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ChemSusChem ; 10(22): 4561-4569, 2017 11 23.
Artigo em Inglês | MEDLINE | ID: mdl-28941193

RESUMO

Bio-mimetic catalysts such as LnCo3 (OR)4 (Ln=Er, Tm; OR=alkoxide) cubanes have recently been in the focus of research for artificial water oxidation processes. Previously, the remarkable adaptability with respect to ligand shell, nuclear structure as well as protonation and oxidation states of those catalysts has been shown to be beneficial for the water oxidation process. We further explored the structural flexibility of those catalysts and present here a series of novel structures in which one metal center is pulled out of the cubane cage. This leads to an open cubane core, which is to some extent reminiscent of observed open/closed cubane-core forms of the oxygen-evolving complex in nature's photosystem II. We investigate how those open cubane core models alter the thermodynamics of the water oxidation cycle and how different solvation approaches influence their stability.


Assuntos
Materiais Biomiméticos/química , Lantânio , Compostos Organometálicos/química , Água/química , Carbono , Catálise , Ligantes , Oxirredução , Complexo de Proteína do Fotossistema II , Termodinâmica
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