阳极支撑型固体氧化物燃料电池内多物理场传递过程的机理与数值分析
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摘要
固体氧化物燃料电池(SOFC)是一种工作在600-1000℃,采用固态陶瓷材料作为传导氧离子电解质的能源转换装置。SOFC具有效率高、污染小、输出功率大、适用燃料广泛、只有气固两相介质、工作原理简单等优点,被认为是最有发展前途的燃料电池之一。阳极支撑型平板SOFC具有较厚的阳极,和相对较低的工作温度。本文建立的三维稳态的阳极支撑型SOFC单电池模型,可描述发生在SOFC内的多物理场过程,其中包括：甲烷蒸汽重整(MSR)、水汽转换反应(WGSR)和电化学反应,以及质量、动量、热量、电荷(电子和氧离子)等传递过程。通过商业CFD软件(Ansys/Fluent12.1)的模拟计算,辅以电流密度、电压与功率密度等试验数据验证,得到相对合理的计算结果,并分析和讨论温度、多孔介质参数,燃料种类、气体通道分布等因素对SOFC中宏观气体反应与传热传质过程的影响。此外以42步单向基元反应机理描述了发生在SOFC多孔阳极上催化材料Ni表面的内重整反应,在表面催化反应的层面上分析了SOFC阳极中多物理场之间的耦合关系。
通过分析发现,如果用单电池的宏观气体反应模型,温度由进口侧沿主流道方向升高,其中出口侧靠近电解质的区域温度最高；阳极中的内重整反应主要发生在阳极顶部靠近气体通道的区域,为电化学反应提供了足够的H2同时消耗了电化学产生的H2O和热量;800℃时CH4的最大转换率只有59.1%,同时H2摩尔分数减少10%,电化学反应较强；电化学反应集中在电解质附近的区域,其中阴极与阳极电化学反应层分别为10um和20um; SOFC中电流密度和电压分布不均匀,受到气体通道、不同区域的温度、气体浓度分布等影响；在给定0.7V的操作电压下,SOFC中总的过电势损失约0.3V,其中阳极和阴极侧的活化过电压分别占70%和20%;操作温度提高50℃,离子和电子电流密度(Iion和Ie)分别提高37.5%和28.6%,电化学和内重整反应加强；多孔介质单位体积表面积提高10倍,电流密度增加53%,电化学反应层厚度减半,活化过电压损失减少40%;如果燃料成分中CH4摩尔分数减少90%, MSR减弱、WGSR增强,温度升高6-10℃；表面催化反应计算结果模型显示Nis(65%)、COS(26%)、Hs(7%)和Os(1%)是几种主要的表面成分;温度增加、多孔介质渗透率增大都会促进Nis增加,HsCOs等下降：不同的基元反应对整个内重整反应的温度、气体分布等会产生不同程度的影响。
Solid oxide fuel cell (SOFC) is one kind of fuel cells with ceramic materials as electrolyte, which can work between600-1000℃. There are many advantages associated with SOFCs which has been recognized as one of the most promising fuel cells in the future, such as high efficiency, low pollution, high power output, flexible fuel supply, simple operational principles. Anode-supported plannar SOFC with thick anode layer can work in relative lower temperature. A3D steady CFD model of a single cell unit has been developed to evaluate the multi-physics processes in SOFCs, including methane steam reforming (MSR), water-gas shift reaction (WGSR) and electrochemical reactions, and the transport processes of mass, momentum, heat and charge (ion/electron). The commercial CFD code Ansys/Fluent12.1has been employed for numerical simulation calculation, and the experimental data of current density, voltage, power density have been used to validate the models and the calculation results. A parameter study is conducted to analyse the effects on the reactions and the transport processes by changing some conditions, such as temperature, porous structures, fuel compositon and gas channel arrangment in SOFCs. Similarly, a3D steady CFD model is developed for the SOFC anode by implementing the42-step elementary reaction mechanism to evaluate the catalytic reactions between the gases and the catalyst (Ni) in the anode porous structure, based on the internal reforming reactions coupled with mass and heat transfer processes.
According to the prediction of the globle gas reaction model in the single cell, the temperature distribution increases along the main flow direction from the inlet, and a maximum value occurs at the electrolyte near the outlet. The internal reforming reactions, which provide H2and consume H2O and heat from the electrochemical reaction near the electrolyte, are stronger in the anode layer close to the fuel channel. The conversion rate of CH4is about59%, while the molar fraction of hydrogen XH2decreases by10%at800℃, which means that the electrochemical reaction is stronger than internal reforming reactions; Regarding to the electrochemical reaction which occurrs in the active layer near the electrolyte, its thickness is about20um in the anode side and10um in the cathode side. The distribution of the current density and the potential is not even, which has been affected by the gas channel, temperature and gas distribution; The total potential losses is0.3V, in which the active overpotential in the anode and the cathode side is about70%and20%, respectively, when the operational voltage is set to0.7V. The current density Iion and Ic increase37.5%and28.6%, respectively, when the temperature is50℃higher. It means that the reforming and electrochemical reactions are stronger; When the permeability is10times bigger, the current density increases about53%, the active overpotential decreases40%, and the thickness of reaction region decreases, the rate of MSR decreases, working temperature becomes high (6-10℃), and the rate of WGSR increases when the molar fraction of CH4has been decreased to10%; There are four major surface species identified, including Nis(65%), COS(26%), Hs(7%) and Os(1%), as predicted by the catalytic surface reaction model; high operating temperature and permeability can improve the reactions towards to the desperation reactions to release more Nis while consume more Hs and COS; It is also found that the temperature, gas species can be affected by each elementary reaction steps.
