含湿量对甲烷湿空气自热重整积碳特性的影响

微动力装置中碳氢燃料催化燃烧被认为是有效的方法,但燃烧室内燃料催化重整普遍存在由积碳导致的催化剂失活等问题.本文采用数值方法研究了微细腔中甲烷湿空气在镍基催化剂上的自热重整反应,重点分析含湿量对甲烷自热重整反应及积碳特性的影响.结果表明:含湿量将增强甲烷重整反应;自热反应散热量和表面积碳浓度均随含湿量增加而降低.混合物...     

基于多物理场模拟的低水甲烷燃料固体氧化物燃料电池的抗积碳阳极设计（英文）

本文采用与实验I-V曲线高度吻合的多物理场全耦合数值模型来模拟低水甲烷燃料SOFC的运行过程.基于抗积碳电流密度实验数据推导出的动力学积碳活性判据,利用多场耦合数值模型系统研究了电池工作参数和阳极扩散阻碍层厚度对阳极积碳倾向的影响.仿真模拟揭示了燃料利用率、电流密度、扩散阻碍层厚度和电池工作电压的相互关系.结果表明,在阳极添加400 um厚的扩散阻碍层是实现SOFC高功率密度和不积碳运行的最优设计.这种阳极结构设计对实现高效率低成本的SOFC技术具有重要意义.     

氧碳比对微细腔内自热重整积碳的影响

针对微动力装置中重整腔内强吸热重整反应和催化剂积碳等问题,耦合甲烷部分氧化反应,实现系统自供热并抑制积碳.为了优化微细腔内甲烷湿空气自热重整反应条件,采用数值方法研究预热温度为800 K,不同水碳比下,氧碳比对绝热的微细腔内甲烷湿空气自热重整反应的影响.结果表明:反应气中水碳比为1～2.5,微细腔内甲烷湿空气自热重整的...     

基于多物理场模拟的低水甲烷燃料固体氧化物燃料电池的抗积碳阳极设计

本文采用与实验I-V曲线高度吻合的多物理场全耦合数值模型来模拟低水甲烷燃料SOFC的运行过程. 基于抗积碳电流密度实验数据推导出的动力学积碳活性判据,利用多场耦合数值模型系统研究了电池工作参数和阳极扩散阻碍层厚度对阳极积碳倾向的影响. 仿真模拟揭示了燃料利用率、电流密度、扩散阻碍层厚度和电池工作电压的相互关系. 结果表明,在阳极添加400 um厚的扩散阻碍层是实现SOFC高功率密度和不积碳运行的最优设计. 这种阳极结构设计对实现高效率低成本的SOFC技术具有重要意义.     

微细腔内变组分CH_4/O_2/H_2O自热重整积碳特性

针对微动力装置中重整腔内催化剂表面容易积碳,重整反应需要大量能量等问题,在重整腔入口引入氧气,使甲烷发生部分氧化反应为催化重整提供热量。本文采用数值方法研究了微细腔中CH_4/O_2/H_2O镍基催化剂上的自热重整反应,重点分析CH_4/O_2/H_2O混合物组分对甲烷自热重整反应及积碳的影响。结果表明:在混合物组分CH_4/O_2/H_2O摩尔比为1:0.2:2时,甲烷自热反应放热量刚好能满足甲烷重整反应的需求,氢气质量分数较高为3.32%,积碳浓度较低为1.19×10~(-6) kmol/m~2。     

基于磁动力学方程的电流感应磁化翻转效应的宏观模型

提出了一个基于磁动力学方程的宏观唯象理论模型，对纳米级赝自旋阀结构的电流感应磁化翻转效应给出了明晰的物理解释：流入自由层的净自旋流和自由层内的自旋弛豫过程的共同作用，导致自由层总磁矩随时间的改变，甚至产生磁化方向的翻转.模型将“铁磁/非铁磁”界面的自旋相关散射，以及铁磁层中的自旋积累和弛豫过程，统一于宏观的磁动力学方程中.通过求解该方程的解析解，给出了赝自旋阀在电流激励下的磁化翻转条件和临界电流密度的表达式.对该效应的定性解释和数值模拟结果都和实验报道良好符合.根据模型分析了影响临界电流密度的诸因素，并指出提高器件性能的途径. 关键词： 电流感应磁化翻转 磁动力学方程 自旋电子学     

微重力池沸腾现象中的临界热流密度

本文利用我国第22颗返回式卫星实验研究了微重力条件下池沸腾临界热流现象,发现基于流体动力学不稳定性机制的LD-Zuber模型可以很好地预测不同重力条件下的池沸腾临界热流变化趋势,尽管热丝无量纲半径比该模型的适用范围扩大了3～4个数量级.这和地面常重力环境中关于临界热流尺度效应的研究结果有很大差异,表明在Bond数很小时,热丝无量纲半径已不再是描述临界热流尺度效应的唯一参数.此外,本文提出了"极限核化尺寸"的概念,来解释了不同条件下临界热流的变化特征.     

