Accelerated Perovskite Oxide Development for Thermochemical Energy Storage by a High-Throughput Combinatorial Approach

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-delta. 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-delta exhibits a chemical energy storage density of 85 kJ kg(ABO3)(-1) under an isobaric condition (with air) between 400 and 800 degrees C whereas Sr0.125Ca0.875Fe0.25Mn0.75O3-delta demonstrates an energy density of 157 kJ kg(ABO3)(-1) between 400 degrees C/0.2 atm O-2 and 1100 degrees C/0.01 atm O-2. 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.