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Hydroxyl-Decorated Diiron Complex as a [FeFe]-Hydrogenase Active Site Model Complex : Light-Driven Photocatalytic Activity and Heterogenization on Ethylene-Bridged Periodic Mesoporous Organosilica
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- Amaro-Gahete, Juan (author)
- Univ Cordoba, Dept Quim Organ, Fac Ciencias, Inst Univ Nanoquim IUNAN, Edificio Marie Curie,Campus Univ Rabanales, E-14071 Cordoba, Spain.
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- Esquivel, Dolores (author)
- Univ Cordoba, Dept Quim Organ, Fac Ciencias, Inst Univ Nanoquim IUNAN, Edificio Marie Curie,Campus Univ Rabanales, E-14071 Cordoba, Spain.
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- Pavliuk, Mariia V. (author)
- Uppsala universitet,Fysikalisk kemi
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- Univ Cordoba, Dept Quim Organ, Fac Ciencias, Inst Univ Nanoquim IUNAN, Edificio Marie Curie,Campus Univ Rabanales, E-14071 Cordoba, Spain Fysikalisk kemi (creator_code:org_t)
- 2022-02-23
- 2022
- English.
- In: Catalysts. - : MDPI. - 2073-4344. ; 12:3
- Journal article (peer-reviewed)
Abstract
Subject headings
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- A biomimetic model complex of the [FeFe]-hydrogenase active site (FeFeOH) with an ethylene bridge and a pendant hydroxyl group has been synthesized, characterized and evaluated as catalyst for the light-driven hydrogen production. The interaction of the hydroxyl group present in the complex with 3-isocyanopropyltriethoxysilane provided a carbamate triethoxysilane bearing a diiron dithiolate complex (NCOFeFe), thus becoming a potentially promising candidate for anchoring on heterogeneous supports. As a proof of concept, the NCOFeFe precursor was anchored by a grafting procedure into a periodic mesoporous organosilica with ethane bridges (EthanePMO@NCOFeFe). Both molecular and heterogenized complexes were tested as catalysts for light-driven hydrogen generation in aqueous solutions. The photocatalytic conditions were optimized for the homogenous complex by varying the reaction time, pH, amount of the catalyst or photosensitizer, photon flux, and the type of light source (light-emitting diode (LED) and Xe lamp). It was shown that the molecular FeFeOH diiron complex achieved a decent turnover number (TON) of 70 after 6 h, while NCOFeFe and EthanePMO@NCOFeFe had slightly lower activities showing TONs of 37 and 5 at 6 h, respectively.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Keyword
- [FeFe]-hydrogenase
- periodic mesoporous organosilica
- biomimetic chemistry
- artificial photosynthesis
- light-driven hydrogen evolution
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