Accelerated Perovskite Oxide Development for Thermochemical Energy Storage by a High‐Throughput Combinatorial Approach
Accelerated Perovskite Oxide Development for Thermochemical Energy Storage by a High‐Throughput Combinatorial Approach
复制标题
DOI：
10.1002/aenm.202203833
复制
发表时间：
2023-03
影响因子：
27.8
通讯作者：
R. Cai;Hilal Bektaş;Xijun Wang;Kyle McClintock;Lauren Teague;Kunran Yang;Fanxing Li
中科院分区：
文献类型：
--
作者：
R. Cai;Hilal Bektaş;Xijun Wang;Kyle McClintock;Lauren Teague;Kunran Yang;Fanxing Li
钙钛矿氧化物的结构和组成灵活性及其复杂而可调的氧化还原特性为热化学储能（TCES）提供了独特的优化机会。为了改进相对低效和基于经验的方法，本文报道了一种高通量组合方法，用于加速TCES钙钛矿氧化物的开发和优化。具体来说，基于热力学的筛选标准应用于2000多个A/B位点掺杂SrFeO3−δ的高通量密度泛函数理论（DFT）模拟结果。基于DFT预测，选择了61个有潜力的TCES候选者。其中，45种纯钙钛矿相材料进行了全面评估。实验结果支持高通量方法在测定钙钛矿氧化物的氧容量和氧化焓方面的有效性。许多筛选的材料在实际操作条件下表现出良好的性能：sr0.75 ba0.125 feo3−δ在400至800°C的等压条件下（与空气）表现出85 kJ kgABO3−1的化学能量存储密度，而sr0.125 ca0.75 fe0.25 mn0.75 o3−δ在400°C/0.2 atm O2和1100°C/0.01 atm O2之间表现出157 kJ kgABO3−1的能量存储密度。基于DFT和实验结果的结合，还开发了一套改进的优化标准，以提高加速氧化还原活性钙钛矿氧化物开发的有效性。
The structural and compositional flexibility of perovskite oxides and their complex yet tunable redox properties offer unique optimization opportunities for thermochemical energy storage (TCES). To improve the relatively inefficient and empirical‐based approaches, a high‐throughput combinatorial approach for accelerated development and optimization of perovskite oxides for TCES is reported here. Specifically, thermodynamic‐based screening criteria are applied to the high‐throughput density functional theory (DFT) simulation results of over 2000 A/B‐site doped SrFeO3−δ. 61 promising TCES candidates are selected based on the DFT prediction. Of these, 45 materials with pure perovskite phases are thoroughly evaluated. The experimental results support the effectiveness of the high‐throughput approach in determining both the oxygen capacity and the oxidation enthalpy of the perovskite oxides. Many of the screened materials exhibit promising performance under practical operating conditions: Sr0.875Ba0.125FeO3−δ exhibits a chemical energy storage density of 85 kJ kgABO3−1 under an isobaric condition (with air) between 400 and 800 °C whereas Sr0.125Ca0.875Fe0.25Mn0.75O3−δ demonstrates an energy density of 157 kJ kgABO3−1 between 400 °C/0.2 atm O2 and 1100 °C/0.01 atm O2. An improved set of optimization criteria is also developed, based on a combination of DFT and experimental results, to improve the effectiveness for accelerated development of redox‐active perovskite oxides.