Evaluating the Origins of Aerobic Oxidation Catalysis with TAM-3, a MOF with Accessible Co(II) Sites and Large Pores

Sur, Aishanee; Sarkar, Subham; Jernigan, Nicholas B.; Bhuvanesh, Nattamai; Powers, David C.

doi:10.1021/acscatal.5c01083

Evaluating the Origins of Aerobic Oxidation Catalysis with TAM-3, a MOF with Accessible Co(II) Sites and Large Pores

Journal Article · Mon Jun 02 00:00:00 EDT 2025 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5c01083· OSTI ID:2570519

^[1]; Sarkar, Subham ^[1]; Jernigan, Nicholas B. ^[1]; Bhuvanesh, Nattamai ^[1]; ^[1]

Texas A & M Univ., College Station, TX (United States)

Metal-organic frameworks (MOFs) are attractive platforms that merge concepts of homogeneous and heterogeneous catalysis. Catalyst design and optimization are enabled by an array of synthetic methods that offer independent control over the local chemical structure of lattice-embedded metal ions (i.e., ligand identity and geometry) and the long-range materials properties (i.e., porosity). Establishing the origin of catalytic activity in MOF-promoted reactions remains a significant challenge: The relative rates of catalyst turnover and substrate diffusion dictate the extent to which interstitial sites are accessible and operational in catalysis. To minimize the contributions of surface sites in catalysis, materials with large pore dimensions are often sought, however, the impact of pore expansion on the origins of catalytic activity is similarly challenging to establish. Here, we describe TAM-3, a Co(II) based MOF with accessible metal sites supported by a facially coordinating tris-tetrazole ligand set. TAM-3 features large channel-like pores (17 × 23 Å) and promotes aerobic C−H oxidation and olefin epoxidation. Using a set of simple kinetics experiments, based on the analysis of kinetic isotope effects and olefin oxidation diastereoselectivities, we demonstrate that despite the large pores, interstitial metal ions do not significantly contribute to the observed substrate oxidation. This study highlights the importance of conducting kinetic experiments to assess the origin of apparent catalytic activity with MOFs and the challenge of harnessing reactive oxidants with microporous catalyst materials.

View Accepted Manuscript (DOE)

Research Organization:: Texas A & M Univ., College Station, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0024121

OSTI ID:: 2570519

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 12 Vol. 15; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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