(327e) Electronic Effects on Open Framework Material-Encapsulated Metal Nanoparticles (NP@OFM) and Implications on Catalysis
Toward this goal it is necessary to understand what the most crucial effects that need to be considered at the design (or computational screening) stage are. Previous studies have decoupled steric effects in NP@MOFs systems from other factors [2-4] and provided insights on how these effects can affect reactivity. However, partly due to insufficient understanding of the structure of the NP/OFM interface, the role of electronic effects originating from the interaction of OFM components and the metal at the NP/OFM interface have yet to be studied. Leveraging recent insights on the interface structure , here we discuss ongoing work in our lab to elucidate the relative importance of electronic effects originating from the mentioned interactions compared to electronic effects originating from changes in NP composition. We study this with the assistance of periodic DFT calculations to elucidate how charge is transferred between the OFM and the NP depending on the kind of bonds occurring at the interface, the chemical functionality of the OFM, and the composition of the metal. Thus, the effect of interactions at the interface and NP composition on the catalyst electronic density of state (DOS) and on the binding of small, common catalytic species (e.g. C*, H3C*, O*, HO*, N*, H*) to the NP surface has been evaluated, also considering implications on catalytic rates (e.g. via available scaling relationships).
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