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Yayci, Abdulkadir (author), Baraibar, Álvaro Gómez (author), Krewing, Marco (author), Fernandez Fueyo, E. (author), Hollmann, F. (author), Alcalde, Miguel (author), Kourist, Robert (author), Bandow, Julia E. (author)Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one-electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a...journal article 2020
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Tieves, F. (author), Tonin, F. (author), Fernandez Fueyo, E. (author), Robbins, John M. (author), Bommarius, Bettina (author), Bommarius, Andreas S. (author), Alcalde, Miguel (author), Hollmann, F. (author)The E-factor has become an important measure for the environmental impact of (bio)chemical reactions. However, summing up the obvious wastes generated in the laboratory neglects energy-related wastes (mostly greenhouse gases) which are generated elsewhere. To estimate these wastes, we propose to extend the E-factor by an energy-term (E<sup>+<...journal article 2019
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Willot, S.J. (author), Fernandez Fueyo, E. (author), Tieves, F. (author), Pesic, M. (author), Alcalde, Miguel (author), Arends, I.W.C.E. (author), Park, Chan Beum (author), Hollmann, F. (author)Peroxygenases require a controlled supply of H<sub>2</sub>O<sub>2</sub> to operate efficiently. Here, we propose a photocatalytic system for the reductive activation of ambient O<sub>2</sub> to produce H<sub>2</sub>O<sub>2</sub> which uses the energy provided by visible light more efficiently based on the combination of wavelength...journal article 2019
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Pedroso de Almeida, T. (author), van Schie, M.M.C.H. (author), Ma, A. (author), Tieves, F. (author), Younes, S.H.H. (author), Fernandez Fueyo, E. (author), Arends, I.W.C.E. (author), Riul, A. (author), Hollmann, F. (author)The selective oxidation of trans-2-hexen-1-ol to the corresponding aldehyde using a recombinant aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) is reported. Especially using the two liquid phase system to overcome solubility and product inhibition issues enabled to achieve more than 2.200.000 catalytic turnovers for the production enzyme...journal article 2019
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van Schie, M.M.C.H. (author), Pedroso de Almeida, T. (author), Laudadio, Gabriele (author), Tieves, F. (author), Fernandez Fueyo, E. (author), Noël, Timothy (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The biocatalytic preparation of trans-hex-2-enal from trans-hex-2-enol using a novel aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) is reported. As O<sub>2</sub>-dependent enzyme PeAAOx-dependent reactions are generally plagued by the poor solubility of O<sub>2</sub> in aqueous media and mass transfer limitations resulting in poor...journal article 2018
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Dong, J. (author), Fernandez Fueyo, E. (author), Hollmann, F. (author), Paul, C.E. (author), Pesic, M. (author), Schmidt, S. (author), Wang, Yonghua (author), Younes, S.H.H. (author), Zhang, W. (author)Oxidation chemistry using enzymes is approaching maturity and practical applicability in organic synthesis. Oxidoreductases (enzymes catalysing redox reactions) enable chemists to perform highly selective and efficient transformations ranging from simple alcohol oxidations to stereoselective halogenations of non‐activated C−H bonds. For many of...journal article 2018
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Zhang, W. (author), Fernandez Fueyo, E. (author), Ni, Y. (author), van Schie, M.M.C.H. (author), Gacs, Jenö (author), Renirie, R. (author), Wever, Ron (author), Mutti, Francesco G. (author), Rother, Dörte (author), Alcalde, Miguel (author), Hollmann, F. (author)Peroxygenases offer an attractive means to address challenges in selective oxyfunctionalization chemistry. Despite this, their application in synthetic chemistry remains challenging due to their facile inactivation by the stoichiometric oxidant H<sub>2</sub>O<sub>2</sub>. Often atom-inefficient peroxide generation systems are required, which...journal article 2018
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Combining Photo-Organo Redox- and Enzyme Catalysis Facilitates Asymmetric C-H Bond FunctionalizationZhang, W. (author), Fernandez Fueyo, E. (author), Hollmann, F. (author), Leemans Martin, L. (author), Pesic, M. (author), Wardenga, Rainer (author), Höhne, Matthias (author), Schmidt, S. (author)In this study, we combined photo-organo redox catalysis and biocatalysis to achieve asymmetric C–H bond functionalization of simple alkane starting materials. The photo-organo catalyst anthraquinone sulfate (SAS) was employed to oxyfunctionalise alkanes to aldehydes and ketones. We coupled this light-driven reaction with asymmetric enzymatic...journal article 2018
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Pesic, M. (author), Willot, S.J. (author), Fernandez Fueyo, E. (author), Tieves, F. (author), Alcalde, Miguel (author), Hollmann, F. (author)There is an increasing interest in the application of peroxygenases in biocatalysis, because of their ability to catalyse the oxyfunctionalisation reaction in a stereoselective fashion and with high catalytic efficiencies, while using hydrogen peroxide or organic peroxides as oxidant. However, enzymes belonging to this class exhibit a very...journal article 2018
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Höfler, G.T. (author), Fernandez Fueyo, E. (author), Pesic, M. (author), Younes, S.H.H. (author), Choi, Eun Gyu (author), Kim, Yong H. (author), Urlacher, Vlada B. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)A photoenzymatic NADH regeneration system was established. The combination of deazariboflavin as a photocatalyst with putidaredoxin reductase enabled the selective reduction of NAD<sup>+</sup> into the enzyme-active 1,4-NADH to promote an alcohol dehydrogenase catalysed stereospecific reduction reaction. The catalytic turnover of all the...journal article 2018
