气体流场与组分对单室燃料电池微堆性能影响机制研究
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摘要
单室固体氧化物燃料电池（SC-SOFC）所具有的结构简单、无需密封等优点使其在便携式发电装置领域呈现出很好的应用前景，但是此前关于该领域的研究主要集中在对单电池的材料、结构和运行条件等方面，对于电池堆的研究比较少，且输出功率不高。本文通过理论模拟和实验验证相结合的方法，针对气体流场分布、供气方式以及气体组分等因素对SC-SOFC微堆性能的影响机制进行研究，创造性的提出了一种双路多点供气的电池微堆结构设计方案，显著提高了SC-SOFC微堆的输出电压和输出功率。
由于SC-SOFC的阴极和阳极处于燃料和氧气的混合气氛下进行工作，气室内部的混合气体在电极附近的分布情况是影响电池输出性能的一个重要因素。本文对混合气体平行流经单电池的两个电极和分别垂直流经电池的阴极和阳极进行了研究，首先通过数值模拟分析了影响机制，继而进行了实验验证。理论模拟和实验验证的结果都表明，气流垂直流过阳极时存在阳极对阴极氧气的争夺，导致阴极的氧分压降低，尽管此时电池的实际温度较高，但电池的开路电压和输出性能却比其他两种结构更差。在此基础上，运用阳极与阴极的气体争夺机制，研究了由两个电池组成的阳极与阴极相对的微堆，数值模拟的结果证明电池间距是影响此种结构微堆输出性能的重要因素。电池间距越小，位于微堆中间位置的阴极表面氧分压越低；当电池间距较大、更靠近气室壁时，影响的是位于电池微堆外侧阴极的氧分压，间距越大，外侧阴极的氧分压越低。针对阳极部分氧化放热反应提高电池实际温度的现象，对具有阳极与阳极相对的微堆结构进行数值模拟，发现此时电池自发放热产生的高温区主要分布于两个电池之间的区域，并且整个区域内的温度均匀，有利于实现微堆的热自维持。
对多个电池组成的微堆进行温度场和气体组分分布的数值模拟，发现传统的单一通气管供气方式很难保证微堆中每个单电池获得的反应气体组分均匀。为了使气流前端和后端的电池获得相同的气体比例和组分，减小气流前端电池对下游电池的影响，本文发明了一种采用分散通气口为SC-SOFC微堆中的每个单电池提供反应气体的多点供气新方法，通过与传统SC-SOFC流场沿管状气室流动的供气方式进行了对比，发现这种多点供气方式可以使电池微堆中的每个单电池达到较为一致的输出性能，从而使微堆的输出功率也高于采用传统SC-SOFC供气方式时的性能。
考虑到电池阳极和阴极之间气体争夺的问题，提出了使用两个通气管同时给单电池的阴极和阳极提供相同比例的反应气体的方法，结果表明单电池的输出性能比传统的SC-SOFC提高了67%。继而在单路多点提供混合反应气的基础上，发明了双路多点供气的SC-SOFC微堆，并对几组不同构型的微堆进行研究。结果表明，平面嵌入式电池微堆的输出性能最佳，由两个有效面积为1.2cm~2的单电池组成的微堆输出功率可以达到1W，6个有效面积约为3.9cm~2单电池组成的SC-SOFC微堆模块最大功率达到8.18W，这种电池将来有望成为便携式的备用电源的核心部件。
针对SC-SOFC采用碳氢化合物燃料时阳极可能存在的碳沉积问题以及金属Ni在燃料和氧气的混合气氛中的氧化还原现象，研究了CH_4和O_2的混合气体组分对SC-SOFC阳极的影响机制。用气体质谱分析仪研究了Ni/YSZ阳极对甲烷和氧气混合气体的催化性能，发现甲烷和氧气的比例（燃氧比R）为1时发生的反应以甲烷的完全氧化反应为主导，而燃氧比大于1时则以甲烷的部分氧化反应为主。在700°C进行5h短期测试，发现燃氧比为2.5时既没有明显积碳，也没有金属镍被氧化的现象，对于SC-SOFC的Ni/YSZ阳极是比较合理的气体比例。
SC-SOFC has received considerable attention for the portable applications due tothe sealing-free and simple gas management. However, current researches focusprimarily on the single cells. Studies of the SC-SOFC stack are also confined to the lowpower output. This paper provides a detailed study on the SC-SOFC stack essentialparameters, including the gas flow field distribution, gas supply method and gascomponent of SC-SOFC, by using the theoretical and experimental methods. ASC-SOFC stack with dual gas supply method is proposed for the first time.
