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Structural Characterization of Nickel-Doped Aluminum Oxide Cations by Cryogenic Ion Trap Vibrational Spectroscopy
| Title: | Structural Characterization of Nickel-Doped Aluminum Oxide Cations by Cryogenic Ion Trap Vibrational Spectroscopy |
| Authors: | Li, Ya-Ke Browse this author | | Babin, Mark C. Browse this author | | Debnath, Sreekanta Browse this author | | Iwasa, Takeshi Browse this author | | Kumar, Sonu Browse this author | | Taketsugu, Tetsuya Browse this author | | Asmis, Knut R. Browse this author | | Lyalin, Andrey Browse this author | | Neumark, Daniel M. Browse this author |
| Issue Date: | 4-Nov-2021 |
| Publisher: | American Chemical Society |
| Journal Title: | Journal of physical chemistry A |
| Volume: | 125 |
| Issue: | 43 |
| Start Page: | 9527 |
| End Page: | 9535 |
| Publisher DOI: | 10.1021/acs.jpca.1c07156 |
| Abstract: | Isolated nickel-doped aluminum oxide cations (NiOm) (Al2O3)(n) (AlO)(+) with m = 1 -2 and n = 1-3 are investigated by infrared photodissociation (IRPD) spectroscopy in combination with density functional theory and the single-component artificial force-induced reaction method. IRPD spectra of the corresponding He-tagged cations are reported in the 400-1200 cm(-1) spectral range and assigned based on a comparison to calculated harmonic IR spectra of low-energy isomers. Simulated spectra of the lowest energy structures generally match the experimental spectra, but multiple isomers may contribute to the spectra of the m = 2 series. The identified structures of the oxides (m = 1) correspond to inserting a Ni-O moiety into an Al-O bond of the corresponding (Al2O3)(1-3)(AlO)(+) cluster, yielding either a doubly or triply coordinated Ni2+ center. The m = 2 clusters prefer similar structures in which the additional O atom either is incorporated into a peroxide unit, leaving the oxidation state of the Ni2+ atom unchanged, or forms a biradical comprising a terminal oxygen radical anion Al-O-center dot(-) and a Ni3+ species. These clusters represent model systems for under-coordinated Ni sites in alumina-supported Ni catalysts and should prove helpful in disentangling the mechanism of selective oxidative dehydrogenation of alkanes by Ni-doped catalysts. |
| Rights: | This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of physical chemistry A, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/articlesonrequest/AOR-3WS6QQZYZGHSZVJJVJDV. |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/87236 |
| Appears in Collections: | 化学反応創成研究拠点：ICReDD (Institute for Chemical Reaction Design and Discovery : ICReDD) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)
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Submitter: LYALIN ANDREY
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