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Reactivation of chromia poisoned oxygen exchange kinetics in mixed conducting solid oxide fuel cell electrodes by serial infiltration of lithia
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-08-11 , DOI: 10.1039/d1ee03975j Han Gil Seo , Anna Friederike Staerz , Dennis S Kim , Dino Klotz , Clement Nicollet , Michael Xu , James M LeBeau , Harry L. Tuller
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-08-11 , DOI: 10.1039/d1ee03975j Han Gil Seo , Anna Friederike Staerz , Dennis S Kim , Dino Klotz , Clement Nicollet , Michael Xu , James M LeBeau , Harry L. Tuller
Solid oxide fuel cells have the potential to render the conversion from fuel to electrical energy more efficienct while lowering emissions. The technology, however, suffers from performance degradation due to cathode poisoning by chromia from metal interconnects. We confirm the deleterious impact of chromia on the performance of the model mixed conducting cathode material Pr0.1Ce0.9O2−δ by examining the oxygen exchange coefficient (kchem) via electrical conductivity relaxation measurements, and the area-specific resistance (ASR) by electrochemical impedance spectroscopy. Liquid Cr-infiltration decreases kchem 20-fold and the oxygen exchange component of ASR increases 20-fold while maintaining the same activation energy. We then demonstrate the ability to not only recover initial kchem and ASR values, but improve properties above those exhibited by the pristine specimen through subsequent Li-infiltration, leading to enhancement of kchem by more than three orders of magnitude and reduction in oxygen exchange component of the ASR by over a factor 100. We attribute these dramatic changes to the depletion of electrons induced by the acidic Cr-infiltrant on the Pr0.1Ce0.9O2−δ surface and the recovery to accumulation of electrons from the basic Li-infiltrant. These results point to acidity as a key descriptor in addressing the long-standing challenge of reactive surface poisoning in applications reliant on rapid oxygen exchange and recovery behavior. The ability to achieve remarkable levels of recovery of electrocatalytic surfaces by controlling the relative acidity of surface species is demonstrated for the first time.
中文翻译:
通过锂离子的连续渗透重新激活混合导电固体氧化物燃料电池电极中氧化铬中毒的氧交换动力学
固体氧化物燃料电池有可能使从燃料到电能的转换更有效,同时降低排放。然而,由于金属互连的氧化铬会导致阴极中毒,该技术会遭受性能下降的困扰。我们通过电导弛豫测量检查氧交换系数 ( k chem )和面积比电阻 (ASR),确认氧化铬对模型混合导电正极材料 Pr 0.1 Ce 0.9 O 2− δ性能的有害影响通过电化学阻抗谱。液体 Cr 渗透降低k chem20 倍,ASR 的氧交换成分增加 20 倍,同时保持相同的活化能。然后,我们展示了不仅恢复初始k chem和 ASR 值的能力,而且通过随后的 Li 渗透改善了原始样品所表现出的性能,导致k chem提高了三个数量级以上并减少了氧交换ASR 的分量超过 100 倍。我们将这些显着变化归因于酸性 Cr 渗透剂在 Pr 0.1 Ce 0.9 O 2- δ上引起的电子耗尽表面和从碱性锂浸渗剂中恢复到电子的积累。这些结果表明,在依赖于快速氧交换和恢复行为的应用中,酸度是解决反应性表面中毒长期挑战的关键描述符。首次证明了通过控制表面物质的相对酸度来实现显着水平的电催化表面回收的能力。
更新日期:2022-08-11
中文翻译:
通过锂离子的连续渗透重新激活混合导电固体氧化物燃料电池电极中氧化铬中毒的氧交换动力学
固体氧化物燃料电池有可能使从燃料到电能的转换更有效,同时降低排放。然而,由于金属互连的氧化铬会导致阴极中毒,该技术会遭受性能下降的困扰。我们通过电导弛豫测量检查氧交换系数 ( k chem )和面积比电阻 (ASR),确认氧化铬对模型混合导电正极材料 Pr 0.1 Ce 0.9 O 2− δ性能的有害影响通过电化学阻抗谱。液体 Cr 渗透降低k chem20 倍,ASR 的氧交换成分增加 20 倍,同时保持相同的活化能。然后,我们展示了不仅恢复初始k chem和 ASR 值的能力,而且通过随后的 Li 渗透改善了原始样品所表现出的性能,导致k chem提高了三个数量级以上并减少了氧交换ASR 的分量超过 100 倍。我们将这些显着变化归因于酸性 Cr 渗透剂在 Pr 0.1 Ce 0.9 O 2- δ上引起的电子耗尽表面和从碱性锂浸渗剂中恢复到电子的积累。这些结果表明,在依赖于快速氧交换和恢复行为的应用中,酸度是解决反应性表面中毒长期挑战的关键描述符。首次证明了通过控制表面物质的相对酸度来实现显着水平的电催化表面回收的能力。