Nanoparticle O–H Bond Dissociation Free Energies from Equilibrium Measurements of Cerium Oxide Colloids

Agarwal, Rishi G.; Kim, Hyun-Jo; Mayer, James M.

doi:10.1021/jacs.0c12799

Title: Nanoparticle O–H Bond Dissociation Free Energies from Equilibrium Measurements of Cerium Oxide Colloids

Journal Article · Wed Feb 10 00:00:00 EST 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c12799· OSTI ID:1785120

^[1]; Kim, Hyun-Jo ^[1];

^[1]

Yale Univ., New Haven, CT (United States)

A novel equilibrium strategy for measuring the hydrogen atom affinity of colloidal metal oxide nanoparticles is presented. Reactions between oleate-capped cerium oxide nanoparticle colloids (nanoceria) and organic proton-coupled electron transfer (PCET) reagents are used as a model system. Nanoceria redox changes, or hydrogen loadings, and overall reaction stoichiometries were followed by both ¹H NMR and X-ray absorption near-edge spectroscopies. Furthermore, these investigations revealed that, in many cases, reactions between nanoceria and PCET reagents reach equilibrium states with good mass balance. Each equilibrium state is a direct measure of the bond strength, or bond dissociation free energy (BDFE), between nanoceria and hydrogen. Further studies, including those with larger nanoceria, indicated that the relevant bond is a surface O–H. Thus, we have measured surface O–H BDFEs for nanoceria—the first experimental BDFEs for any nanoscale metal oxide. Remarkably, the measured CeO–H BDFEs span 13 kcal mol^–1 (0.56 eV) with changes in the average redox state of the nanoceria colloid. Possible chemical models for this strong dependence are discussed. We propose that the tunability of ceria BDFEs may be important in explaining its effectiveness in catalysis. More generally, metal oxide BDFEs have been used as predictors of catalyst efficacy that, traditionally, have only been accessible by computational methods. These results provide important experimental benchmarks for metal oxide BDFEs and demonstrate that the concepts of molecular bond strength thermochemistry can be applied to nanoscale materials.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division (SUF); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; CHE-1609434; CHE-1904813

OSTI ID:: 1785120

Journal Information:: Journal of the American Chemical Society, Vol. 143, Issue 7; Related Information: The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.0c12799.; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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