Comprehensive structural performance study of multi-core–shell catalysts through an experimental/numerical approach: Cyclohexane dehydrogenation case study

Core–shell structures offer the unique ability to integrate multiple functionalities within a single nanoparticle (NP), presenting significant potential for the development of advanced catalytic processes. Optimizing such systems requires a fundamental understanding of the structure–performance relations, particularly the impact of spatial configuration on catalytic behavior. In this study, we systematically evaluate a “dragon fruit” catalyst morphology, in which Pt NPs are uniformly distributed throughout a mesoporous silica shell. This architecture is introduced as an efficient alternative to the “peach” structure, where Pt NPs are concentrated in the center of a core–shell NP. Both morphologies were synthesized via a rational and straightforward two-step approach under identical shell chemistry. The dragon fruit accommodates a significantly higher Pt loading compared to the peach morphology, with comparable particle sizes, surface areas, and surface chemistry. Cyclohexane dehydrogenation was used as a model reaction to evaluate catalytic performance. The dragon fruit structure achieved the highest specific benzene yield per mg of catalyst, while both morphologies exhibited comparable activity per mg of Pt. A qualitative simulation model based on experimental characterization corroborated these results. Comprehensive mass transfer analysis verified the absence of internal and external diffusion limitations under the studied conditions. This assessment further supports that the variation in catalytic performance can be attributed primarily to the ability of the dragon fruit morphology to contain a higher amount of Pt in spatial distribution. These findings underscore the influence of active site configuration and suggest the dragon fruit morphology as a promising and scalable design for next-generation core–shell catalysts. • Systematic investigation of catalyst distribution inside Multi-Core-Shell structures. • Dragon fruit morphology is a promising and scalable design. • Theoretical validation of experimental results with a modeling approach. • Thorough characterization of pre-synthesized-Pt nanoparticles morphologies.