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2023 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 11, no 20, p. 10669-10676Article in journal (Refereed) Published
Abstract [en]
Water oxidation is the holy grail reaction of natural and artificial photosynthesis. How to design an efficient water-oxidation catalyst remains a long-term challenge for solar fuel production. The rate of water oxidation in photosystem II by the oxygen-evolving complex (OEC) Mn4CaO5 cluster is as high as 100-400 s−1. Mimicking the structures of the OEC is a straightforward strategy to design water-oxidation catalysts. However, the high efficiency of the OEC relies on not only its highly active site but also its holistic system for well-organized electron transfer and proton transport. Lacking such a holistic functional system makes δ-MnO2 a poor water-oxidation catalyst, although the local structure of δ-MnO2 is similar to that of the Mn4CaO5 cluster. Electrocatalysts simultaneously imitating the catalytically active sites, fast electron transfer, and promoted proton transport in a natural OEC have been rarely reported. The significance of the synergy of a holistic system is underrated in the design of water-oxidation catalysts. In this work, we fabricated holistic functional biomimetic composites of two-dimensional manganese oxide nanosheets and pyridyl-modified graphene (MnOx-NS/py-G) for electrocatalytic water oxidation. MnOx-NS/py-G simultaneously imitates the synergy of catalytically active sites, fast electron transfer, and promoted proton transport in a natural OEC, resulting in overall 600 times higher activity than that of typical δ-MnO2. This work demonstrates the significance of holistic functional biomimetic design and guides the development of highly active electrocatalysts for small molecule activation related to solar energy storage.
Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2023
National Category
Physical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-331571 (URN)10.1039/d3ta01040f (DOI)000983915400001 ()2-s2.0-85159156124 (Scopus ID)
Note
QC 20230711
2023-07-112023-07-112023-09-06Bibliographically approved