An outstanding challenge in the field of heterogeneous catalysis is the synthesis of catalysts (typically clusters of metal atoms or ions in combination with oxy ligands) with single-atom control over the catalyst/cluster composition and structure. A related challenge is to maintain the catalyst structure over the course of catalytic reactions. Satisfying these conditions can facilitate the discovery of meaningful structure/reactivity relationships and aid the hypothesis-driven, computationally guided development of new catalysts. Clusters can be highly catalytic on a per-atom basis because essentially all atoms are reactant accessible. The catalytic activity and chemical selectivity of clusters in the few-to-several atom size range can be highly sensitive to the exact cluster size and configuration – thus the need to pursue single-atom precision. Arrays of catalytic clusters of uniform size and composition can be obtained by subjecting chemically and thermally robust, high-surface area, metal-organic frameworks (MOFs) to “AIM” or ALD In MOFs. ALD is atomic layer deposition. AIM and a related solution-based technique termed “SIM” have proven effective for the synthesis of scores of new cluster-based catalysts. This presentation will focus on an example or two, drawn primarily from reations entailing selective oxdidation, oxygenation, or reduction of small hydrocarbons, and will illustrate synthesis, atomically precise structural characterization, characterization, operando assessment of catalyst/molecule(reactant) interactions, and mechanism of catalysis.

AIM-ing for catalyst synthesis with single-atom precision

256th National Meeting (2018)

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