多孔介质内反应气的化学和热质非同性传递过程特性

针对集成板式固体氧化物燃料电池,建立了数学物理模型,分析阳极侧多孔支撑层内富氢气体的内重整反应传递过程特性.讨论了操作温度、入口处H2O:CH4比值以及多孔材料的孔隙率对甲烷蒸汽重整转换率和氢气的生成量的影响,得到了在电池的一定运行工况范围内比较有利的反应条件.     

催化剂薄层内甲烷水蒸气重整反应强化管内对流换热的数值模拟

本文以竖直圆管内壁催化剂薄层内发生甲烷水蒸气重整反应强化对流换热作为研究对象,对其进行了数值模拟．结果发现,催化剂薄层内的吸热化学反应可以有效地强化对流换热,降低流体和壁面温度,从而对壁面起到保护作用;极限热流密度的大小与流体的入口温度有关,存在最佳入口温度使极限热流密度最大．     

电流对苯甲醚电催化重整过程的影响

用电催化重整方法和NiCuZn-Al₂O₃催化剂进行生物油模型化合物苯甲醚的水蒸气重整制氢研究,结果表明,在700 oC和4 A条件下,获得的最高碳转化率和氢产率分别为98.3%和88.7%,电催化重整过程中发现的电流促进效应主要归结于重整反应床中温度分布的改变和电阻丝发射的热电子影响. 利用X射线衍射方法分析了反应前后的NiCuZn-Al₂O₃催化剂结构变化. 实验导出的苯甲醚重整反应表观活化能为99.54 kJ/mol,明显高于乙醇、乙酸和生物油轻质组分的重整反应表观活化能.     

Internal reforming in intermediate temperature solid oxide fuel cells running on natural gas

Methane steam reforming has been studied over a range of nickel/ceria-gadolinia cermet anodes, over the temperature range 500–700 °C appropriate for intermediate temperature ceriagadolinia based SOFCs. The influence of operating temperature and methane/steam ratio on the reforming characteristics, methane conversion and product selectivity, and the carbon deposition on the anode during reforming, has been determined for each anode. Nickel/ceria powders made from gas atomised intermetallic precursors have been studied as potential anode materials for intermediate temperature ceria-gadolinia based SOFCs running on natural gas. The powders have been characterised structurally and evaluated for their methane reforming characteristics and their resistance to carbon deposition during internal reforming, especially at low steam/methane ratios, over the relevant operating temperature ranges of ceriagadolinia based SOFCs. Their performance has been compared to conventionally prepared anodes and anodes generated from cast alloys, with very favourable results. Paper presented at the 9th EuroConference on Ionics, Ixia, Rhodes, Greece, Sept. 15 – 21, 2002.     

Sites for catalysis and electrochemistry in solid oxide fuel cell (SOFC) anode

Fuel cells represent a challenging overlap of catalysis and electrochemistry. This is illustrated by anode reactions in a solid oxide fuel cell. The sites for catalytic conversion of methane and electrochemical conversion of hydrogen on an SOFC anode appear not to be the same. The fuel (methane, hydrogen, etc.) is activated by chemisorption on the nickel surface of the anode. This is linked to the electrochemical reaction at the interface of the electrolyte and the nickel crystals converting oxygen ions into electrons and water by reactions with adsorbed hydrogen atoms resulting from the activation of the fuel. The sites for these reactions appear not to be the same. This is reflected by different sensitivities of the two steps to sulphur poisoning. The role of different sites on the nickel surface for the steam reforming reaction is well understood in terms of impact on activity for methane activation, carbon formation and sintering. The study is supplemented by an analysis of anodes having been exposed to 13000 of operation using a number of characterisation methods. PACS 82.47.Ed; 82.45.-h; 82.65.-s     

Interrelation of anode and cathode processes in electrochemical carbon oxidation in a fuel cell with molten carbonate electrolyte

The object to be investigated is a fuel cell with a free molten carbonate electrolyte, which ensures direct electrochemical oxidation of solid hydrocarbons. The polarization characteristics of anode and cathode fuel cell assemblies, and also composition and gas release rate of gaseous products of anode reactions are studied. It is shown that the maximum voltages in the open cell circuit are obtained when the oxygen-carbon dioxide ratio in the cathode gas mixture corresponds to stoichiometric reaction coefficients that ensure replenishment of ions in electrolyte. However, the maximum current density values were obtained with a low carbon dioxide content. It is found that at high current values, anode potential fluctuations are observed. It is shown that carbon monoxide is the product of anode processes, along with carbon dioxide. The carbon monoxide content grows with temperature. The carbon dioxide content grows with increasing current in the fuel cell and with growing carbon dioxide content in cathode gases. The release rate of carbon oxidation products nonlinearly depends on the current value in the fuel cell. It is concluded that there is interrelation between the mass-exchange processes in the fuel cell, which is determined by the balance between cathode gas incoming into the reaction zone, the number of molecules generated during fuel oxidation, molecule dissolution and diffusion into the cathode region, and also the amount of gas released in the form of bubbles.     

