是最为关键的操作参数。反应器操作参数的变化会影响放电过程。同轴式反应器和废水雾化对污染物的矿化有利。在废水流量50 mL/min、载气流量15 L/min、放电频率17 kHz的最佳条件下处理60 min,2,4-DCP和TOC的去除率分别为69.77%和31.85%。