Design of CO2-Resistant High-Entropy Perovskites Based on Ba0.5Sr0.5Co0.8Fe0.2O3-δ Materials

High-entropy perovskite materials (HEPMs), characterized by their multi-element composition and highly disordered structure, can incorporate multiple rare earth elements at the A-site, producing perovskites with enhanced CO2 resistance, making them stay high performance and structurally stable in the CO2 atmosphere. However, this modification may result in reduced oxygen permeability. In this study, we investigated La0.2Pr0.2Nd0.2Ba0.2Sr0.2Co0.8Fe0.2O3-δ (L0.2M1.8) high-entropy perovskite materials, focusing on enhancing their oxygen permeability in both air and CO2 atmospheres through strategic design modifications at the B-sites and A/B-sites. We prepared Ni-substituted La0.2Pr0.2Nd0.2Ba0.2Sr0.2Co0.7Fe0.2Ni0.1O3-δ (L0.2M1.7N0.1) HEPMs by introducing Ni elements at the B-site, and further innovatively introduced A-site defects to prepare La0.2Pr0.2Nd0.2Ba0.2Sr0.2Co0.7Fe0.2Ni0.1O3-δ (L0.1M1.7N0.1) materials. In a pure CO2 atmosphere, the oxygen permeation flux of the L0.1M1.7N0.1 membrane can reach 0.29 mL·cm−2·min−1. Notably, the L0.1M1.7N0.1 membrane maintained a good perovskite structure after stability tests extending up to 120 h under 20% CO2/80% He atmosphere. These findings suggest that A-site-defect high-entropy perovskites hold great promise for applications in CO2 capture, storage, and utilization.