Oxygen Atom Transfer Reactions of Colloidal Metal Oxide Nanoparticles

Lee, Justin L.; Gentry, Noreen Elizabeth; Peper, Jennifer L.; Hetzel, Staci; Quist, Christine; Menges, Fabian S.; Mayer, James M.

doi:10.1021/acsnano.4c17955

Title: Oxygen Atom Transfer Reactions of Colloidal Metal Oxide Nanoparticles

Journal Article · Tue Mar 04 00:00:00 UTC 2025 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.4c17955 · OSTI ID:2570631

^[1]; Gentry, Noreen Elizabeth ^[1]; Peper, Jennifer L. ^[1]; Hetzel, Staci ^[1]; Quist, Christine ^[1];

^[1];

^[1]

Yale University, New Haven, CT (United States)

Redox transformations at metal oxide (MO_x)/solution interfaces are broadly important, and oxygen atom transfer (OAT) is one of the simplest and most fundamental examples of such reactivity. OAT is a two-electron transfer process, well-known in gas/solid reactions and catalysis. However, OAT is rarely directly observed at oxide/water interfaces, whose redox reactions are typically proposed to occur in one-electron steps. Reported here are stoichiometric OAT reactions of organic molecules with aqueous colloidal titanium dioxide and iridium oxide nanoparticles (TiO₂ and IrO_x NPs). Me₂SO (DMSO) oxidizes reduced TiO₂ NPs with the formation of Me₂S, and IrO_x NPs transfer O atoms to a water-soluble phosphine and a thioether. The reaction stoichiometries were established and the chemical mechanisms were probed using typical solution spectroscopic techniques, exploiting the high surface areas and transparency of the colloids. Furthermore, these OAT reactions, including a catalytic example, utilize the ability of the individual NPs to accumulate many electrons and/or holes. Observing OAT reactions of two different materials, in opposite directions, is a step toward harnessing oxide nanoparticles for valuable multi-electron and multi-hole transformations.

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Research Organization:: Yale University, New Haven, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); United States-Israel Binational Science Foundation

Grant/Contract Number:: SC0001059; SC0021298

OSTI ID:: 2570631

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 10 Vol. 19; ISSN ANCAC3; ISSN 1936-086X; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Oxygen Atom Transfer Reactions of Colloidal Metal Oxide Nanoparticles

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