提高电化学性能和长期稳定性的纳米结构LSC薄膜电极

Katherine Develos Bagarinao, Ozden Celikbilek, Gwilherm Kerherve, Sarah Fearn, Stephen J Skinner, Haruo Kishimoto
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摘要

纳米结构的La 0.6 Sr 0.4 CoO 3-δ (LSC)薄膜电极表现出异常高的氧表面交换性能,超越了传统的微尺度电极结构,这是固体氧化物电池(SOC)应用的理想选择[1-2]。另一方面,在SOC工作所需的高温下,LSC纳米结构也会发生显著的形态变化,导致性能迅速下降。本文以提高纳米结构LSC薄膜电化学性能的长期稳定性为目标,系统地研究了加工温度对长期稳定性的影响。通过改变沉积温度(500℃至室温),脉冲激光沉积制备的LSC薄膜的生长特征纳米结构可以从高密度的纳米柱状颗粒调整到具有高孔隙率的纳米纤维结构。沉积温度的变化也导致生长LSC薄膜表面结合/晶格结合的Sr和Co 2+ /Co 3+比例的差异;然而,在空气中700℃的长时间退火基本上使表面转变为主要由晶格结合的Sr和Co 3+组成的最终状态。然而,与致密薄膜相比,具有初始纳米纤维结构的LSC薄膜在高温下不易发生晶粒烧结效应,电极极化电阻的退化程度也较低。在较低的沉积温度下,LSC/GDC界面上发生的阳离子相互扩散也被显著抑制,因此与在较高沉积温度下制备的材料相比,界面稳定性更好。这些结果突出了薄膜电极的特征纳米结构与电化学性能之间的关系,并为设计具有更好长期稳定性的电极提供了指导。[10] J. Januschewsky, M. Ahrens, A. Opitz, F. Kubel, J. Fleig, ad . Funct。板牙。中国农业科学,2009,19,3151-3156。[10]刘建军,刘建军,刘建军,等。能源工程学报,2011,26(1):1 - 7。[10] K. Develos-Bagarinao, O. Celikbilek, R. A. Budiman, G. Kerherve, S. Fearn, S. J. Skinner, H.岸本,J. Mater。化学。[j] .农业工程学报,2016,33(2):445- 459(2022)。
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Nanostructured LSC Thin Film Electrodes with Improved Electrochemical Performance and Long-Term Stability
Nanostructured La 0.6 Sr 0.4 CoO 3-δ (LSC) thin film electrodes exhibit exceptionally high oxygen surface exchange properties, surpassing those of conventional microscale electrode structures, which are desirable for application in solid oxide cells (SOC) [1-2]. On the other hand, the LSC nanostructures also tend to undergo significant morphological changes at typically high temperatures required for SOC operation, leading to rapid degradation in performance. Here, towards the goal of improving the long-term stability of electrochemical performance of nanostructured LSC thin films, a systematic investigation of the effect of processing temperatures on long-term stability was carried out [3]. By varying the deposition temperature (500 °C to room temperature), the as-grown characteristic nanostructures of LSC thin films prepared using pulsed laser deposition can be tuned from highly dense nanocolumnar grains to nanofibrous structures with high porosity. Variations in the deposition temperature also resulted to differences in the proportion of surface-bound/lattice-bound Sr and Co 2+ /Co 3+ at the surfaces of the as-grown LSC thin films; however, prolonged annealing at 700 °C in air essentially transforms the surfaces to a final state with mostly lattice-bound Sr and Co 3+ . Nevertheless, LSC films with initially nanofibrous structures are found to be less prone to the grain sintering effect occurring at high temperatures and exhibit less degradation of the electrode polarization resistance as compared to well-dense films. Using lower deposition temperatures, cation interdiffusion occurring at LSC/GDC interfaces is also significantly suppressed, thus leading to better interfacial stability as compared to those prepared at higher deposition temperatures. These results highlight the relationship between characteristic nanostructures of thin film electrodes and electrochemical performance and provide guidance on designing electrodes with improved long-term stability. [1] J. Januschewsky, M. Ahrens, A. Opitz, F. Kubel and J. Fleig, Adv. Funct. Mater., 2009, 19, 3151–3156. [2] J. Hayd, L. Dieterle, U. Guntow, D. Gerthsen and E. Ivers-Tiffee, J. Power Sources, 2011, 196, 7263–7270. [3] K. Develos-Bagarinao, O. Celikbilek, R. A. Budiman, G. Kerherve, S. Fearn, S. J. Skinner and H. Kishimoto, J. Mater. Chem. A, 10, 2445-2459 (2022).
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