一类煤与天然气互补利用的新型发电系统

提出一种新型发电系统,通过煤和天然气的互补利用来减少能量转化过程的不可逆损失。煤气化炉采用空气和水蒸气做氧化剂,碳转化率约为60%,未转化部分形成半焦,半焦燃烧释放的热量驱动天然气重整反应,制取合成气。煤部分气化所得气化煤气和半焦燃烧驱动天然气重整所得合成气混合,作为联合循环的燃料。结果显示,新系统的热效率为51.5%,效率为50.3%,天然气折合发电效率为61%。新系统为高效合理利用煤和天然气提供了一种新途径。     

Effect of nitrogen and carbon dioxide as fuel impurities on PEM fuel cell performances

Polymer electrolyte membrane (PEM) fuel cells are considered to have the highest power density of all the fuel cells. They operate on hydrogen fuel, which is generally produced by reforming of hydrocarbons, and may contain large amounts of impurities such as carbon dioxide, nitrogen, and trace amounts of carbon monoxide. We studied the effect of dilution of hydrogen gas with carbon dioxide on PEM fuel cells by polarization studies. The polarization curves were different when hydrogen gas was diluted with same quantities of carbon dioxide and with nitrogen. It may be due to carbon monoxide formation by reverse shift reaction and poisoning of anode platinum catalyst. Use of Pt–Ru alloy catalyst was found to suppress the poisoning. The effects of hydrogen gas composition, temperature, current density, and anode catalyst on fuel cell performances were examined in this study.     

Samaria-doped Ceria Modified Ni/YSZ Anode for Direct Methane Fuel in Tubular Solid Oxide Fuel Cells by Impregnation Method

以NiO和8%(摩尔分数)氧化钇稳定的氧化锆为原料,采用注凝成型工艺制备了管状固体氧化物燃料电池阳极支撑体．用离子浸渍法对阳极支撑体进行表面修饰．用电化学工作站测单电池交流阻抗和输出性能并且用化学气相色谱仪对电池尾气进行分析．测试结果表明修饰后的阳极在通甲烷的情况下出现了一定程度的积炭,但是积炭现象在一定的测试时间内达到平衡,没有对电池造成破坏,并且显著地提高了电池阳极的电化学性能．单电池在通入氢气和甲烷的情况下最大输出功率密度分别达到了225和400 mW/cm²．     

Performance of a tubular solid oxide fuel cell with model kerosene reformate gas

A performance of an anode-supported tubular Ni–8YSZ/Ni–ScSZ/ScSZ/GDC/LSC cell was investigated at 650–750 °C by feeding model kerosene reformate gas (H₂, H₂O, CO, CO₂, and CH₄) to a Ni–8YSZ/Ni–ScSZ anode. Variations of gas composition were observed not only between inlet and outlet of anode to estimate the degree of internal reforming, but also during current input by online quadrupole mass spectrometry and Fourier-transform infrared spectrometry.The electrochemical performance of the cell was independent of reforming temperature of kerosene, i.e. gas composition (in particular CH₄ concentration) at moderate anode gas flow rates. At open-circuit states, 10% or less methane in the kerosene-reformed gas was readily converted by steam or CO₂ over the Ni–8YSZ/Ni–ScSZ electrode so that gas compositions could almost follow the thermodynamic equilibrium at 650–750 °C. This suggests that the internal reforming should proceed almost completely over the Ni anode. Consumption of H₂ and CO and production of CO₂ were observed during current input. I–V characteristics remained constant at 650 °C as long as anodic W/F was more than 0.2 kg mmol^− 1 s. It was demonstrated that a catalytic activity of an anode electrode for hydrocarbons will be important for SOFCs with liquid fuels such as kerosene in order not to deteriorate cell performance.     

小分子醇对天然气发动机热化学重整的影响

天然气发动机缸内热化学重整技术对于开发新型的满足更严格排放法规的天然气发动机有着重要意义,为了探究不同醇类对缸内热化学重整影响的化学反应动力学机理,本文选取甲醇、乙醇与乙二醇三种小分子醇作为加浓燃料,通过流动反应器实验和CHEMKIN模拟,对三者掺混时重整气的生成量以及甲烷的消耗量进行了对比,并对反应路径进行了分析以判断不同燃料掺混产生差异的原因,通过分组对比探讨了醇类燃料碳链长度与羟基数目对重整效果的影响.通过研究发现,小分子醇的碳链长度相同时,羟基数目增加有利于促进重整过程;羟基数目相同时,碳链长度缩短有利于促进重整过程。     

新型多能源互补系统的热力经济性分析

本文对SOLRGT系统（一种新型的中低温太阳能与化石燃料互补的动力系统）进行了热力经济性分析。该系统基于化学回热循环,通过中低温太阳能品位的间接提升、与先进燃气轮机的集成,实现中低温太阳能的高效、低成本热功转换以及和化石燃料的综合梯级利用。本文将其与同等输入下的两种单输入发电系统进行对比分析,研究表明：基本工况下,SO...