非平衡等离子体重整甲烷制氢的研究
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摘要
氢能作为一种清洁高效的二次能源,在燃料电池、氢内燃机和汽轮机等应用领域有着广阔的发展前景。但目前氢气的存储和运输技术尚不成熟,因此以天然气为原料的小型分布式制氢系统得以有一席之地。特别是等离子体与非均相催化剂的协同效应在制氢研究中的应用已经受到越来越多的关注。等离子体中存在大量的电子、离子、自由基和激发态原子与分子等活性粒子,等离子体的存在能够促进化学反应快速进行。与传统的热化学方法相比,等离子体转化甲烷制氢具有反应速度快、反应温度低等优点,其装置体积小、启动快,特别适合发展成为车载制氢系统和小型分布式制氢系统。与热等离子体相比,非平衡等离子体能耗低,在较低温度条件下也能诱导反应物发生反应,因此非平衡等离子体应用于气体燃料的转化具有得天独厚的优势。制氢研究中非平衡等离子体的产生方法包括非热电弧放电、火花放电、电晕放电、微波放电和介质阻挡放电等。
基于非平衡等离子体技术为背景,分别进行了介质阻挡放电和非热电弧放电结合催化剂转化甲烷制氢的研究,设计建立了填充床介质阻挡放电反应器、多孔陶瓷介质阻挡放电反应器、非热电弧反应器及配套实验系统,进行了放电实验、制氢实验、数值模拟与反应器结构优化等研究工作。本论文的主要研究内容和结果如下：
提出并构建了电晕诱导介质阻挡放电反应器(放电间隙1Omm),放电区域均匀分布有金属镍粉颗粒,利用颗粒的电晕诱导作用降低了产生放电所需的外加电压,提高放电的均匀性和反应器稳定性。研究大气压较低温度条件下电晕诱导介质阻挡放电反应器内甲烷的部分氧化水蒸气重整制氢。反应器内电晕诱导颗粒的存在使介质阻挡放电可以在大间隙、低电压条件下均匀发生。分析了输入功率、氧气／甲烷摩尔比、以及预热温度对甲烷转化率和氢气选择性的影响。实验结果表明：输入功率在27-50W之间时输入功率的增加明显促进甲烷转化率升高,但当输入功率大于50W时,功率的增加对甲烷转化的促进作用相对较弱；氧气／甲烷摩尔比既影响甲烷转化率,又影响氢气选择性,在本论文实验条件下氧气／甲烷摩尔比为0.6时,氢气的选择性最高能达到112%；电晕诱导介质阻挡放电和催化剂联合作用下的甲烷转化率接近热力学平衡时的甲烷转化率,而前者反应速率明显高于后者。
用造孔剂法制备了一系列氧化铝多孔陶瓷,并研究了多孔陶瓷的材料特性,放电特性。在外加交流高压的条件下,多孔陶瓷内可以产生稳定的大气压微放电。通过对放电的图片以及电压、电流的分析得出微放电的部分物理特性,结果显示陶瓷微孔内的微放电并不是由陶瓷的表面放电转变而成；多孔陶瓷孔内微放电的起始放电电压随着陶瓷厚度增加而升高,而随着多孔陶瓷孔隙率的增加而降低。
催化剂/介质阻挡放电联合作用转化甲烷制氢的结果显示,其甲烷转化率远高于催化剂和介质阻挡放电各自单独作用结果之和；同时金属镍颗粒催化剂的存在降低了介质阻挡放电的放电电压,提高了放电的均匀性和稳定性,证明了催化剂/介质阻挡放电的相互增强作用。介质阻挡放电/催化剂联合作用在于降低反应温度和提高反应速率,相对于介质阻挡放电单独作用降低了能耗,以臭氧产生为例,单纯的介质阻挡放电的电耗高达7kWh/kgO3(反应物为氧气),加入催化剂后电耗降至2.7kWh/kgO3(反应物为氧气)。但介质阻挡放电应用于能源转化可能不合适,从本文试验的结果也可看出：介质阻挡放电消耗高品位的电能活化甲烷分子,提高了被活化甲烷分子的反应速率,但系统不具备良好的经济性。
为提高小型等离子体制氢系统的经济性,设计了非热电弧等离子体结合催化剂重整甲烷制氢反应器,提高非热电弧的非平衡度从而提高等离子体能量效率。研究分析了非热电弧反应器的放电特性和点火性能。当一级旋转气流量大于80sL/min时,非热电弧能不间断产生。氧碳摩尔比率大于0.8时甲烷转化率高于80%,氢气选择性在氧碳摩尔比率较大的变化范围内超过70%。非热电弧反应器最大产氢量为1.07kgH2/h,比电耗在降为0.47MJ/kgH2,具有快速启动性能,预热条件下可在30sec启动制氢,2-3min达到稳定参数,非预热条件下10min以内即可快速启动。
Hydrogen is considered to be an ideal source of energy that could play a key role in fuel cells, combustion engines or gas turbines. Currently, the technology of hydrogen storage and transportation is not yet mature. Consequently, the design and operation of compact and distributed hydrogen production devices has attracted considerable interest for combining plasma-chemical activation of reactants with heterogeneous catalysis in hydrogen production. Compared with traditional chemical processes, plasma technology has the potential to allow design of smaller hydrogen production units with the capability of rapid response to load variations, and to offer a unique way to induce gas phase reactions. Non-equilibrium plasmas have been considered very promising for fuel gas treatment because of their non-equilibrium properties, low power requirement and capacity to induce reactions at relatively low temperatures. Non-equilibrium plasmas that have been applied to hydrogen production include non-thermal arc, spark discharge, corona discharge, microwave discharge and dielectric barrier discharge (DBD).
