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Observation and reactivity studies of an unusual RhI intermediate in H2 evolution catalysis

Aguirre Quintana, Luis and Gray, Harry and Winkler, Jay and Blakemore, James D. (2016) Observation and reactivity studies of an unusual RhI intermediate in H2 evolution catalysis. In: 251st American Chemical Society National Meeting & Exposition, March 13-17, 2016, San Diego, CA.

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Understanding mechanisms of hydrogen evolution is important for improving catalysts that generate clean fuels. Catalysts often operate via unknown mechanism(s) due to the difficulty of observing or isolating key intermediates in the 2e-/2H+ redn. process. For our study, we prepd. a family of RhI complexes bearing the pentamethylcyclopentadienyl (η5-Cp*) ligand in addn. to derivs. of 4,4'- bipyridyl or 1,10- phenanthroline (bound in the κ2 mode). Under carefully chosen conditions, these compds. formed intermediate species that suggest a previously unknown mechanism of H2 evolution involving protonhydride tautomerism driven by the Cp* ligand. This intermediate complex could be isolated in a MeCN soln., and even as a solid, making it amenable to further mechanistic investigations. The intermediate species were analyzed by mass spectrometry, 1H NMR, and 2H NMR (NMR is NMR spectroscopy). Results will be discussed concerning the properties and reactivity of these active intermediates.

Item Type:Conference or Workshop Item (Paper)
Related URLs:
URLURL TypeDescription Website
Gray, Harry0000-0002-7937-7876
Winkler, Jay0000-0002-4453-9716
Blakemore, James D.0000-0003-4172-7460
Additional Information:© 2016 American Chemical Society.
Record Number:CaltechAUTHORS:20160422-084313796
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:66395
Deposited By: Tony Diaz
Deposited On:22 Apr 2016 16:28
Last Modified:22 Nov 2019 09:58

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