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Willot, S.J. (author), Tieves, F. (author), Girhard, Marco (author), Urlacher, Vlada B. (author), Hollmann, F. (author), De Gonzalo, G. (author)A set of dual functional small molecules (DFSMs) containing different amino acids has been synthesized and employed together with three different variants of the cytochrome P450 monooxygenase P450BM3 from Bacillus megaterium in H2O2-dependent oxidation reactions. These DFSMs enhance P450BM3 activity with hydrogen peroxide as an oxidant,...journal article 2019
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Kim, Jinhyun (author), Lee, Sahng Ha (author), Tieves, F. (author), Paul, C.E. (author), Hollmann, F. (author), Park, Chan Beum (author)Nicotinamide adenine dinucleotide (NAD<sup>+</sup>) is a key redox compound in all living cells responsible for energy transduction, genomic integrity, life-span extension, and neuromodulation. Here, we report a new function of NAD<sup>+</sup> as a molecular photocatalyst in addition to the biological roles. Our spectroscopic and...journal article 2019
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Leemans, Laura (author), van Langen, Luuk (author), Hollmann, F. (author), Schallmey, Anett (author)A concurrent bienzymatic cascade for the synthesis of optically pure (S)-4-methoxymandelonitrile benzoate ((S)-3) starting from 4-anisaldehyde (1) has been developed. The cascade involves an enantioselective Manihot esculenta hydroxynitrile lyase-catalyzed hydrocyanation of 1, and the subsequent benzoylation of the resulting cyanohydrin (S)-2...journal article 2019
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Zhang, Jie (author), Tonin, F. (author), Zhang, W. (author), Hagedoorn, P.L. (author), Mallée, L. (author), Hollmann, F. (author)We report the use of commercial laundry powder as a biocatalyst for a range of lipase-catalysed reactions including (trans)esterification, ester hydrolysis and chemoenzymatic epoxidation reactions. The enzymatic laundry powder exhibited excellent stability and recyclability, making it a readily available and cheap biocatalyst for chemical...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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Chatzoudis, Apostolos (author), Giannopoulos, Vasileios (author), Hollmann, F. (author), Smonou, Ioulia (author)A new photocatalytic reactivity of carbon-nanodot-doped graphitic carbon nitride (CD-C<sub>3</sub>N<sub>4</sub>) with alkenes and dienes, has been disclosed. We have shown that CD-C<sub>3</sub>N<sub>4</sub> photosensitizes the oxidation of unsaturated substrates in a variety of solvents according to two competing mechanisms: the energy...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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Aslan-Üzel, Aşkın S. (author), Beier, Andy (author), Kovář, David (author), Cziegler, Clemens (author), Padhi, Santosh K. (author), Schuiten, Eva D. (author), Dörr, Mark (author), Böttcher, Dominique (author), Hollmann, F. (author)Halide assays are important for the study of enzymatic dehalogenation, a topic of great industrial and scientific importance. Here we describe the development of a very sensitive halide assay that can detect less than a picomole of bromide ions, making it very useful for quantifying enzymatic dehalogenation products. Halides are oxidised...journal article 2019
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Yoon, Jaeho (author), Lee, S.H. (author), Tieves, F. (author), Rauch, M.C.R. (author), Hollmann, F. (author), Park, Chan Beum (author)We report visible light-driven, asymmetric hydrogenation of C=C bonds using an ene-reductase from Thermus scotoductus SA-01 (TsOYE) and a light-harvesting dye (rose bengal, RB) co-immobilized in an alginate hydrogel. Highly efficient encapsulation of RB in alginate hydrogel was achieved using the intrinsic affinity between TsOYE and RB,...journal article 2019
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Bormann, Sebastian (author), van Schie, M.M.C.H. (author), Pedroso de Almeida, T. (author), Zhang, W. (author), Stöckl, Markus (author), Ulber, Roland (author), Hollmann, F. (author), Holtmann, Dirk (author)Various enzymes utilize hydrogen peroxide as an oxidant. Such “peroxizymes” are potentially very attractive catalysts for a broad range of oxidation reactions. Most peroxizymes, however, are inactivated by an excess of H<sub>2</sub>O<sub>2</sub>. The electrochemical reduction of oxygen can be used as an in situ generation method for hydrogen...journal article 2019
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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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Vignali, Valentina (author), S. Miranda, Barbara (author), Lodoso-Torrecilla, Irene (author), Van Nisselroy, Cathelijn A.J. (author), Hoogenberg, Bas Jan (author), Dantuma, Sybren (author), Hollmann, F. (author), De Vries, Jan Willem (author)Engineered viruses are finding an increasing number of applications in basic, translational research and materials science. Genetic and chemical engineering of capsids represents a key point for tailoring the properties of viral particles, but the synthetic efforts and limits accompanying these processes still hinder their usability. Here, a...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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Höfler, G.T. (author), But, A. (author), Hollmann, F. (author)Haloperoxidases are very active catalysts for the in situ generation of electrophilic halide species for oxidative halogenation reactions. In the synthetic community, these catalysts, however, are not widely used. The aim of this mini-review is to critically summarise the current state-of-the-art of haloperoxidase catalysis for organic...journal article 2019
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Musa, Musa M. (author), Hollmann, F. (author), Mutti, Francesco G. (author)Deracemisation via chemo-enzymatic or multi-enzymatic approaches is the optimum substitute for kinetic resolution, which suffers from the limitation of a theoretical maximum 50% yield albeit high enantiomeric excess is attainable. This review covers the recent progress in various deracemisation approaches applied to the synthesis of...review 2019
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Leemans, Laura (author), Walter, Marc D. (author), Hollmann, F. (author), Schallmey, Anett (author), van Langen, L.M. (author)Enantiopure β-amino alcohols constitute one of the most significant building blocks for the synthesis of active pharmaceutical ingredients. Despite the availability of a range of chiral β-amino alcohols from a chiral pool, there is a growing demand for new enantioselective synthetic routes to vicinal amino alcohols and their derivatives. In...journal article 2019
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Choi, Da Som (author), Lee, Hojin (author), Tieves, F. (author), Lee, Yang Woo (author), Son, Eun Jin (author), Zhang, W. (author), Shin, Byungha (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases catalyze selective oxyfunctionalization of hydrocarbons with high conversion efficiencies using H<sub>2</sub>O<sub>2</sub> as a key cosubstrate. Here, we report an unbiased photoelectrochemical (PEC) tandem structure consisting of a FeOOH/BiVO<sub>4</sub> photoanode, a Cu(In,Ga)Se<sub>2</sub> solar absorber, and a graphitic...journal article 2019
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Ismail, M.B.M. (author), Schroeder, Lea (author), Frese, Marcel (author), Kottke, Tilman (author), Hollmann, F. (author), Paul, C.E. (author), Sewald, Norbert (author)Flavin-dependent halogenases are known to regioselectively introduce halide substituents into aromatic moieties, for example, the indole ring of tryptophan. The process requires halide salts and oxygen instead of molecular halogen in the chemical halogenation. However, the reduced cofactor flavin adenine dinucleotide (FADH<sub>2</sub>) has to...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