采用切向气流和磁场协同驱动的旋转滑动弧氩等离子体,先通过光谱分析法计算了其电子温度和电子密度,了解其物理特性,将其应用于甲烷裂解制氢,研究了进气流量和CH_4/Ar比对反应效果的影响。结果表明,该滑动弧系统电子温度为1.0-2.0 e V,...采用切向气流和磁场协同驱动的旋转滑动弧氩等离子体,先通过光谱分析法计算了其电子温度和电子密度,了解其物理特性,将其应用于甲烷裂解制氢,研究了进气流量和CH_4/Ar比对反应效果的影响。结果表明,该滑动弧系统电子温度为1.0-2.0 e V,电子密度高达1015cm^(-3),是介于热与低温等离子体之间的一种等离子体形式,具有独特的物理特性,可以在达到较高反应效率的同时,保持较大的处理量;在CH_4裂解制氢实验中,CH_4转化率可达22.1%-70.2%,并随进气流量和CH_4/Ar比的增大均逐渐降低;H_2选择性为21.2%-61.2%,并随进气流量的增大先基本不变后有所增大,随CH_4/Ar比的增大逐渐降低;与应用于甲烷裂解的不同形式的低温等离子体对比(如微波、射频、介质阻挡放电等)可以发现,旋转滑动弧在获得较高甲烷转化率、较高H_2选择性和较低制氢能耗的同时,还可以保持较大的处理量,即进气流量可达6-20 L/min。展开更多
The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surroga...The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surrogate.Based on a previous investigation of discharge properties,product distribution and energy efficiency,the operating parameters such as CH4 concentration,applied voltage and gas flow rate can effectively affect the CH4 conversion rate,the selectivity of H2 and the properties of solid generated carbon.Nevertheless,the basic properties of RGA plasma and its role in CH4 conversion are scarcely mentioned.In the present work,a 3D RGA model,with a detailed nonequilibrium CH4/Ar plasma chemistry,is developed to validate the previous experiments on CBM conversion,aiming in particular at the distribution of H2 and other gas products.Our results demonstrate that the dynamics of RGA is derived from the joint effects of electron convection,electron migration and electron diffusion,and is prominently determined by the variation of the gas flow rate and applied voltage.Subsequently,a combined experimental and chemical kinetical simulation is performed to analyze the selectivity of gas products in an RGA reaction,taking into consideration the formation and loss pathways of crucial targeted substances(such as CH4,C2H2,H2 and H radicals)and corresponding contribution rates.Additionally,the effects of operating conditions on the properties of solid products are investigated by scanning electron microscopy(SEM)and Raman spectroscopy.The results show that increasing the applied voltage and decreasing CH4 concentration will change the solid carbon from its initial spherical structure into folded multilayer graphene sheets,while the size of the graphene sheets is slightly affected by the change in gas flow rate.展开更多
In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the init...In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the initial concentration increased from 100 mg/L to 160 mg/L, the discolouration rate of AO7 decreased from 99.3% to 95.9%, whereas the COD removal rate decreased from 37.9% to 22.6%. Air provided the best discolouration and COD removal rates （99.3% and 3？.9%, respectively）. In the presence of a zero-valent iron （ZVI） catalyst, the AO？ COD removal rate increased to 76.4%. The degradation products were analysed by a GC-MS, revealing that the degradation of the dye molecule was initiated through the cleavage of the -N=N- bond before finally being converted to organic acids.展开更多
The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external a...The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external antenna voltage and current increase with the augment of RF power, whereas decline with the enhancement of gas pressure and flow rate conversely.Compared with gas flow rate and pressure, the power transfer efficiency is significantly improved by RF power, and achieved its maximum value of 0.85 after RF power injected excess125 W. Optical emission spectroscopy（OES） provides the local mean values of electron excited temperature and electron density in inductively coupled plasma（ICP） post regime, which vary in a range of 0.81 eV to 1.15 eV and 3.7×10^（16）m^（-3）to 8.7×10^（17）m^（-3）respectively. Numerical results of the average magnitudes of electron temperature and electron density in twodimensional distribution exhibit similar variation trend with the experimental results under different operating condition by using COMSOL Multiphysics. By comprehensively understanding the characteristics in a low pressure ICP, optimized operating conditions could be anticipated aiming at different academic and industrial applications.展开更多
