Methane Decomposition and C2 Hydrocarbon Formation under the Condition of DC Discharge Plasma

The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The processes of methane decomposition and formation of C2 hydrocarbons were studied. The experiment shows that methane decomposition can be divided into three periods as the reaction proceeds.In the first period, a large number of free radicals were formed. While in the last period, the formation of C2 hydrocarbons and the decrease of free radicals were observed. The time and conditions of methane decomposition and formation of C2 hydrocarbons are different.     

Methane Coupling Using Hydrogen Plasma and Pt／γ—Al2O3 Catalyst

In this paper,methane coupling at ambient temperature, under atmospheric pressure and in the presence of hydrogen was firstly investigated by using pulse corona plasma and Pt/γ-Al2O3 catalyst. Experimental results showed that Pt/γ-Al2O3 catalyst has catalytic activity for methane couplin to C2H4. Over sixty percent o outcomes of C2 hydrocarbons were detected to be ethylene.     

Pd／Sulfated Alumina： a Novel Catalyst for Selective Catalytic Reduction of NO with Methane

Recently ,muchattentionhasbeendirectedtotheselectivecatalyticreduction (SCR)ofNOwithmethaneasreductant[1,2 ] .Pd basedcatalystshavebeenfoundtobeactiveforthereaction[3～ 6 ] .Howev er,theperformanceofthePd basedcatalystsforthisreactiondependsstronglyonthenatureofthesup ports[3,4 ] .Sofar ,onlyacidiczeolites[3,4 ] andacidiczirconia[4～ 6 ] havebeenshowntobetheeffectivesup portsforthePd basedcatalysts .Incontrast,Pd/γ Al2 O3,whichisoneofthemostwidelyusedthree waycatalystsatpresent[7] ,exhibi…     

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.     

甲烷参与下催化剂填充型介质阻挡放电等离子体脱除NOx

 将In/HZSM-5催化剂填充于介质阻挡放电反应器中,考察了甲烷参与下NOx的脱除及其脱除产物. 结果表明,在200～350 ℃间,等离子体与催化剂共同作用时NOx的转化率明显高于等离子体或催化剂单独作用时NOx的转化率. 在0.03%NO-0.05%CH4-2%O2-97.92%N2,空速7200 h-1和300 ℃的条件下,单纯等离子体、单纯催化剂和二者共同作用下NOx的转化率分别为24%,25%和65%. 甲烷参与下等离子体和催化剂共同作用时,在催化剂表面没有硝酸盐或亚硝酸盐生成,仅有少量副产物N2O生成. 由此可以推断,NOx脱除的主要产物为N2. 低于300 ℃时,NOx的脱除以分解途径为主,甲烷的作用主要是抑制放电条件下NOx生成的副反应; 在300～350 ℃间,甲烷作为还原剂被等离子体和催化剂协同活化,NOx的脱除以还原途径为主. 采用催化剂填充型介质阻挡放电反应器,可在非常宽的温度区间实现NOx的脱除.     

Oxidative Conversion of PFC via Plasma Processing with Dielectric Barrier Discharges

Perfluorocompounds (PFCs) have been extensively used as plasma etching andchemical vapor deposition (CVD) gases for semiconductor manufacturingprocesses. PFCs have significant effects on the global warming and havevery long atmospheric lifetimes. Laboratory-scale experiments were performedto evaluate the effectiveness of CF4 conversion by using dielectric barrierdischarges (DBD). The results of this study revealed that the removalefficiency of CF₄ increased with application of higher voltage, gas residence time, oxygen content, and frequency. Combined plasma catalysis(CPC) is an innovative way for abatement of PFC and experimental results indicated that combining plasma with catalysts could effectively remove CF4. Products were analyzed by Fourier transform–infrared spectroscopy (FT–IR) and the major products of the CF4 processing with DBD were CO2, COF2, and CO, when O was included in the discharge process. Preliminary results indicated that as high as 65.9% of CF4 was decomposed with CPC operated at 15 kV, 240 Hz for the gas stream containing 300 ppmv CF₄,20% by volume O₂, and 40% by volume Ar, with N₂ as thecarrier gas.     

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.     

