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Copper(II) defect-cubane water oxidation electrocatalysts: from molecular tetramers to oxidic nanostructures


Adiyeri Saseendran, Devi Prasad; Fischer, Jörg W A; Müller, Lea; Abbott, Daniel F; Mougel, Victor; Jeschke, Gunnar; Triana, Carlos A; Patzke, Greta R (2023). Copper(II) defect-cubane water oxidation electrocatalysts: from molecular tetramers to oxidic nanostructures. Chemical Communications, 59(39):5866-5869.

Abstract

We report on the synthesis and spectroscopic evidence for a sequence of structural transformations of a new defect-cubane type copper complex, [Cu4(pyalk)4(OAc)4](ClO4)(HNEt3), which acts as a pre-catalyst for water oxidation. In situ and post-catalytic studies showed that the tetrameric complex undergoes a structural transformation into dimeric and monomeric species, induced by water molecules and carbonate anions, respectively. Further, the observed electrocatalytic water oxidation activity has been confirmed to arise from in situ-generated Cu(II) oxidic nanostructures at the electrode interface.

Abstract

We report on the synthesis and spectroscopic evidence for a sequence of structural transformations of a new defect-cubane type copper complex, [Cu4(pyalk)4(OAc)4](ClO4)(HNEt3), which acts as a pre-catalyst for water oxidation. In situ and post-catalytic studies showed that the tetrameric complex undergoes a structural transformation into dimeric and monomeric species, induced by water molecules and carbonate anions, respectively. Further, the observed electrocatalytic water oxidation activity has been confirmed to arise from in situ-generated Cu(II) oxidic nanostructures at the electrode interface.

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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
Scopus Subject Areas:Physical Sciences > Electronic, Optical and Magnetic Materials
Physical Sciences > Catalysis
Physical Sciences > Ceramics and Composites
Physical Sciences > General Chemistry
Physical Sciences > Surfaces, Coatings and Films
Physical Sciences > Metals and Alloys
Physical Sciences > Materials Chemistry
Uncontrolled Keywords:Materials Chemistry, Metals and Alloys, Surfaces, Coatings and Films, General Chemistry, Ceramics and Composites, Electronic, Optical and Magnetic Materials, Catalysis
Language:English
Date:24 April 2023
Deposited On:20 Feb 2024 09:09
Last Modified:29 Jun 2024 01:41
Publisher:Royal Society of Chemistry
ISSN:1359-7345
OA Status:Hybrid
Publisher DOI:https://doi.org/10.1039/d3cc01005h
PubMed ID:37089062
  • Content: Published Version
  • Language: English
  • Licence: Creative Commons: Attribution-NonCommercial 4.0 International (CC BY-NC 4.0)