One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties ...One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties of the ICPECVD process were revealed via electrical diagnosis and optical emission spectroscopy. The coil current and voltage increased linearly with the augmenting of injected power, and CH, C2, H2 and H were detected at a wavelength from 300 to 700 nm, implying the generation of abundant graphene-building species. The morphology and structure of solid carbon products, graphene nanosheets, were systemically characterized in terms of the variations of operating conditions, such as pressure, temperature, gas proportion, etc. The results indicated that an appropriate operating condition was indispensable for the growth process of graphene nanosheets. In the present work, the optimized result was achieved at the pressure, heating temperature, applied power and gas proportion of 600 mTorr, 800 ~C, 500 W and 20：20：15, respectively, and the augmenting of both CH4 and H2 concentrations had a positive effect on the etching of amorphous carbon. Additionally, H2 and C2 hydrocarbons were detected as the main exhaust gases. The selectivity of H2 and C2H2, measured in exhaust gases, reached up to 52% and 8%, respectively, which implied a process of free radical reactions and electron collision dissociation. Based on a comprehensive investigation of spectral and electrical parameters and synthesized products, the reaction mechanism of collision, dissociation, diffusion, etc, in ICPECVD could be speculated, providing a probable guide for experimental and industrial applications.展开更多
A facile and controllable one-step method to treat liquid hydrocarbons and synthesize vertical graphene nanowalls has been developed by using the technique of inductively-coupled plasma-enhanced chemical vapor deposit...A facile and controllable one-step method to treat liquid hydrocarbons and synthesize vertical graphene nanowalls has been developed by using the technique of inductively-coupled plasma-enhanced chemical vapor deposition for plasma cracking of n-dodecane.Herein,the morphology and microstructure of solid carbon material and graphene nanowalls are characterized in terms of different operating conditions,i.e.input power,H2/Ar ratio,injection rate and reaction temperature.The results reveal that the optimal operating conditions were 500 W,5:10,30μl min^-1 and 800℃ for the input power,H2/Ar ratio,injection rate and reaction temperature,respectively.In addition,the degree of graphitization and the gaseous product are analyzed by Raman spectroscopy and gas chromatography detection.It can be calculated from the Raman spectrum that the relative intensity of ID/IG is approximately 1.55,and I2D/IG is approximately 0.48,indicating that the graphene prepared from n-dodecane has a rich defect structure and a high degree of graphitization.By calculating the mass loading and detecting the outlet gas,we find that the cracking rate of n-dodecane is only 6%-7%and that the gaseous products below C2 mainly include CH4,C2H2,C2H4,C2H6 and H2.Among them,the proportion of hydrogen in the outlet gas of n-dodecane cracking ranges from 1.3%-15.1%under different hydrogen flows.Based on our research,we propose a brand new perspective for both liquid hydrocarbon treatment and other value-added product syntheses.展开更多
文摘采用切向气流和磁场协同驱动的旋转滑动弧氩等离子体,先通过光谱分析法计算了其电子温度和电子密度,了解其物理特性,将其应用于甲烷裂解制氢,研究了进气流量和CH_4/Ar比对反应效果的影响。结果表明,该滑动弧系统电子温度为1.0-2.0 e V,电子密度高达1015cm^(-3),是介于热与低温等离子体之间的一种等离子体形式,具有独特的物理特性,可以在达到较高反应效率的同时,保持较大的处理量;在CH_4裂解制氢实验中,CH_4转化率可达22.1%-70.2%,并随进气流量和CH_4/Ar比的增大均逐渐降低;H_2选择性为21.2%-61.2%,并随进气流量的增大先基本不变后有所增大,随CH_4/Ar比的增大逐渐降低;与应用于甲烷裂解的不同形式的低温等离子体对比(如微波、射频、介质阻挡放电等)可以发现,旋转滑动弧在获得较高甲烷转化率、较高H_2选择性和较低制氢能耗的同时,还可以保持较大的处理量,即进气流量可达6-20 L/min。
基金supported by the Foundation for Innovative Research Groups of National Natural Science Foundation of China (No. 51621005)China Postdoctoral Science Foundation (No. 2018M630672)
文摘The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surrogate.Based on a previous investigation of discharge properties,product distribution and energy efficiency,the operating parameters such as CH4 concentration,applied voltage and gas flow rate can effectively affect the CH4 conversion rate,the selectivity of H2 and the properties of solid generated carbon.Nevertheless,the basic properties of RGA plasma and its role in CH4 conversion are scarcely mentioned.In the present work,a 3D RGA model,with a detailed nonequilibrium CH4/Ar plasma chemistry,is developed to validate the previous experiments on CBM conversion,aiming in particular at the distribution of H2 and other gas products.Our results demonstrate that the dynamics of RGA is derived from the joint effects of electron convection,electron migration and electron diffusion,and is prominently determined by the variation of the gas flow rate and applied voltage.Subsequently,a combined experimental and chemical kinetical simulation is performed to analyze the selectivity of gas products in an RGA reaction,taking into consideration the formation and loss pathways of crucial targeted substances(such as CH4,C2H2,H2 and H radicals)and corresponding contribution rates.Additionally,the effects of operating conditions on the properties of solid products are investigated by scanning electron microscopy(SEM)and Raman spectroscopy.The results show that increasing the applied voltage and decreasing CH4 concentration will change the solid carbon from its initial spherical structure into folded multilayer graphene sheets,while the size of the graphene sheets is slightly affected by the change in gas flow rate.
