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Photoinduced hole t...
Photoinduced hole transfer from tris(bipyridine)ruthenium dye to a high-valent iron-based water oxidation catalyst
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- Shylin, Sergii I. (författare)
- Uppsala universitet,Fysikalisk kemi
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- Pavliuk, Mariia V. (författare)
- Uppsala universitet,Fysikalisk kemi,Uppsala Univ, Angstrom Lab, Dept Chem, POB 523, S-75120 Uppsala, Sweden
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- D'Amario, Luca (författare)
- Uppsala universitet,Fysikalisk kemi,Free Univ Berlin, Phys Dept, Arnimallee 14, D-14195 Berlin, Germany
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- Fritsky, Igor O. (författare)
- Taras Shevchenko Natl Univ Kyiv, Dept Chem, Volodymyrska 64, UA-01601 Kiev, Ukraine;PBMR Labs Ukraine, Murmanska 1, UA-02094 Kiev, Ukraine
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- Berggren, Gustav (författare)
- Uppsala universitet,Molekylär biomimetik
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(creator_code:org_t)
- 2019
- 2019
- Engelska.
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Ingår i: Faraday discussions. - : ROYAL SOC CHEMISTRY. - 1359-6640 .- 1364-5498. ; 215, s. 162-174
- Relaterad länk:
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https://doi.org/10.1...
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https://uu.diva-port... (primary) (Raw object)
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https://pubs.rsc.org...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
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- An efficient water oxidation system is a prerequisite for developing solar energy conversion devices. Using advanced time-resolved spectroscopy, we study the initial catalytic relevant electron transfer events in the light-driven water oxidation system utilizing [Ru(bpy)(3)](2+) (bpy = 2,2 '-bipyridine) as a light harvester, persulfate as a sacrificial electron acceptor, and a high-valent iron clathrochelate complex as a catalyst. Upon irradiation by visible light, the excited state of the ruthenium dye is quenched by persulfate to afford a [Ru(bpy)(3)](3+)/SO4- pair, showing a cage escape yield up to 75%. This is followed by the subsequent fast hole transfer from [Ru(bpy)(3)](3+) to the Fe-IV catalyst to give the long-lived Fe-V intermediate in aqueous solution. In the presence of excess photosensitizer, this process exhibits pseudo-first order kinetics with respect to the catalyst with a rate constant of 3.2(1) x 10(10) s(-1). Consequently, efficient hole scavenging activity of the high-valent iron complex is proposed to explain its high catalytic performance for water oxidation.
Ämnesord
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
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