Recently, the development and characterization of a wide variety of metal-organic frameworks (MOFs) with large surface areas and versatile metal sites has opened the floodgates to broad and diverse new areas of potentially novel catalytic activity. MOF NU-1000 is of particular interest because of its high thermal and pH stability relative to many other MOFs currently under investigation. Atomic layer deposition (ALD) of Ni(II) onto the zirconium nodes of NU-1000 results in a catalyst which has shown extraordinary efficacy and high turnover number for ethylene hydrogenation.<br/><br/>In this presentation, we will discuss the DFT (M06-L) computed energetics for the ALD process, characterization of the Ni sites, activation of the catalyst with H<sub>2</sub>, and the proposed mechanistic cycle for ethylene hydrogenation. Our results align well with experimental studies on this catalytic system, and provide valuable insight into the topology of the catalyst structure and the nature of its reactivity. This work was done in order to inform the development of new single-site heterogeneous catalysts for organic reactions of industrial interest.

Quantum chemical insight into a single-site nickel hydrogenation catalyst produced via atomic layer deposition on a metal-organic framework

251st National Meeting (2016)

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