基金supported by National Natural Science Foundation of China(Nos.50908237,51076142)the Open Foundation of the State Key Laboratory of Clean Energy Utilization of China(No.ZJUCEU2009008)
文摘In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the initial concentration increased from 100 mg/L to 160 mg/L, the discolouration rate of AO7 decreased from 99.3% to 95.9%, whereas the COD removal rate decreased from 37.9% to 22.6%. Air provided the best discolouration and COD removal rates （99.3% and 3？.9%, respectively）. In the presence of a zero-valent iron （ZVI） catalyst, the AO？ COD removal rate increased to 76.4%. The degradation products were analysed by a GC-MS, revealing that the degradation of the dye molecule was initiated through the cleavage of the -N=N- bond before finally being converted to organic acids.
基金supported by National Natural Science Foundation of China(No.51576174)
文摘The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external antenna voltage and current increase with the augment of RF power, whereas decline with the enhancement of gas pressure and flow rate conversely.Compared with gas flow rate and pressure, the power transfer efficiency is significantly improved by RF power, and achieved its maximum value of 0.85 after RF power injected excess125 W. Optical emission spectroscopy（OES） provides the local mean values of electron excited temperature and electron density in inductively coupled plasma（ICP） post regime, which vary in a range of 0.81 eV to 1.15 eV and 3.7×10^（16）m^（-3）to 8.7×10^（17）m^（-3）respectively. Numerical results of the average magnitudes of electron temperature and electron density in twodimensional distribution exhibit similar variation trend with the experimental results under different operating condition by using COMSOL Multiphysics. By comprehensively understanding the characteristics in a low pressure ICP, optimized operating conditions could be anticipated aiming at different academic and industrial applications.
基金supported by National Natural Science Foundation of China(No.51576174)China Postdoctoral Science Foundation Funded Project(No.2018M630672)
文摘One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties of the ICPECVD process were revealed via electrical diagnosis and optical emission spectroscopy. The coil current and voltage increased linearly with the augmenting of injected power, and CH, C2, H2 and H were detected at a wavelength from 300 to 700 nm, implying the generation of abundant graphene-building species. The morphology and structure of solid carbon products, graphene nanosheets, were systemically characterized in terms of the variations of operating conditions, such as pressure, temperature, gas proportion, etc. The results indicated that an appropriate operating condition was indispensable for the growth process of graphene nanosheets. In the present work, the optimized result was achieved at the pressure, heating temperature, applied power and gas proportion of 600 mTorr, 800 ~C, 500 W and 20：20：15, respectively, and the augmenting of both CH4 and H2 concentrations had a positive effect on the etching of amorphous carbon. Additionally, H2 and C2 hydrocarbons were detected as the main exhaust gases. The selectivity of H2 and C2H2, measured in exhaust gases, reached up to 52% and 8%, respectively, which implied a process of free radical reactions and electron collision dissociation. Based on a comprehensive investigation of spectral and electrical parameters and synthesized products, the reaction mechanism of collision, dissociation, diffusion, etc, in ICPECVD could be speculated, providing a probable guide for experimental and industrial applications.
文摘A facile and controllable one-step method to treat liquid hydrocarbons and synthesize vertical graphene nanowalls has been developed by using the technique of inductively-coupled plasma-enhanced chemical vapor deposition for plasma cracking of n-dodecane.Herein,the morphology and microstructure of solid carbon material and graphene nanowalls are characterized in terms of different operating conditions,i.e.input power,H2/Ar ratio,injection rate and reaction temperature.The results reveal that the optimal operating conditions were 500 W,5:10,30μl min^-1 and 800℃ for the input power,H2/Ar ratio,injection rate and reaction temperature,respectively.In addition,the degree of graphitization and the gaseous product are analyzed by Raman spectroscopy and gas chromatography detection.It can be calculated from the Raman spectrum that the relative intensity of ID/IG is approximately 1.55,and I2D/IG is approximately 0.48,indicating that the graphene prepared from n-dodecane has a rich defect structure and a high degree of graphitization.By calculating the mass loading and detecting the outlet gas,we find that the cracking rate of n-dodecane is only 6%-7%and that the gaseous products below C2 mainly include CH4,C2H2,C2H4,C2H6 and H2.Among them,the proportion of hydrogen in the outlet gas of n-dodecane cracking ranges from 1.3%-15.1%under different hydrogen flows.Based on our research,we propose a brand new perspective for both liquid hydrocarbon treatment and other value-added product syntheses.
