BIBLIOS

Tipo
Artigos em Revista

Tipo de Documento
Artigo Completo

Título
Unveiling a Photoinduced Hydrogen Evolution Reaction Mechanism via the Concerted Formation of Uranyl Peroxide

Participantes na publicação
Enric Petrus (Author)
Mireia Segado (Author)
Nuno A. G. Bandeira (Author)
Dep. Química e Bioquímica
BioISI
Carles Bo (Author)

Resumo
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.


Suporte
Inorganic Chemistry

Identificadores da Publicação
ISSN - 0020-1669

Editora
American Chemical Society (ACS)



Identificadores do Documento
DOI - https://doi.org/10.1021/acs.inorgchem.0c00757
URL - http://dx.doi.org/10.1021/acs.inorgchem.0c00757

Identificadores de Qualidade
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