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van Schie, M.M.C.H. (author), Kaczmarek, Alexander T. (author), Tieves, F. (author), Gomez de Santos, Patricia (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Alcalde, Miguel (author), Schwarz, Günter (author), Hollmann, F. (author)H<sub>2</sub>O<sub>2</sub> can be accepted by several peroxygenases as a clean oxidant, able to supply both the necessary electrons and oxygen atom at the same time. The biocatalysts, in turn, are able to catalyse an array of interesting oxygen insertion reactions at enantio- and regio-selectivities hard to attain with classical chemical...journal article 2020
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Höfler, G.T. (author), But, A. (author), Younes, S.H.H. (author), Wever, Ron (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The scale-up of chemoenzymatic bromolactonization to 100 g scale is presented, together with an identification of current limitations. The preparative-scale reaction also allowed for meaningful mass balances identifying current bottlenecks of the chemoenzymatic reaction.journal article 2020
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Willot, S.J. (author), Hoang, Manh Dat (author), Paul, C.E. (author), Alcalde, Miguel (author), Arends, I.W.C.E. (author), Bommarius, Andreas S. (author), Bommarius, Bettina (author), Hollmann, F. (author)The novel formate oxidase from Aspergillus oryzae (AoFOx) is a useful catalyst to promote H<sub>2</sub>O<sub>2</sub>-dependent oxyfunctionalisation reactions. In this contribution we exploit the substrate promiscuity of AoFOx to fully oxidise methanol and formaldehyde to CO<sub>2</sub> and drive peroxygenase-catalysed stereoselective...journal article 2020
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Rauch, M.C.R. (author), Huijbers, M.M.E. (author), Pabst, Martin (author), Paul, C.E. (author), Pesic, M. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Direct, NAD(P)H-independent regeneration of Old Yellow Enzymes represents an interesting approach for simplified reaction schemes for the stereoselective reduction of conjugated C=C-double bonds. Simply by illuminating the reaction mixtures with blue light in the presence of sacrificial electron donors enables to circumvent the costly and...journal article 2020
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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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van Schie, M.M.C.H. (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Two-component-diffusible-flavomonooxygenases are versatile biocatalysts for selective epoxidation-, hydroxylation- or halogenation reactions. Their complicated molecular architecture can be simplified using photochemical regeneration of the catalytically active, reduced FADH <sub>2</sub> prosthetic group. In this contribution we provide the...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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Rauch, M.C.R. (author), Gallou, Y. (author), Delorme, L. (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Elemental metals are shown to be suitable sacrificial electron donors to drive the stereoselective reduction of conjugated C=C double bonds using Old Yellow Enzymes as catalysts. Both direct electron transfer from the metal to the enzyme as well as mediated electron transfer is feasible, although the latter excels by higher reaction rates....journal article 2019
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Gacs, Jenő (author), Zhang, W. (author), Knaus, Tanja (author), Mutti, Francesco G. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The consecutive photooxidation and reductive amination of various alcohols in a cascade reaction were realized by the combination of a photocatalyst and several enzymes. Whereas the photocatalyst (sodium anthraquinone-2-sulfonate) mediated the light-driven, aerobic oxidation of primary and secondary alcohols, the enzymes (various ω...journal article 2019
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van Schie, M.M.C.H. (author), Zhang, W. (author), Tieves, F. (author), Choi, Da Som (author), Park, Chan Beum (author), Burek, Bastien O. (author), Bloh, Jonathan Z. (author), Arends, I.W.C.E. (author), Paul, C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H<sub>2</sub>O<sub>2</sub> can be addressed via in situ generation of H<sub>2</sub>O<sub>2<...journal article 2019
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Rauch, M.C.R. (author), Tieves, F. (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)Biocatalytic oxyfunctionalisation reactions are traditionally conducted in aqueous media limiting their production yield. Here we report the application of a peroxygenase in neat reaction conditions reaching product concentrations of up to 360 mM.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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van Schie, M.M.C.H. (author), Younes, S.H.H. (author), Rauch, M.C.R. (author), Pesic, M. (author), Paul, C.E. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Deazaflavins are potentially useful redox mediators for the direct, nicotinamide-independent regeneration of oxidoreductases. Especially the O<sub>2</sub>-stability of their reduced forms have attracted significant interest for the regeneration of monooxygenases. In this contribution we further investigate the photochemical properties of...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), Gacs, Jenő (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The aerobic organocatalytic oxidation of alcohols was achieved by using water-soluble sodium anthraquinone sulfonate. Under visible-light activation, this catalyst mediated the aerobic oxidation of alcohols to aldehydes and ketones. The photo-oxyfunctionalization of alkanes was also possible under these conditions.journal article 2017
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Rauch, M.C.R. (author), Schmidt, S. (author), Arends, I.W.C.E. (author), oppelt, K. (author), Kara, S (author), Hollmann, F. (author)The photocatalytic oxidation of NADH using a flavin photocatalyst and a simple blue LED light source is reported. This in situ NAD+ regeneration system can be used to promote biocatalytic, enantioselective oxidation reactions. Compared to the traditional use of white light bulbs this method enables very significant reductions in energy...journal article 2016
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Holtmann, D. (author), Fraaije, M.W. (author), Arends, I.W.C.E. (author), Oppermand, D.J. (author), Hollmann, F. (author)The scope and limitations of oxygenases as catalysts for preparative organic synthesis is discussed.journal article 2014
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De Torres, M. (author), Dimroth, J. (author), Arends, I.W.C.E. (author), Keilitz, J. (author), Hollmann, F. (author)Rh(III)-TsDPEN, an immobilized analog of the well-known [Cp*Rh(bpy)(H2O)]2+ was evaluated as a heterogeneous, recyclable regeneration catalyst for reduced oxidoreductase cofactors [NAD(P)H]. Repeated use of this catalyst was established and the catalytic properties were initially investigated. Apparently, Rh(III)-TsDPEN is prone to severe...journal article 2012
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Hollmann, F. (author), Arends, I.W.C.E. (author)Biocatalysis is propagating into practically every area of organic chemistry, amongst them radical polymerizations. A review of the recent developments of this dynamic and quickly evolving area of research is presented together with a critical evaluation of its potential to yield novel polymers and/or environmentally more benign synthetic...journal article 2012
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Perez, D.I. (author), Grau, M.M. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Robust peroxidase-catalyzed enantiospecific oxyfunctionalizations can be achieved by simple light-driven in situ generation of hydrogen peroxide.journal article 2009