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Exsolution of surface and bulk nanoparticles in perovskites has been recently employed in chemical looping methane partial oxidation because of the emergent materials' properties such as oxygen capacity, redox stability, durability, coke resistance and enhanced activity. Here we attempt to further lower the temperature of methane conversion by complementing exsolution with infiltration. We prepare an endo/exo-particle system using exsolution and infiltrate it with minimal amount of Rh (0.1 wt%) in order to functionalize the surface and induce low temperature activity. We achieve a temperature decrease by almost 220 °C and an increase of the activity up to 40%. We also show that the initial microstructure of the perovskite plays a key role in controlling nanoparticle anchorage and carbon deposition. Our results demonstrate that microstructure tuning and surface functionalization are important aspects to consider when designing materials for redox cycling applications. [ABSTRACT FROM AUTHOR]