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Martin-Diaz, Javier (author), Molina-Espeja, Patricia (author), Hofrichter, Martin (author), Hollmann, F. (author), Alcalde, Miguel (author)Fungal unspecific peroxygenases (UPOs) are efficient biocatalysts that insert oxygen atoms into nonactivated C–H bonds with high selectivity. Many oxyfunctionalization reactions catalyzed by UPOs are favored in organic solvents, a milieu in which their enzymatic activity is drastically reduced. Using as departure point the UPO secretion...journal article 2021
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Duong, Hong T. (author), Wu, Y. (author), Sutor, Alexander (author), Burek, Bastien O. (author), Hollmann, F. (author), Bloh, Jonathan Z. (author)Light-driven biocatalytic processes are notoriously hampered by poor penetration of light into the turbid reaction media. In this study, wirelessly powered light-emitting diodes are found to represent an efficient and scalable approach for process intensification of the photobiosynthetic production of diesel alkanes from renewable fatty acids...journal article 2021
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Biocatalytic Aromaticity-Breaking Epoxidation of Naphthalene and Nucleophilic Ring-Opening ReactionsZhang, W. (author), Li, Huanhuan (author), Younes, S.H.H. (author), Gómez De Santos, Patricia (author), Tieves, F. (author), Grogan, Gideon (author), Pabst, Martin (author), Alcalde, Miguel (author), Whitwood, Adrian C. (author), Hollmann, F. (author)Aromatic hydroxylation reactions catalyzed by heme-thiolate enzymes proceed via an epoxide intermediate. These aromatic epoxides could be valuable building blocks for organic synthesis giving access to a range of chiral trans-disubstituted cyclohexadiene synthons. Here, we show that naphthalene epoxides generated by fungal peroxygenases can...journal article 2021
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Holtmann, Dirk (author), Hollmann, F. (author)Process intensification aims at enabling bridging the gap between fundamental research such as identification of new catalysts and reactions and their implementation in industrial environments. Especially the field of biocatalysis has seen some tremendous improvements and the development of new tools and approaches to bridge this gap. In this...journal article 2021
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Carballares, Diego (author), Morellon-Sterling, Roberto (author), Xu, X. (author), Hollmann, F. (author), Fernandez-Lafuente, Roberto (author)This paper outlines the immobilization of the recombinant dimeric unspecific peroxygenase from Agrocybe aegerita (rAaeUPO). The enzyme was quite stable (remaining unaltered its activity after 35 h at 47<sup>◦</sup>C and pH 7.0). Phosphate destabilized the enzyme, while glycerol stabilized it. The enzyme was not immobilized on glyoxyl-agarose...journal article 2021
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Tonin, F. (author), Tieves, F. (author), Willot, S.J. (author), Van Troost, Anouska (author), van Oosten, R.J.C. (author), Breestraat, Stefaan (author), Van Pelt, Sander (author), Alcalde, Miguel (author), Hollmann, F. (author)The pilot-scale production of the peroxygenase from Agrocybe aegerita (rAaeUPO) is demonstrated. In a fed-batch fermentation of the recombinant Pichia pastoris, the enzyme was secreted into the culture medium to a final concentration of 0.29 g L-1 corresponding to 735 g of the peroxygenase in 2500 L of the fermentation broth after 6 days. Due...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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Hobisch, Markus (author), van Schie, M.M.C.H. (author), Kim, Jinhyun (author), Røjkjær Andersen, Kasper (author), Alcalde, Miguel (author), Kourist, Robert (author), Park, Chan Beum (author), Hollmann, F. (author), Kara, S. (author)The use of neat reaction media, that is the avoidance of additional solvents, is the simplest and the most efficient approach to follow in biocatalysis. Here, we show that unspecific peroxygenase from Agrocybe aegerita (AaeUPO) can hydroxylate the neat model substrate cyclohexane. H<sub>2</sub>O<sub>2</sub> was photocatalytically generated in...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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Yayci, Abdulkadir (author), Dirks, Tim (author), Kogelheide, Friederike (author), Alcalde, Miguel (author), Hollmann, F. (author), Awakowicz, Peter (author), Bandow, Julia E. (author)In plasma-driven biocatalysis, enzymes are employed to carry out reactions using species generated by non-thermal plasmas as the precursors. We have previously demonstrated that this is feasible in principle, but that the approach suffers from the short lifetime of the biocatalyst under operating conditions. In this work, protection...journal article 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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Li, Yongru (author), Ma, Yunjian (author), Li, Peilin (author), Zhang, Xizhen (author), Ribitsch, Doris (author), Alcalde, Miguel (author), Hollmann, F. (author), Wang, Yonghua (author)A bienzymatic cascade for selective sulfoxidation is presented. The evolved recombinant peroxygenase from Agrocybe aegeritra catalyses the enantioselective sulfoxidation of thioanisole whereas the choline oxidase from Arthrobacter nicotianae provides the H2 O2 necessary via reductive activation of ambient oxygen. The reactions are performed...journal article 2020
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Cha, Hee Jeong (author), Hwang, Se Yeun (author), Lee, Da Som (author), Kumar, Akula Ravi (author), Kwon, Yong Uk (author), Voß, Moritz (author), Schuiten, Eva (author), Bornscheuer, Uwe T. (author), Hollmann, F. (author)Long-chain aliphatic amines such as (S,Z)-heptadec-9-en-7-amine and 9-aminoheptadecane were synthesized from ricinoleic acid and oleic acid, respectively, by whole-cell cascade reactions using the combination of an alcohol dehydrogenase (ADH) from Micrococcus luteus, an engineered amine transaminase from Vibrio fluvialis (Vf-ATA), and a...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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Xu, X. (author), But, A. (author), Wever, Ron (author), Hollmann, F. (author)The chemoenzymatic oxidative decarboxylation of glutamic acid to the corresponding nitrile using the vanadium chloroperoxidase from Curvularia inaequalis (CiVCPO) as HOBr generation catalysts has been investigated. Product inhibition was identified as major limitation. Nevertheless, 1630000 turnovers and k<sub>cat</sub> of 75 s<sup>−1</sup>...journal article 2020
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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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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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Choi, Da Som (author), Kim, Jinhyun (author), Hollmann, F. (author), Park, Chan Beum (author)Inspired by natural photosynthesis, biocatalytic photoelectrochemical (PEC) platforms are gaining prominence for the conversion of solar energy into useful chemicals by combining redox biocatalysis and photoelectrocatalysis. Herein, we report a dual biocatalytic PEC platform consisting of a molybdenum (Mo)-doped BiVO<sub>4</sub> (Mo:BiVO<sub...journal article 2020