Base the technology of non-equilibrium plasma, dielectric barrier discharge and non-thermal arc discharge combined with catalyst were used to conversion methane for hydrogen production, respectively. We designed packed-bed dielectric barrier discharge reactor, porous ceramic dielectric barrier discharge reactor, non-thermal arc reactor and supporting experimental system. Discharge experiments, hydrogen production experiments, numerical simulation and reactor structural optimization were conducted. The main research contents and results are as follows:
Larger discharge gap and volume may be important issues to develop a compact DBD reactor as an in situ hydrogen production device. A novel corona inducing dielectric barrier discharge (CIDBD) reactor with discharge gap10mm, with nickel powder uniformly distributed in the discharge zone, was developed to reduce the applied voltage and improve plasma uniformity. This corona inducing technique allows dielectric barrier discharge to occur uniformly in a large gap at relatively low applied voltage. Hydrogen production by reforming methane with steam and air was investigated with the hybrid reactor under atmospheric pressure and temperatures below600℃. The effects of input power, O2/C molar ratio and preheat temperature on methane conversion and hydrogen selectivity were investigated experimentally. It was found that higher methane conversions were obtained at higher discharge power, and methane conversion increased significantly with input power less than50W; the optimized molar ratio of O2/C was0.6to obtain the highest hydrogen selectivity (112%); under the synergy of dielectric barrier discharge and catalyst, methane conversion was close to the thermodynamic equilibrium conversion rate.
Porous ceramics are sintered from alumina (wt94%), silica (wt3.5%) and MgO (wt2.5%), and the thickness range of the ceramics is4.0mm to10.7mm, the pore size of the ceramics is100μm, and the porosities of the ceramics are35%,39%and45%, respectively. We investigate the physical characteristics of discharge in porous ceramics by photographic visualization and electrical measurements. The microdischarges generated inside porous ceramics by AC high voltage represent a novel way to create stable atmospheric pressure plasmas. The physical characteristics of discharge in porous ceramics are investigated by photographic visualization and electrical measurements. Experimental results show that the surface discharge do not transit into pore microdischarges, and the onset voltage of pore microdischarges increases with thickness of ceramics, while significantly decreases with increasing porosity of ceramics.
