Identificador persistente para citar o vincular este elemento: http://hdl.handle.net/10553/74724
Título: Hydrogen Evolution in [NiFe] Hydrogenases: A Case of Heterolytic Approach between Proton and Hydride
Autores/as: Qiu, Siyao
Azofra Mesa, Luis Miguel 
Macfarlane, Douglas R.
Sun, Chenghua
Clasificación UNESCO: 221001 Catálisis
Fecha de publicación: 2019
Publicación seriada: Inorganic Chemistry 
Resumen: The mechanism for Hydrogen Evolution Reaction (HER) in [NiFe] hydrogenase enzymes distinguishes them from inorganic catalysts. The first H+/e– pair injected to the active site of the hydrogenases transforms into hydride, while the second H+/e– pair injection leads to the formation of the H–/H+ pair both binding to the active site. The two opposite charged hydrogens heterolytically approach each other in order to form dihydrogen (H2), which is enhanced by the Coulomb force. Two previously proposed reaction routes for this process have been examined by Conceptual Density Functional Theory (DFT) in this work. One presents better agreement with experimental spectra, while the other is thermodynamically more favorable. Both paths suggest that the approach and the charge transfer between the proton and hydride are motivated by the stabilization of the electronic activity and the electrophilicity of Ni. After the heterolytic approach of the proton and hydride moieties, the two hydrogen atoms attach to the Ni ion and combine homolytically.
URI: http://hdl.handle.net/10553/74724
ISSN: 0020-1669
DOI: 10.1021/acs.inorgchem.8b02812
Fuente: Inorganic Chemistry [ISSN 0020-1669], v. 58, 5, p. 2979-2986
Colección:Artículos
miniatura
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