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Water Oxidation by Pentapyridyl Base Metal Complexes? : A Case Study

Boniolo, Manuel (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Hossain, Md Kamal (författare)
Uppsala universitet,Syntetisk molekylär kemi,Synthetic Molecular Chemistry, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Chernev, Petko (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
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Suremann, Nina F. (författare)
Uppsala universitet,Syntetisk molekylär kemi,Synthetic Molecular Chemistry, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Heizmann, Philipp A. (författare)
Uppsala universitet,Syntetisk molekylär kemi,Synthetic Molecular Chemistry, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Lyvik, Amanda S.L. (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Beyer, Paul (författare)
Physics Department, Freie Universität Berlin, 14195 Berlin, Germany
Haumann, Michael (författare)
Physics Department, Freie Universität Berlin, 14195 Berlin, Germany
Huang, Ping (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Salhi-Benachenhou, Nessima (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Cheah, Mun Hon (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Shylin, Sergii I. (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Lundberg, Marcus, 1974- (författare)
Uppsala universitet,Molekylär biomimetik,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Thapper, Anders (författare)
Uppsala universitet,Syntetisk molekylär kemi,Synthetic Molecular Chemistry, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
Messinger, Johannes, 1963- (författare)
Umeå universitet,Uppsala universitet,Molekylär biomimetik,Department of Chemistry, Chemical Biological Centre, Umeå University, 90187 Umeå, Sweden,Kemiska institutionen,Molecular Biomimetics, Department of Chemistry, Ångström Laboratory, Uppsala University, Uppsala, Sweden
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 (creator_code:org_t)
2022-06-06
2022
Engelska.
Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 61:24, s. 9104-9118
Relaterad länk:
https://doi.org/10.1...
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https://doi.org/10.1...
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  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
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  • The design of molecular water oxidation catalysts (WOCs) requires a rational approach that considers the intermediate steps of the catalytic cycle, including water binding, deprotonation, storage of oxidizing equivalents, O–O bond formation, and O2 release. We investigated several of these properties for a series of base metal complexes (M = Mn, Fe, Co, Ni) bearing two variants of a pentapyridyl ligand framework, of which some were reported previously to be active WOCs. We found that only [Fe(Py5OMe)Cl]+ (Py5OMe = pyridine-2,6-diylbis[di-(pyridin-2-yl)methoxymethane]) showed an appreciable catalytic activity with a turnover number (TON) = 130 in light-driven experiments using the [Ru(bpy)3]2+/S2O82– system at pH 8.0, but that activity is demonstrated to arise from the rapid degradation in the buffered solution leading to the formation of catalytically active amorphous iron oxide/hydroxide (FeOOH), which subsequently lost the catalytic activity by forming more extensive and structured FeOOH species. The detailed analysis of the redox and water-binding properties employing electrochemistry, X-ray absorption spectroscopy (XAS), UV–vis spectroscopy, and density-functional theory (DFT) showed that all complexes were able to undergo the MIII/MII oxidation, but none was able to yield a detectable amount of a MIV state in our potential window (up to +2 V vs SHE). This inability was traced to (i) the preference for binding Cl– or acetonitrile instead of water-derived species in the apical position, which excludes redox leveling via proton coupled electron transfer, and (ii) the lack of sigma donor ligands that would stabilize oxidation states beyond MIII. On that basis, design features for next-generation molecular WOCs are suggested.

Ämnesord

NATURVETENSKAP  -- Kemi -- Oorganisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)

Nyckelord

Artificial photosynthesis
water oxidation
catalysis
Chemistry with specialization in Inorganic Chemistry
Kemi med inriktning mot oorganisk kemi

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