通过分析发现,如果用单电池的宏观气体反应模型,温度由进口侧沿主流道方向升高,其中出口侧靠近电解质的区域温度最高；阳极中的内重整反应主要发生在阳极顶部靠近气体通道的区域,为电化学反应提供了足够的H2同时消耗了电化学产生的H2O和热量;800℃时CH4的最大转换率只有59.1%,同时H2摩尔分数减少10%,电化学反应较强；电化学反应集中在电解质附近的区域,其中阴极与阳极电化学反应层分别为10um和20um; SOFC中电流密度和电压分布不均匀,受到气体通道、不同区域的温度、气体浓度分布等影响；在给定0.7V的操作电压下,SOFC中总的过电势损失约0.3V,其中阳极和阴极侧的活化过电压分别占70%和20%;操作温度提高50℃,离子和电子电流密度(Iion和Ie)分别提高37.5%和28.6%,电化学和内重整反应加强；多孔介质单位体积表面积提高10倍,电流密度增加53%,电化学反应层厚度减半,活化过电压损失减少40%;如果燃料成分中CH4摩尔分数减少90%, MSR减弱、WGSR增强,温度升高6-10℃；表面催化反应计算结果模型显示Nis(65%)、COS(26%)、Hs(7%)和Os(1%)是几种主要的表面成分;温度增加、多孔介质渗透率增大都会促进Nis增加,HsCOs等下降：不同的基元反应对整个内重整反应的温度、气体分布等会产生不同程度的影响。
Solid oxide fuel cell (SOFC) is one kind of fuel cells with ceramic materials as electrolyte, which can work between600-1000℃. There are many advantages associated with SOFCs which has been recognized as one of the most promising fuel cells in the future, such as high efficiency, low pollution, high power output, flexible fuel supply, simple operational principles. Anode-supported plannar SOFC with thick anode layer can work in relative lower temperature. A3D steady CFD model of a single cell unit has been developed to evaluate the multi-physics processes in SOFCs, including methane steam reforming (MSR), water-gas shift reaction (WGSR) and electrochemical reactions, and the transport processes of mass, momentum, heat and charge (ion/electron). The commercial CFD code Ansys/Fluent12.1has been employed for numerical simulation calculation, and the experimental data of current density, voltage, power density have been used to validate the models and the calculation results. A parameter study is conducted to analyse the effects on the reactions and the transport processes by changing some conditions, such as temperature, porous structures, fuel compositon and gas channel arrangment in SOFCs. Similarly, a3D steady CFD model is developed for the SOFC anode by implementing the42-step elementary reaction mechanism to evaluate the catalytic reactions between the gases and the catalyst (Ni) in the anode porous structure, based on the internal reforming reactions coupled with mass and heat transfer processes.
According to the prediction of the globle gas reaction model in the single cell, the temperature distribution increases along the main flow direction from the inlet, and a maximum value occurs at the electrolyte near the outlet. The internal reforming reactions, which provide H2and consume H2O and heat from the electrochemical reaction near the electrolyte, are stronger in the anode layer close to the fuel channel. The conversion rate of CH4is about59%, while the molar fraction of hydrogen XH2decreases by10%at800℃, which means that the electrochemical reaction is stronger than internal reforming reactions; Regarding to the electrochemical reaction which occurrs in the active layer near the electrolyte, its thickness is about20um in the anode side and10um in the cathode side. The distribution of the current density and the potential is not even, which has been affected by the gas channel, temperature and gas distribution; The total potential losses is0.3V, in which the active overpotential in the anode and the cathode side is about70%and20%, respectively, when the operational voltage is set to0.7V. The current density Iion and Ic increase37.5%and28.6%, respectively, when the temperature is50℃higher. It means that the reforming and electrochemical reactions are stronger; When the permeability is10times bigger, the current density increases about53%, the active overpotential decreases40%, and the thickness of reaction region decreases, the rate of MSR decreases, working temperature becomes high (6-10℃), and the rate of WGSR increases when the molar fraction of CH4has been decreased to10%; There are four major surface species identified, including Nis(65%), COS(26%), Hs(7%) and Os(1%), as predicted by the catalytic surface reaction model; high operating temperature and permeability can improve the reactions towards to the desperation reactions to release more Nis while consume more Hs and COS; It is also found that the temperature, gas species can be affected by each elementary reaction steps.
引文
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