As the SC-SOFC worked in the fuel and air mixture, gas flow distribution is animportant factor limiting the cell performance. Numerical simulation and experimentalverification are studied with different gas flow distribution. Results showed that thepartial pressure of oxygen at the cathode side of the cell with gas flow direction facingthe anode was very low, which was caused by the catalytic reaction at the anode. Theperformance of the cells with gas flow direction facing the cathode and parallel to theelectrodes were nearly the same. Numerical simulation of the SC-SOFC stack wasstudied due to the gas competition between the anode and cathode. The cell distance ofan anode-facing-cathode two cell stack influences the performances of the cells.Numerical simulation showed that the partial pressure of oxygen and surface temperatureof the cathode facing the narrow gas path is influenced obviously with smaller spacing.While the oxygen partial pressure of the cathode on the outside is influenced with largerspacing. Numerical simulation of the two cell stack with anode-facing-anodeconfiguration was also studied. Results showed that the heat released by the exothermicreaction of the anodes is concentrated between the cells, which is propitious to achievethe thermally self-sustained of SC-SOFC stack.
Numerical simulation showed that the performances of the cells of SC-SOFC microstack with traditional gas supply method are seriously limited by the uneven flowgeometry, where the downstream portion of the stack is exposed to by-products resultingfrom fuel oxidation in the upstream portion of the stack. In view of this problem, a novelgas supply method with multi-point gas vents in the gas tube is proposed in this paper.The traditional gas supply method was also investigated for comparison. Experimentalresults showed that the single cells could obtain a uniform open-circuit voltage andpower output by using the separated gas supply method. For the traditional gas supplymethod, the cell at the outlet position yielded inferior performance compared to that ofthe inlet cell. Finally, the stack operated with the multi-point gas supply methodproduced a higher power output than that operated with the traditional gas supplymethod.
In view of the gas competition between the anode and cathode, dual gas supplymethod for anode and cathode by using multi-point gas transmission tubes is proposed.The performance of the cell with dual gas supply method was increased by67%than thatof the conventional SC-SOFC. As a result, several SC-SOFC micro-stacks with two gastubes were studied. The cells with an anode-facing-cathode configuration were connectedin serial by zigzag sliver sheets. The maximum power output are192,230and276mWat CH_4flow rate of50,70and100sccm, respectively. The performance of SC-SOFCmicro-stacks with congener-electrode-facing configuration was better than that of theanode-facing-cathode configuration stack. A two-cell SC-SOFC stack with cellsembedded in plane configuration demonstrated a maximum power output of1.04W atthe flow rate of260sccm CH_4and130sccm O_2. Finally, a scaled-up stack with six cellsin series generated an OCV of6.4V and a maximum power output of8.18W.
Consider of carbon deposition and oxidation of Ni metal at the Ni/YSZ anode inCH_4/O_2gas mixture, influencing mechanism of CH_4/O_2gas component over Ni/YSZanode was studied by using gas mass spectrometer. Results showed that completeoxidation of CH_4was the main reaction with the CH_4/O_2ratio of1. Partial oxidationreaction of CH_4was the main reaction with higher CH_4/O_2ratio. Neither carbondeposition occurs nor nickel protoxide be observed at CH_4/O_2ratio of2.5at700°C,which is a reasonable proportion of CH_4and O_2for the Ni/YSZ anode of SC-SOFC.
由于SC-SOFC的阴极和阳极处于燃料和氧气的混合气氛下进行工作，气室内部的混合气体在电极附近的分布情况是影响电池输出性能的一个重要因素。本文对混合气体平行流经单电池的两个电极和分别垂直流经电池的阴极和阳极进行了研究，首先通过数值模拟分析了影响机制，继而进行了实验验证。理论模拟和实验验证的结果都表明，气流垂直流过阳极时存在阳极对阴极氧气的争夺，导致阴极的氧分压降低，尽管此时电池的实际温度较高，但电池的开路电压和输出性能却比其他两种结构更差。在此基础上，运用阳极与阴极的气体争夺机制，研究了由两个电池组成的阳极与阴极相对的微堆，数值模拟的结果证明电池间距是影响此种结构微堆输出性能的重要因素。电池间距越小，位于微堆中间位置的阴极表面氧分压越低；当电池间距较大、更靠近气室壁时，影响的是位于电池微堆外侧阴极的氧分压，间距越大，外侧阴极的氧分压越低。针对阳极部分氧化放热反应提高电池实际温度的现象，对具有阳极与阳极相对的微堆结构进行数值模拟，发现此时电池自发放热产生的高温区主要分布于两个电池之间的区域，并且整个区域内的温度均匀，有利于实现微堆的热自维持。
对多个电池组成的微堆进行温度场和气体组分分布的数值模拟，发现传统的单一通气管供气方式很难保证微堆中每个单电池获得的反应气体组分均匀。为了使气流前端和后端的电池获得相同的气体比例和组分，减小气流前端电池对下游电池的影响，本文发明了一种采用分散通气口为SC-SOFC微堆中的每个单电池提供反应气体的多点供气新方法，通过与传统SC-SOFC流场沿管状气室流动的供气方式进行了对比，发现这种多点供气方式可以使电池微堆中的每个单电池达到较为一致的输出性能，从而使微堆的输出功率也高于采用传统SC-SOFC供气方式时的性能。
考虑到电池阳极和阴极之间气体争夺的问题，提出了使用两个通气管同时给单电池的阴极和阳极提供相同比例的反应气体的方法，结果表明单电池的输出性能比传统的SC-SOFC提高了67%。继而在单路多点提供混合反应气的基础上，发明了双路多点供气的SC-SOFC微堆，并对几组不同构型的微堆进行研究。结果表明，平面嵌入式电池微堆的输出性能最佳，由两个有效面积为1.2cm~2的单电池组成的微堆输出功率可以达到1W，6个有效面积约为3.9cm~2单电池组成的SC-SOFC微堆模块最大功率达到8.18W，这种电池将来有望成为便携式的备用电源的核心部件。
