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Performance of a Direct Methane Solid Oxide Fuel Cell Using Nickel-Ceria-Yttria Stabilized Zirconia as the Anode

机译:镍-氧化铈-氧化钇稳定的氧化锆作为阳极的直接甲烷固体氧化物燃料电池的性能

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摘要

A nickel-ceria-yttria stabilized zirconia (Ni-CYSZ) cermet material was synthesized and tested as the anode for the direct oxidation of methane in a solid oxide fuel cell (SOFC) with YSZ as the electrolyte and strontium-doped lanthanum manganite (LSM) as the cathode. Initially, the electrochemical behavior was investigated under several load demands in wet (3% H O) CH at 850 °C during 144 h using I-V curves, impedance spectra, and potentiostatic measurements. Long-term tests were subsequently conducted under 180 mA·cm in wet CH for 236 h and dry CH for 526 h at 850 °C in order to assess the cell stability. Material analysis was carried out by SEM-EDS after operation was complete. Similar cell performance was observed with wet (3% H O) and dry CH , and this indicates that the presence of water is not relevant under the applied load demand. Impedance spectra of the cell showed that at least three processes govern the direct electrochemical oxidation of methane on the Ni-CYSZ anode and these are related to charge transfer at high frequency, the adsorption/desorption of charged species at medium frequency and the non-charge transfer processes at low frequency. The cell was operated for more than 900 h in CH and 806 h under load demand, with a low degradation rate of ~0.2 mV·h observed during this period. The low degradation in performance was mainly caused by the increase in charge transfer resistance, which can be attributed to carbon deposition on the anode causing a reduction in the number of active centers. Carbon deposits were detected mostly on the surface of Ni particles but not near the anode/electrolyte interface or the cerium surface. Therefore, the incorporation of cerium in the anode structure could improve the cell lifetime by reducing carbon formation.
机译:合成了镍-二氧化铈-氧化钇稳定的氧化锆(Ni-CYSZ)金属陶瓷材料,并作为阳极将固体氧化物燃料电池(SOFC)中的甲烷直接氧化,并以YSZ作为电解质和掺锶锶的锰酸镧(LSM) )作为阴极。最初,使用I-V曲线,阻抗谱和恒电位测量,在144 h下在850°C的湿(3%H O)CH中的几种负载需求下,研究了电化学行为。随后在850°C的湿式CH中在180 mA·cm的条件下进行了236 h的长期测试,在850°C的干CH中进行了526 h的长期测试,以评估电池的稳定性。操作完成后,通过SEM-EDS进行材料分析。在湿(3%H O)和干CH上观察到相似的电池性能,这表明在所施加的负载需求下水的存​​在无关紧要。电池的阻抗谱表明,至少有三个过程控制着甲烷在Ni-CYSZ阳极上的直接电化学氧化,这些过程与高频下的电荷转移,中频下带电物质的吸附/解吸以及不带电有关。低频传输过程。该电池在负载条件下在CH中运行900 h以上,在806 h下运行,在此期间观察到〜0.2 mV·h的低降解速率。性能降低的主要原因是电荷转移电阻增加,这可以归因于阳极上的碳沉积,导致活性中心数量减少。大部分在Ni颗粒表面检测到碳沉积,但在阳极/电解质界面或铈表面附近未检测到碳沉积。因此,在阳极结构中掺入铈可以通过减少碳的形成来改善电池寿命。

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