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Discovery of Open Cubane Core Structures for Biomimetic LnCo3 (OR)4 Water Oxidation Catalysts


Schilling, Mauro; Hodel, Florian H; Luber, Sandra (2017). Discovery of Open Cubane Core Structures for Biomimetic LnCo3 (OR)4 Water Oxidation Catalysts. ChemSusChem, 10(22):4561-4569.

Abstract

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.

Abstract

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.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Uncontrolled Keywords:General Energy, General Materials Science, General Chemical Engineering, Environmental Chemistry
Language:English
Date:23 November 2017
Deposited On:28 Dec 2017 07:21
Last Modified:24 Sep 2018 00:00
Publisher:Wiley-VCH Verlag
ISSN:1864-5631
Funders:Swiss National Science Foundation, National Center of Competence in Research "Materials Revolution: Computational Design and Discovery of Novel Materials" (NCCR-MARVEL), University Research Priority Program "Solar Light to Chemical Energy Conversion" (LightChEC)
OA Status:Green
Publisher DOI:https://doi.org/10.1002/cssc.201701527
Project Information:
  • : FunderSNSF
  • : Grant ID
  • : Project TitleSwiss National Science Foundation
  • : Funder
  • : Grant ID
  • : Project TitleNational Center of Competence in Research "Materials Revolution: Computational Design and Discovery of Novel Materials" (NCCR-MARVEL)
  • : Funder
  • : Grant ID
  • : Project TitleUniversity Research Priority Program "Solar Light to Chemical Energy Conversion" (LightChEC)

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