Abstract
Exsolution has been recently demonstrated as one of the most effective strategies for designing highly stable and active catalysts, offering precise control over nanoparticle size, composition, structure, and morphology. This approach has gained significant attention for CO2 utilisation, particularly in the reverse water-gas shift (rWGS) reaction. However, the efficiency of exsolved catalysts is governed by multiple factors that influence nanoparticle formation, distribution, and stability. To gain a comprehensive understanding of how these various parameters interplay in exsolved catalysts, this study systematically investigates the impact of dopant levels, composition, reduction temperature, and material microstructure on the exsolution of iron and cobalt nanoparticles from perovskite materials and assesses their catalytic performance in the rWGS reaction. Our findings highlight the critical role of microstructure refinement, dopant chemistry, and pre-treatment conditions in optimising exsolution behaviour and catalytic performance. This work offers valuable insights toward establishing a standardised framework for the rational design of efficient and stable next-generation exsolved catalysts for CO2 utilisation but is also expected to impact many other applications.