Precise synthesis of small, essentially molecular metal complexes and metal clusters on oxide, zeolite, and MOF support surfaces is bringing new insights to catalysis, linking solution and surface catalysis, and pointing the way to systematic catalyst design. We summarize recent work unraveling effects of key design variables of site-isolated catalysts: the metal, metal nuclearity, support, and other ligands on the metals. The catalysts were synthesized to be structurally simple and nearly uniform to facilitate the physical characterization. The catalytic species are synthesized by reactions of organometallic precursors with support surfaces; the precursors include M(L)2(acetylacetonate)1-2, with M = Ru, Rh, Ir, or Au and the ligands L = C2H4, CO, or CH3. Supported metal clusters are formed from precursors that incorporate metal–metal bonds (e.g., Os3(CO)12 and Ir4(CO)12). The characterization methods include IR, X-ray absorption, and NMR spectroscopies, density functional theory, and atomic-resolution electron microscopy for imaging of individual metal atoms. The data provide examples resolving the roles of the catalyst design variables and place the catalysis science on a firm foundation of organometallic chemistry linked with surface science.

Molecular metal catalysis on supports:  Synthesis, characterization, and progress toward design

251st National Meeting (2016)

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