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Paul, C.E. (author), Hanefeld, U. (author), Hollmann, F. (author), Qu, Ge (author), Yuan, Bo (author), Sun, Zhoutong (author)Contemporary Biocatalysis heavily relies on enzyme engineering as natural enzymes frequently lack the requisite attributes for effective organic synthesis. The inherent limitations in stability, catalytic activity, and selectivity of wild-type enzymes often hinder their suitability for chemical synthesis. Over the past 25 years, there has...journal article 2024
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Wu, Y. (author), Paul, C.E. (author), Hilberath, T. (author), Jongkind, E.P.J. (author), Zhang, Wuyuan (author), Alcalde, Miguel (author), Hollmann, F. (author)Utilisation of fatty acids generally relies on pre-existing functional groups such as the carboxylate group or C=C-double bonds. Addition of new functionalities into the hydrocarbon part opens up new possibilities for fatty acid valorisation. In this contribution we demonstrate the synthetic potential of a peroxygenase mutant AaeUPO−Fett for...journal article 2023
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Xu, X. (author), van Hengst, J.M.A. (author), Mao, Yejia (author), Martinez, Mireia (author), Roda, Sergi (author), Floor, Martin (author), Guallar, Victor (author), Paul, C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)A peroxygenase-catalysed hydroxylation of organosilanes is reported. The recombinant peroxygenase from Agrocybe aegerita (AaeUPO) enabled efficient conversion of a broad range of silane starting materials in attractive productivities (up to 300 mM h<sup>−1</sup>), catalyst performance (up to 84 s<sup>−1</sup> and more than 120 000 catalytic...journal article 2023
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Wu, Y. (author), Paul, C.E. (author), Hollmann, F. (author)This review article critically compares two widely used types of catalysis, chemo- and biocatalysis, and provides insights on their greenness according to specified parameters. A comparative analysis of the environmental impact of chemo- and biocatalytic oxyfunctionalisation reactions based on published experimental data reveals that both...journal article 2023
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Reeve, Holly A. (author), Nicholson, Jake (author), Altaf, Farieha (author), Lonsdale, Thomas H. (author), Preissler, Janina (author), Lauterbach, Lars (author), Lenz, Oliver (author), Leimkühler, Silke (author), Hollmann, F. (author), Paul, C.E. (author), Vincent, Kylie A. (author)We demonstrate a recycling system for synthetic nicotinamide cofactor analogues using a soluble hydrogenase with turnover number of >1000 for reduction of the cofactor analogues by H2. Coupling this system to an ene reductase, we show quantitative conversion of N-ethylmaleimide to N-ethylsuccinimide. The biocatalyst system retained >50%...journal article 2022
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Hanefeld, U. (author), Hollmann, F. (author), Paul, C.E. (author)Biocatalysis has an enormous impact on chemical synthesis. The waves in which biocatalysis has developed, and in doing so changed our perception of what organic chemistry is, were reviewed 20 and 10 years ago. Here we review the consequences of these waves of development. Nowadays, hydrolases are widely used on an industrial scale for the...review 2022
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Xu, X. (author), Brasselet, H.L.Y. (author), Jongkind, E.P.J. (author), Alcalde, Miguel (author), Paul, C.E. (author), Hollmann, F. (author)In this study, we developed a new bienzymatic reaction to produce enantioenriched phenylethanols. In a first step, the recombinant, unspecific peroxygenase from Agrocybe aegerita (rAaeUPO) was used to oxidise ethylbenzene and its derivatives to the corresponding ketones (prochiral intermediates) followed by enantioselective reduction into the...journal article 2022
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Höfler, G.T. (author), Hollmann, F. (author), Paul, C.E. (author), Rauch, M.C.R. (author), van Schie, M.M.C.H. (author), Willot, S.J. (author)Cofactors assist enzymes to catalyze reactions and are indispensable and ubiquitous in nature, playing a central role in metabolic pathways. In biocatalysis, common redox cofactors such as nicotinamide, flavin and heme can be activated by light or synthetized to vary redox potentials, leading to different types of reactions for the formation...book chapter 2021
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Wu, Y. (author), Paul, C.E. (author), Hollmann, F. (author)The fatty acid photodecarboxylase from Chlorella variabilis NC64 A (CvFAP) catalyses the light-dependent decarboxylation of fatty acids. Photoinactivation of CvFAP still represents one of the major limitations of this interesting enzyme en route to practical application. In this study we demonstrate that the photostability of CvFAP can easily...journal article 2021
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Martinez Montero, L. (author), Tischler, Dirk (author), Süss, Philipp (author), Schallmey, Anett (author), Franssen, Maurice C.R. (author), Hollmann, F. (author), Paul, C.E. (author)Enantioenriched azido alcohols are precursors for valuable chiral aziridines and 1,2-amino alcohols, however their chiral substituted analogues are difficult to access. We established a cascade for the asymmetric azidohydroxylation of styrene derivatives leading to chiral substituted 1,2-azido alcohols via enzymatic asymmetric epoxidation,...journal article 2021
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Al-Shameri, Ammar (author), Willot, S.J. (author), Paul, C.E. (author), Hollmann, F. (author), Lauterbach, Lars (author)Correction for 'H2 as a fuel for flavin- and H2O2-dependent biocatalytic reactions' by Ammar Al-Shameri et al., Chem. Commun., 2020, DOI: 10.1039/d0cc03229h.journal article 2020
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Al-Shameri, Ammar (author), Willot, S.J. (author), Paul, C.E. (author), Hollmann, F. (author), Lauterbach, Lars (author)The soluble hydrogenase from Ralstonia eutropha provides an atom efficient regeneration system for reduced flavin cofactors using H2 as an electron source. We demonstrated this system for highly selective ene-reductase-catalyzed CC-double bond reductions and monooxygenase-catalyzed epoxidation. Reactions were expanded to aerobic conditions to...journal article 2020
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Hollmann, F. (author), Opperman, Diederik J. (author), Paul, C.E. (author)Reductions play a key role in organic synthesis, producing chiral products with new functionalities. Enzymes can catalyse such reactions with exquisite stereo-, regio- and chemoselectivity, leading the way to alternative shorter classical synthetic routes towards not only high-added-value compounds but also bulk chemicals. In this review we...review 2020
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Guarneri, A. (author), Westphal, Adrie H. (author), Leertouwer, C.J. (author), Lunsonga, Joy (author), Franssen, Maurice C.R. (author), Opperman, Diederik J. (author), Hollmann, F. (author), van Berkel, Willem J.H. (author), Paul, C.E. (author)Regioselective aromatic hydroxylation is desirable for the production of valuable compounds. External flavin-containing monooxygenases activate and selectively incorporate an oxygen atom in phenolic compounds through flavin reduction by the nicotinamide adenine dinucleotide coenzyme, and subsequent reaction with molecular oxygen. This study...journal article 2020
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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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Phonbuppha, Jittima (author), Tinikul, Ruchanok (author), Wongnate, Thanyaporn (author), Intasian, Pattarawan (author), Hollmann, F. (author), Paul, C.E. (author), Chaiyen, Pimchai (author)Bacterial luciferase (Lux) catalyzes a bioluminescence reaction by using long-chain aldehyde, reduced flavin and molecular oxygen as substrates. The reaction can be applied in reporter gene systems for biomolecular detection in both prokaryotic and eukaryotic organisms. Because reduced flavin is unstable under aerobic conditions, another...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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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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