In order to improve the efficiency of arc discharge energy, we increase non-equilibrium degree of non-thermal arc plasma combined with catalyst. Discharge characteristics and ignition performance of the non-thermal arc reactor were studied. When first rotating gas flow rate greater than80sL/min the non-thermal arc was produced uninterruptedly. The methane conversion rate was higher than80%when the molar ratio of oxygen to carbon greater than0.8. Hydrogen selectivity was higher than70%within large range of variation of the molar ratio of oxygen to carbon. Maximum hydrogen yield of the non-thermal arc reactor is1.07kgH2/h. The specific power consumption of non-thermal arc reactor is0.47MJ/kgH2. The non-thermal arc reactor has fast start-up performance, it can start to produce hydrogen within30seconds at pre-heating condition and reach steady state within3minutes. At non-preheating condition, it can be started to produce hydrogen within10minutes.
基于非平衡等离子体技术为背景,分别进行了介质阻挡放电和非热电弧放电结合催化剂转化甲烷制氢的研究,设计建立了填充床介质阻挡放电反应器、多孔陶瓷介质阻挡放电反应器、非热电弧反应器及配套实验系统,进行了放电实验、制氢实验、数值模拟与反应器结构优化等研究工作。本论文的主要研究内容和结果如下：
提出并构建了电晕诱导介质阻挡放电反应器(放电间隙1Omm),放电区域均匀分布有金属镍粉颗粒,利用颗粒的电晕诱导作用降低了产生放电所需的外加电压,提高放电的均匀性和反应器稳定性。研究大气压较低温度条件下电晕诱导介质阻挡放电反应器内甲烷的部分氧化水蒸气重整制氢。反应器内电晕诱导颗粒的存在使介质阻挡放电可以在大间隙、低电压条件下均匀发生。分析了输入功率、氧气／甲烷摩尔比、以及预热温度对甲烷转化率和氢气选择性的影响。实验结果表明：输入功率在27-50W之间时输入功率的增加明显促进甲烷转化率升高,但当输入功率大于50W时,功率的增加对甲烷转化的促进作用相对较弱；氧气／甲烷摩尔比既影响甲烷转化率,又影响氢气选择性,在本论文实验条件下氧气／甲烷摩尔比为0.6时,氢气的选择性最高能达到112%；电晕诱导介质阻挡放电和催化剂联合作用下的甲烷转化率接近热力学平衡时的甲烷转化率,而前者反应速率明显高于后者。
用造孔剂法制备了一系列氧化铝多孔陶瓷,并研究了多孔陶瓷的材料特性,放电特性。在外加交流高压的条件下,多孔陶瓷内可以产生稳定的大气压微放电。通过对放电的图片以及电压、电流的分析得出微放电的部分物理特性,结果显示陶瓷微孔内的微放电并不是由陶瓷的表面放电转变而成；多孔陶瓷孔内微放电的起始放电电压随着陶瓷厚度增加而升高,而随着多孔陶瓷孔隙率的增加而降低。
催化剂/介质阻挡放电联合作用转化甲烷制氢的结果显示,其甲烷转化率远高于催化剂和介质阻挡放电各自单独作用结果之和；同时金属镍颗粒催化剂的存在降低了介质阻挡放电的放电电压,提高了放电的均匀性和稳定性,证明了催化剂/介质阻挡放电的相互增强作用。介质阻挡放电/催化剂联合作用在于降低反应温度和提高反应速率,相对于介质阻挡放电单独作用降低了能耗,以臭氧产生为例,单纯的介质阻挡放电的电耗高达7kWh/kgO3(反应物为氧气),加入催化剂后电耗降至2.7kWh/kgO3(反应物为氧气)。但介质阻挡放电应用于能源转化可能不合适,从本文试验的结果也可看出：介质阻挡放电消耗高品位的电能活化甲烷分子,提高了被活化甲烷分子的反应速率,但系统不具备良好的经济性。
为提高小型等离子体制氢系统的经济性,设计了非热电弧等离子体结合催化剂重整甲烷制氢反应器,提高非热电弧的非平衡度从而提高等离子体能量效率。研究分析了非热电弧反应器的放电特性和点火性能。当一级旋转气流量大于80sL/min时,非热电弧能不间断产生。氧碳摩尔比率大于0.8时甲烷转化率高于80%,氢气选择性在氧碳摩尔比率较大的变化范围内超过70%。非热电弧反应器最大产氢量为1.07kgH2/h,比电耗在降为0.47MJ/kgH2,具有快速启动性能,预热条件下可在30sec启动制氢,2-3min达到稳定参数,非预热条件下10min以内即可快速启动。
Hydrogen is considered to be an ideal source of energy that could play a key role in fuel cells, combustion engines or gas turbines. Currently, the technology of hydrogen storage and transportation is not yet mature. Consequently, the design and operation of compact and distributed hydrogen production devices has attracted considerable interest for combining plasma-chemical activation of reactants with heterogeneous catalysis in hydrogen production. Compared with traditional chemical processes, plasma technology has the potential to allow design of smaller hydrogen production units with the capability of rapid response to load variations, and to offer a unique way to induce gas phase reactions. Non-equilibrium plasmas have been considered very promising for fuel gas treatment because of their non-equilibrium properties, low power requirement and capacity to induce reactions at relatively low temperatures. Non-equilibrium plasmas that have been applied to hydrogen production include non-thermal arc, spark discharge, corona discharge, microwave discharge and dielectric barrier discharge (DBD).
