We will present fundamental understanding of the chemistry of transition-metal single atoms supported by metal oxides and metal-organic frameworks (MOF) provided by density functional theory calculations. First, the mechanism of CO oxidation on Pt atoms at two sites of the anatase TiO<sub>2</sub>(101) surface will be revealed, including a comparison of Mars van Krevelen and Langmuir-Hinshelwood pathways. Second, the hydrolysis of nerve agents on a recently synthesized MOF featuring single-atom chemistry will be discussed. The MOF is based on the widely popular and robust UiO-66 Zr(IV) MOF, modified with the addition of Cu single atoms at the defect sites in the secondary building units. The catalytic promise of the Cu(I) and Cu(II) variants of the MOF to hydrolyze nerve agents will be contrasted with the well-established performance of the unmodified UiO-66 MOF. Comparison with extant experiments will be used throughout to validate the computational models.

Computational studies of single-atom oxidative and hydrolytic chemistry on metal oxides and metal-organic frameworks

ACS Spring Meeting 2021

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