Ruthenium hydrides encapsulated in sol-gel glasses exhibit new ultrafast vibrational dynamics

Cynthia G. Pyles, Joel Patrow, Yukun Cheng, Ian A. Tonks, Aaron M. Massari

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Vibrational dynamics were measured by IR pump-probe spectroscopy and two-dimensional IR spectroscopy for triruthenium dodecacarbonyl and the undecacarbonyl hydride that forms when it is encapsulated in an alumina sol-gel glass. For comparison, a triruthenium undecacarbonyl hydride salt was also synthesized and studied in neat solution to identify the potential influence of the confined solvent environment on the dynamics experienced by carbon monoxide ligands. The vibrational lifetime was found to be significantly decreased for both hydride species relative to the dodecacarbonyl compound. Conversely, spectral diffusion of the CO vibrations was measured to be faster for the parent compound. The most significant dynamic changes occurred upon transformation from the starting compound to the hydride, while only minor differences were observed between the dynamics of the freely dissolved and sol-gel encapsulated hydrides. The results suggest that the structural change to the hydride has the largest impact on the dynamics and that its improved catalytic properties likely do not originate from confined solvent effects.

Original languageEnglish (US)
Article number124502
JournalJournal of Chemical Physics
Issue number12
StatePublished - Mar 28 2022

Bibliographical note

Funding Information:
The authors gratefully acknowledge partial support from the National Science Foundation under Grant No. CHE-1856589. C.G.P. was supported, in part, by a Newman and Lillian Bortnick Fellowship. J.G.P. was supported, in part, by a Mistletoe Research Fellowship.

Publisher Copyright:
© 2022 Author(s).


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