Abstract
Peroxygenases require a controlled supply of H2O2 to operate efficiently. Here, we propose a photocatalytic system for the reductive activation of ambient O2 to produce H2O2 which uses the energy provided by visible light more efficiently based on the combination of wavelength-complementary photosensitizers. This approach was coupled to an enzymatic system to make formate available as a sacrificial electron donor. The scope and current limitations of this approach are reported and discussed.
Highlights
Peroxygenases are receiving tremendous interest as catalysts for selective oxyfunctionalization reactions.[1−3] Compared to the well-known P450 monooxygenases, peroxygenases exhibit a comparable reactivity pattern as both rely on an oxyferryl species (Compound I) as catalytically active compound
To generate Compound I, P450 monooxygenases rely on complicated electron transport chains while peroxygenases require only hydrogen peroxide
EMnozyremareticcenHtl2yO, 2algseoneerlaetcitornocshyesmteimcasl4h,9a−v1e2 been and developed.[5−8] photocatalytic alternatives have moved into the focus.[13−18] The latter bear the promise of utilizing sunlight as a thermodynamic driving force to promote selective oxyfunctionalization reactions
Summary
Peroxygenases are receiving tremendous interest as catalysts for selective oxyfunctionalization reactions.[1−3] Compared to the well-known P450 monooxygenases, peroxygenases exhibit a comparable reactivity pattern as both rely on an oxyferryl species (Compound I) as catalytically active compound. Proposed Photoenzymatic System for in Situ Generation of H2O2 To Promote Peroxygenase-Catalyzed Hydroxylation Reactions Drawing correlations between the physicochemical and structural properties of the photocatalysts and their activity (Table 1) is difficult as factors such as redox potential, photoexcitability, and reactivity of the reduced form with O2 contribute to the macroscopically observed H2O2 generation rate.
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