Document type
Journal articles
Document subtype
Full paper
Title
Unveiling a Photoinduced Hydrogen Evolution Reaction Mechanism via the Concerted Formation of Uranyl Peroxide
Participants in the publication
Enric Petrus (Author)
Mireia Segado (Author)
Nuno A. G. Bandeira (Author)
Dep. Química e Bioquímica
BioISI
Carles Bo (Author)
Summary
We present a density functional theory study for the photochemical water oxidation reaction promoted by uranyl nitrate upon sunlight radiation. First, we explored the most stable uranyl complex in the absence of light. The reaction in a dark environmen proceeds through the condensation of uranyl monomers to form dimeric hydroxo-bridged species, which is the first step toward a hydrogen evolution reaction (HER). We found a triplet-state-driven mechanism that leads to the formation of uranyl peroxide and hydrogen gas. To describe in detail this reaction path, we characterized the singlet and triplet low-lying states of the dimeric hydroxo-bridged species, including minima, transition states, minimal energy crossing points, and adiabatic energies. Our computational results provide mechanistic insights that are in good agreement with the experimental data available.
Date of Publication
2020-06-04
Where published
Inorganic Chemistry
Publication Identifiers
ISSN - 0020-1669
Publisher
American Chemical Society (ACS)
Number of pages
7
Starting page
8353
Last page
8360
Document Identifiers
DOI -
https://doi.org/10.1021/acs.inorgchem.0c00757
URL -
http://dx.doi.org/10.1021/acs.inorgchem.0c00757
Rankings
SCIMAGO Q1 (2019) - 1.349 - Chemistry (miscellaneous)
SCIMAGO Q1 (2019) - 1.349 - Inorganic Chemistry
SCIMAGO Q1 (2019) - 1.349 - Physical and Theoretical Chemistry
SCOPUS Q1 (2019) - 7.9 - Physical and Theoretical Chemistry
SCOPUS Q1 (2019) - 7.9 - Inorganic Chemistry
Web Of Science Q1 (2019) - 4.825 - CHEMISTRY, INORGANIC & NUCLEAR - SCIE
SCIMAGO Q1 (2020) - 1.348 - Chemistry (miscellaneous)
Web Of Science Q1 (2020) - 5.165 - CHEMISTRY, INORGANIC & NUCLEAR - SCIE