Base the technology of non-equilibrium plasma, dielectric barrier discharge and non-thermal arc discharge combined with catalyst were used to conversion methane for hydrogen production, respectively. We designed packed-bed dielectric barrier discharge reactor, porous ceramic dielectric barrier discharge reactor, non-thermal arc reactor and supporting experimental system. Discharge experiments, hydrogen production experiments, numerical simulation and reactor structural optimization were conducted. The main research contents and results are as follows:
Larger discharge gap and volume may be important issues to develop a compact DBD reactor as an in situ hydrogen production device. A novel corona inducing dielectric barrier discharge (CIDBD) reactor with discharge gap10mm, with nickel powder uniformly distributed in the discharge zone, was developed to reduce the applied voltage and improve plasma uniformity. This corona inducing technique allows dielectric barrier discharge to occur uniformly in a large gap at relatively low applied voltage. Hydrogen production by reforming methane with steam and air was investigated with the hybrid reactor under atmospheric pressure and temperatures below600℃. The effects of input power, O2/C molar ratio and preheat temperature on methane conversion and hydrogen selectivity were investigated experimentally. It was found that higher methane conversions were obtained at higher discharge power, and methane conversion increased significantly with input power less than50W; the optimized molar ratio of O2/C was0.6to obtain the highest hydrogen selectivity (112%); under the synergy of dielectric barrier discharge and catalyst, methane conversion was close to the thermodynamic equilibrium conversion rate.
Porous ceramics are sintered from alumina (wt94%), silica (wt3.5%) and MgO (wt2.5%), and the thickness range of the ceramics is4.0mm to10.7mm, the pore size of the ceramics is100μm, and the porosities of the ceramics are35%,39%and45%, respectively. We investigate the physical characteristics of discharge in porous ceramics by photographic visualization and electrical measurements. The microdischarges generated inside porous ceramics by AC high voltage represent a novel way to create stable atmospheric pressure plasmas. The physical characteristics of discharge in porous ceramics are investigated by photographic visualization and electrical measurements. Experimental results show that the surface discharge do not transit into pore microdischarges, and the onset voltage of pore microdischarges increases with thickness of ceramics, while significantly decreases with increasing porosity of ceramics.
In order to improve the efficiency of arc discharge energy, we increase non-equilibrium degree of non-thermal arc plasma combined with catalyst. Discharge characteristics and ignition performance of the non-thermal arc reactor were studied. When first rotating gas flow rate greater than80sL/min the non-thermal arc was produced uninterruptedly. The methane conversion rate was higher than80%when the molar ratio of oxygen to carbon greater than0.8. Hydrogen selectivity was higher than70%within large range of variation of the molar ratio of oxygen to carbon. Maximum hydrogen yield of the non-thermal arc reactor is1.07kgH2/h. The specific power consumption of non-thermal arc reactor is0.47MJ/kgH2. The non-thermal arc reactor has fast start-up performance, it can start to produce hydrogen within30seconds at pre-heating condition and reach steady state within3minutes. At non-preheating condition, it can be started to produce hydrogen within10minutes.
引文
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