NDLI: Layered manganese oxides for water-oxidation: alkaline earth cations influence catalytic activity in a photosystem II-like fashion

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Chemical Science Vol - 3 Issue - 6

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Layered manganese oxides for water-oxidation: alkaline earth cations influence catalytic activity in a photosystem II-like fashion

Content Provider	Royal Society of Chemistry (RSC)
Author	Kurz, Philipp Zaharieva, Ivelina Dau, Holger Wiechen, Mathias
Copyright Year	2012
Abstract	In reaction sequences for light driven water-splitting into H2 and O2, water-oxidation is a crucial reaction step. In vivo, the process is catalysed within a photoenzyme called photosystem II (PSII) by a μ-oxido CaMn4 cluster, the oxygen-evolving complex (OEC). The OEC is known to be virtually inactive if Ca2+ is removed from its structure. Activity can be restored not only by the addition of Ca2+ but also Sr2+ ions. We have recently introduced layered calcium manganese oxides of the birnessite mineral family as functional synthetic model compounds for the OEC. Here, we present the syntheses of layered manganese oxides where we varied the interlayer cations, preparing a series of K-, Ca-, Sr- and Mg-containing birnessites. Structural motifs within these materials were determined using X-ray absorption spectroscopy (XAS) showing that all materials have similar atomic structures despite their different elemental compositions. Water-oxidation experiments were carried out to elucidate structure-reactivity relations. These experiments demonstrated that the oxides—like the OEC—require the presence of calcium in their structures to reach maximum catalytic activity. As another similarity to the OEC, Sr2+ is the “second best choice” for the secondary cation. The results thus support mechanistic proposals which involve an important catalytic role for Ca2+ in biological water-oxidation. Additionally, they offer valuable hints for the development of synthetic, manganese-based water-oxidation catalysts for artificial photosynthesis.
Starting Page	2330
Ending Page	2339
Page Count	10
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	3
Issue Number	7
Journal	Chemical Science
DOI	10.1039/c2sc20226c
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Birnessite Mineral Absorption spectroscopy Oxygen Calcium Artificial photosynthesis Oxygen-evolving complex Ion Photosystem II X-ray absorption spectroscopy OEC Manganese
Content Type	Text
Resource Type	Article
Subject	Chemistry

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Layered manganese oxides for water-oxidation: alkaline earth cations influence catalytic activity in a photosystem II-like fashion

Structural Changes of the Oxygen-evolving Complex in Photosystem II during the Catalytic Cycle

Calcium EXAFS establishes the Mn-Ca cluster in the oxygen-evolving complex of Photosystem II

Calcium EXAFS establishes the Mn-Ca cluster in the oxygen-evolving complex of Photosystem II

X-ray and vibrational spectroscopy of manganese complexes relevant to the oxygen-evolving complex of photosynthesis

Capturing the sequence of events during the water oxidation reaction in photosynthesis using XFELs

X-ray absorption spectroscopy

X-ray spectroscopy of the photosynthetic oxygen-evolving complex

X-ray absorption spectroscopy on the calcium cofactor to the manganese cluster in photosynthetic oxygen evolution

Layered manganese oxides for water-oxidation: alkaline earth cations influence catalytic activity in a photosystem II-like fashion

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