The ability to synthesize transition metal-based active sites with atomic precision is well-established in homogeneous catalysis, but techniques from this field are rarely applied rigorously in heterogeneous catalysis due to difficulties in controlling surface reactions and characterizing species. Nevertheless, recent advances in both fields are converging to make possible the construction of solid catalysts with a high degree of local order, that are therefore amenable to rigorous kinetic study and computational analysis. For example, directed reactions of volatile molecular metal complexes such as GaR<sub>3</sub> and ZnR<sub>2</sub> with either the dilute Bronsted acid sites or the silanol defects of HZSM-5 give rise to very different, specific ligand substitution patterns and reactivities in the highly dispersed metal sites. Atomically-precise Cu nanoclusters constructed using techniques from molecular synthesis and characterization are also amenable to rigorous kinetic and mechanistic analysis of their ligand substitution and metal redistribution reactions. Such systems have the potential to provide precise, reproducible data that can be used to develop new catalyst design principles.

Well-defined transition metal-based heterogeneous catalysts: From isolated sites to atomically-precise clusters

253rd National Meeting (2017)

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