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Zhang, W. (author), Burek, Bastien O. (author), Fernandez Fueyo, E. (author), Alcalde, Miguel (author), Bloh, Jonathan Z. (author), Hollmann, F. (author)Selective oxyfunctionalizations of inert C−H bonds can be achieved under mild conditions by using peroxygenases. This approach, however, suffers from the poor robustness of these enzymes in the presence of hydrogen peroxide as the stoichiometric oxidant. Herein, we demonstrate that inorganic photocatalysts such as gold–titanium dioxide...journal article 2017
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Martínez, Angel T. (author), Ruiz-Dueñas, Francisco J. (author), Camarero, Susana (author), Serrano, Ana (author), Linde, Dolores (author), Lund, Henrik (author), Vind, Jesper (author), Tovborg, Morten (author), Herold-Majumdar, Owik M. (author), Hofrichter, Martin (author), Liers, Christiane (author), Ullrich, René (author), Scheibner, Katrin (author), Sannia, Giovanni (author), Piscitelli, Alessandra (author), Pezzella, Cinzia (author), Sener, Mehmet E. (author), Kılıç, Sibel (author), van Berkel, Willem J.H. (author), Guallar, Victor (author), Lucas, Maria Fátima (author), Zuhse, Ralf (author), Ludwig, Roland (author), Hollmann, F. (author), Fernandez Fueyo, E. (author), Record, Eric (author), Faulds, Craig B. (author), Tortajada, Marta (author), Winckelmann, Ib (author), Rasmussen, Jo Anne (author), Gelo-Pujic, Mirjana (author), Gutiérrez, Ana (author), del Río, José C. (author), Rencoret, Jorge (author), Alcalde, Miguel (author)Fungi produce heme-containing peroxidases and peroxygenases, flavin-containing oxidases and dehydrogenases, and different copper-containing oxidoreductases involved in the biodegradation of lignin and other recalcitrant compounds. Heme peroxidases comprise the classical ligninolytic peroxidases and the new dye-decolorizing peroxidases, while...review 2017
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Dong, J. (author), Fernandez Fueyo, E. (author), Li, Jingbo (author), Guo, Zheng (author), Renirie, Rokus (author), Wever, Ron (author), Hollmann, F. (author)The vanadium-dependent chloroperoxidase from Curvularia inaequalis is a stable and efficient biocatalyst for the hydroxyhalogenation of a broad range of alkenes into halohydrins. Up to 1 200 000 TON with 69 s−1 TOF were observed for the biocatalyst. A bienzymatic cascade to yield epoxides as reaction products is presented.journal article 2017
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Choi, Da Som (author), Ni, Y. (author), Fernandez Fueyo, E. (author), Lee, Minah (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases are very promising catalysts for oxyfunctionalization reactions. Their practical applicability, however, is hampered by their sensitivity against the oxidant (H<sub>2</sub>O<sub>2</sub>), therefore necessitating in situ generation of H<sub>2</sub>O<sub>2</sub>. Here, we report a photoelectrochemical approach to provide...journal article 2017
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Pesic, M. (author), Fernandez Fueyo, E. (author), Hollmann, F. (author)Old Yellow Enzymes (OYEs) have become practical catalysts for the stereoselective trans-hydrogenation of conjugated C=C-double bonds. Despite their importance, in-depth characterization of their kinetic parameters and factors influencing their activity and stability have largely been neglected in the past years. In this study, we close this...journal article 2017
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Gjonaj, L. (author), Pinkse, M.W.H. (author), Fernandez Fueyo, E. (author), Hollmann, F. (author), Hanefeld, U. (author)Nitrile reductases catalyse a two-step reduction of nitriles to amines. This requires the binding of two NADPH molecules during one catalytic cycle. For the nitrile reductase from E. coli (EcoNR) mass spectrometry studies of the catalytic mechanism were performed. EcoNR is dimeric and has no Rossman fold. It was demonstrated that during...journal article 2016
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Fernandez Fueyo, E. (author), Younes, S.H.H. (author), Van Rootselaar, Stefan (author), Aben, René W M (author), Renirie, R. (author), Wever, Ron (author), Holtmann, Dirk (author), Rutjes, Floris P J T (author), Hollmann, F. (author)A catalytic, enzyme-initiated (aza-) Achmatowicz reaction is presented. The involvement of a robust vanadium-dependent peroxidase from Curvularia inaequalis allows the simple use of H<sub>2</sub>O<sub>2</sub> and catalytic amounts of bromide.journal article 2016
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Fernandez Fueyo, E. (author), Ni, Y. (author), Gomez Baraibar, A. (author), Alcalde, Miguel (author), van Langen, L.M. (author), Hollmann, F. (author)The peroxygenase from Agrocybe aegerita (AaeUPO) has been evaluated for stereoselective oxyfunctionalization chemistry under non-aqueous reaction conditions. The stereoselective hydroxylation of ethylbenzene to (R)-1-phenylethanol was performed in neat substrate as reaction medium together with the immobilized biocatalyst and <sup>tert</sup...journal article 2016
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Peroxygenase-catalyzed oxyfunctionalization reactions promoted by the complete oxidation of methanolNi, Y. (author), Fernandez Fueyo, E. (author), Baraibar, AG (author), Ullrich, R (author), Hofrichter, Martin (author), Yanase, H (author), Alcalde, Miguel (author), van Berkel, WJH (author), Hollmann, F. (author)Peroxygenases catalyze a broad range of (stereo)selective oxyfunctionalization reactions. However, to access their full catalytic potential, peroxygenases need a balanced provision of hydrogen peroxide to achieve high catalytic activity while minimizing oxidative inactivation. Herein, we report an enzymatic cascade process that employs methanol...journal article 2016