Over the last decade, exsolution has emerged as a powerful new method for decorating oxide supports with uniformly dispersed nanoparticles for energy and catalytic applications. Due to their exceptional anchorage, resilience to various degradation mechanisms, as well as numerous ways in which they can be produced, transformed and applied, exsolved nanoparticles have set new standards for nanoparticles in terms of activity, durability and functionality. In conjunction with multifunctional supports such as perovskite oxides, exsolution becomes a powerful platform for the design of advanced energy materials. In the following sections, we review the current status of the exsolution approach, seeking to facilitate transfer of ideas between different fields of application. We also explore future directions of research, particularly noting the multi-scale development required to take the concept forward, from fundamentals through operando studies to pilot scale demonstrations.
Perovskite-type oxides are highly flexible materials that show properties that are beneficial for application in reverse water-gas shift processes (rWGS). Due to their stable nature, the ability to incorporate catalytically active dopants in their lattice structure, and the corresponding feature of nanoparticle exsolution, they are promising candidates for a materials design approach. On an industrial level, the rWGS has proven to be an excellent choice for the efficient utilisation of CO2 as an abundant and renewable carbon source, reflected by the current research on novel and improved catalyst materials. In the current study, a correlation between rWGS reaction environments (CO2 to H2 ratios and temperature), surface morphology, and catalytic activity of three perovskite catalysts (Nd0.6Ca0.4Fe0.9Co0.1O3-δ, Nd0.6Ca0.4Fe0.97Co0.03O3-δ, and Nd0.6Ca0.4Fe0.97Ni0.03O3-δ) is investigated, combining catalytic measurements with SEM and NAP-XPS. The materials were found to react dynamically to the conditions showing both activation due to in situ nanoparticle exsolution and deactivation via CaCO3 formation. This phenomenon could be influenced by choice of material and conditions: less reductive conditions (larger CO2 to H2 or lower temperature) lead to smaller exsolved particles and reduced carbonate formation. However, the B-site doping was also important; only with 10% Co-doping, a predominant activation could be achieved.
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