针对SC-SOFC采用碳氢化合物燃料时阳极可能存在的碳沉积问题以及金属Ni在燃料和氧气的混合气氛中的氧化还原现象，研究了CH_4和O_2的混合气体组分对SC-SOFC阳极的影响机制。用气体质谱分析仪研究了Ni/YSZ阳极对甲烷和氧气混合气体的催化性能，发现甲烷和氧气的比例（燃氧比R）为1时发生的反应以甲烷的完全氧化反应为主导，而燃氧比大于1时则以甲烷的部分氧化反应为主。在700°C进行5h短期测试，发现燃氧比为2.5时既没有明显积碳，也没有金属镍被氧化的现象，对于SC-SOFC的Ni/YSZ阳极是比较合理的气体比例。
SC-SOFC has received considerable attention for the portable applications due tothe sealing-free and simple gas management. However, current researches focusprimarily on the single cells. Studies of the SC-SOFC stack are also confined to the lowpower output. This paper provides a detailed study on the SC-SOFC stack essentialparameters, including the gas flow field distribution, gas supply method and gascomponent of SC-SOFC, by using the theoretical and experimental methods. ASC-SOFC stack with dual gas supply method is proposed for the first time.
As the SC-SOFC worked in the fuel and air mixture, gas flow distribution is animportant factor limiting the cell performance. Numerical simulation and experimentalverification are studied with different gas flow distribution. Results showed that thepartial pressure of oxygen at the cathode side of the cell with gas flow direction facingthe anode was very low, which was caused by the catalytic reaction at the anode. Theperformance of the cells with gas flow direction facing the cathode and parallel to theelectrodes were nearly the same. Numerical simulation of the SC-SOFC stack wasstudied due to the gas competition between the anode and cathode. The cell distance ofan anode-facing-cathode two cell stack influences the performances of the cells.Numerical simulation showed that the partial pressure of oxygen and surface temperatureof the cathode facing the narrow gas path is influenced obviously with smaller spacing.While the oxygen partial pressure of the cathode on the outside is influenced with largerspacing. Numerical simulation of the two cell stack with anode-facing-anodeconfiguration was also studied. Results showed that the heat released by the exothermicreaction of the anodes is concentrated between the cells, which is propitious to achievethe thermally self-sustained of SC-SOFC stack.
Numerical simulation showed that the performances of the cells of SC-SOFC microstack with traditional gas supply method are seriously limited by the uneven flowgeometry, where the downstream portion of the stack is exposed to by-products resultingfrom fuel oxidation in the upstream portion of the stack. In view of this problem, a novelgas supply method with multi-point gas vents in the gas tube is proposed in this paper.The traditional gas supply method was also investigated for comparison. Experimentalresults showed that the single cells could obtain a uniform open-circuit voltage andpower output by using the separated gas supply method. For the traditional gas supplymethod, the cell at the outlet position yielded inferior performance compared to that ofthe inlet cell. Finally, the stack operated with the multi-point gas supply methodproduced a higher power output than that operated with the traditional gas supplymethod.
In view of the gas competition between the anode and cathode, dual gas supplymethod for anode and cathode by using multi-point gas transmission tubes is proposed.The performance of the cell with dual gas supply method was increased by67%than thatof the conventional SC-SOFC. As a result, several SC-SOFC micro-stacks with two gastubes were studied. The cells with an anode-facing-cathode configuration were connectedin serial by zigzag sliver sheets. The maximum power output are192,230and276mWat CH_4flow rate of50,70and100sccm, respectively. The performance of SC-SOFCmicro-stacks with congener-electrode-facing configuration was better than that of theanode-facing-cathode configuration stack. A two-cell SC-SOFC stack with cellsembedded in plane configuration demonstrated a maximum power output of1.04W atthe flow rate of260sccm CH_4and130sccm O_2. Finally, a scaled-up stack with six cellsin series generated an OCV of6.4V and a maximum power output of8.18W.
Consider of carbon deposition and oxidation of Ni metal at the Ni/YSZ anode inCH_4/O_2gas mixture, influencing mechanism of CH_4/O_2gas component over Ni/YSZanode was studied by using gas mass spectrometer. Results showed that completeoxidation of CH_4was the main reaction with the CH_4/O_2ratio of1. Partial oxidationreaction of CH_4was the main reaction with higher CH_4/O_2ratio. Neither carbondeposition occurs nor nickel protoxide be observed at CH_4/O_2ratio of2.5at700°C,which is a reasonable proportion of CH_4and O_2for the Ni/YSZ anode of SC-SOFC.
引文
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