Methane Conversion to Higher Hydrocarbons in the Presence of Carbon Dioxide Using Dielectric-Barrier Discharge Plasmas

Experimental investigation has been conducted to convert methane into higher hydrocarbons in the presence of carbon dioxide within dielectric-barrier discharge (DBD) plasmas. The objectives of cofeed of carbon dioxide are to inhibit carbon deposit and to increase methane conversion. The products from this plasma methane conversion include: (1) syngas (H₂+CO), (2) gaseous hydrocarbons containing ethylene, acetylene, and propylene, (3) liquid hydrocarbons, (4) plasma-polymerized film, and (5) oxygenates. The selectivity of products is subject to the DBD plasma-reactive conditions and catalyst applied. The liquid hydrocarbons produced by this way are highly branched, which represents a better fuel production.     

Gas-Phase Removal of Acetaldehyde via Packed-Bed Dielectric Barrier Discharge Reactor

The effectiveness of applying packed-bed dielectric barrier discharge(PBDBD) technology for removing acetaldehyde from gas streams wasinvestigated. Operating parameters examined in this study include appliedvoltage, oxygen content, and gas-flow rate. Experimental results indicatethat the destruction efficiency of acetaldehyde predominantly depends onthe applied voltage. Removal of 99% of acetaldehyde has been achieved forgas streams containing 1000 ppmv acetaldehyde, 5% oxygen, with nitrogen asthe carrier gas. The oxygen content in the gas stream plays an importantrole in removing acetaldehyde within PBDBD. A higher CH3CHO removalefficiency is achieved for the gas stream containing less oxygen, since itwill dissipate energy due to its electronegative property. Carbon dioxideis the major end product, which is less hazardous to the environment and tohuman health. However, undesirable products, e.g., NO₂ and N₂O,CH₃OC₂H₅, CH₃COOH, CH₃NO₂,HCN, CH₃NO₃, and CH₃OH, are detected as well.     

Direct Non-oxidative Methane Conversion by Non-thermal Plasma: Experimental Study

The direct non-oxidative conversion of methane to higher hydrocarbons in non-thermal plasma, namely dielectric barrier discharge and corona discharge, has been investigated experimentally at atmospheric pressure. In dielectric barrier discharge, the methane is mainly converted to ethane and propane with small amounts of unsaturated and higher hydrocarbons. While in corona discharge, methane was activated mainly to acetylene with small amount of other higher hydrocarbons. Decreasing the gas flow or increasing power input will improve the methane conversion and product yields. It is found that the methane conversion and main product yield against the input specific energy were special functions in both dielectric barrier discharge and corona discharge, independent of the reactor size, and whether fixing flow rate or power input and changing the power input or flow rate. The corona discharge is a promising alternative method for methane conversion to produce acetylene and hydrogen at low temperature.     

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.     

低温等离子体转化NO/O2/N2气氛中NO的实验研究

通过建立低温等离子体实验系统, 研究了介质阻挡放电型低温等离子体反应器作用于NO/O2/N2混合气体系时, NO, O2初始浓度对NO的转化效率的影响以及NOx, O3浓度随能量密度的变化关系. 低温等离子体作用于NO/O2/N2混合气体系时, NO同时发生氧化还原反应, 氧化反应占主导地位, 大部分NO转化为NO2; NO转化率随O2, NO初始浓度增大而降低, 能量密度在450～600 J/L时转化率较高; 产生的O3浓度随能量密度的增大呈先增后减的趋势.     

Direct Non-oxidative Methane Conversion by Non-thermal Plasma: Modeling Study

The direct non-oxidative conversion of methane to higher hydrocarbons in dielectric barrier discharges has been investigated theoretically at atmospheric pressure. Preliminary modeling of the results is presented, based on a well-stirred reactor model to determine the spatially and time-averaged species composition through the solution of balance equations for species, mass, gas and electron energy. The results show good quantitative agreement between model predications and experimental measurements by considering the glow and after-glow regions. Moreover, the model has predicted that there exists a transition where the main product of ethane will transform to acetylene by increasing the specific energy. The dominant reaction paths and the possibility of selective to C₂ hydrocarbons have been discussed. A list of gas-phase reactions has been compiled for modeling methane conversion in non-thermal plasma and can be employed in more sophisticated two- or three-dimensional plasma simulations.