ORCID Profile
0000-0002-9075-3035
Current Organisation
Instituto de Ciencia de Materiales de Madrid
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Publisher: American Chemical Society (ACS)
Date: 05-09-2017
DOI: 10.1021/JACS.7B06828
Abstract: A molecular water oxidation catalyst based on the copper complex of general formula [(L
Publisher: American Chemical Society (ACS)
Date: 09-08-2016
DOI: 10.1021/JACS.6B05680
Abstract: X-ray transient absorption spectroscopy (X-TAS) has been used to study the light-induced hydrogen evolution reaction catalyzed by a tetradentate macrocyclic cobalt complex with the formula [LCo(III)Cl2](+) (L = macrocyclic ligand), [Ru(bpy)3](2+) photosensitizer, and an equimolar mixture of sodium ascorbate/ascorbic acid electron donor in pure water. X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analysis of a binary mixture of the octahedral Co(III) precatalyst and [Ru(bpy)3](2+) after illumination revealed in situ formation of a Co(II) intermediate with significantly distorted geometry and electron-transfer kinetics of 51 ns. On the other hand, X-TAS experiments of the complete photocatalytic system in the presence of the electron donor showed the formation of a square planar Co(I) intermediate species within a few nanoseconds, followed by its decay in the microsecond time scale. The Co(I) structural assignment is supported by calculations based on density functional theory (DFT). At longer reaction times, we observe the formation of the initial Co(III) species concomitant to the decay of Co(I), thus closing the catalytic cycle. The experimental X-ray absorption spectra of the molecular species formed along the catalytic cycle are modeled using a combination of molecular orbital DFT calculations (DFT-MO) and finite difference method (FDM). These findings allowed us to assign the full mechanistic pathway, followed by the catalyst as well as to determine the rate-limiting step of the process, which consists in the protonation of the Co(I) species. This study provides a complete kinetics scheme for the hydrogen evolution reaction by a cobalt catalyst, revealing unique information for the development of better catalysts for the reductive side of hydrogen fuel cells.
Publisher: Wiley
Date: 06-04-2020
Publisher: Springer Science and Business Media LLC
Date: 28-09-2020
Publisher: Wiley
Date: 14-04-2018
Abstract: We report the light-induced electronic and geometric changes taking place within a heteroleptic Cu
Location: Germany
No related grants have been discovered for Dooshaye Moonshiram.