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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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Evolved Peroxygenase-Aryl Alcohol Oxidase Fusions for Self-Sufficient Oxyfunctionalization ReactionsGomez De Santos, Patricia (author), Lazaro, Sofia (author), Viña-Gonzalez, Javier (author), Hoang, Manh Dat (author), Sánchez-Moreno, Israel (author), Glieder, Anton (author), Hollmann, F. (author), Alcalde, Miguel (author)Fungal peroxygenases are deemed emergent biocatalysts for selective C-H bond oxyfunctionalization reactions. In this study, we have engineered a functional and stable self-sufficient chimeric peroxygenase-oxidase fusion. The bifunctional biocatalyst carried a laboratory-evolved version of the fungal peroxygenase fused to an evolved fungal...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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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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Wever, Ron (author), Renirie, R. (author), Hollmann, F. (author)In this chapter the catalytic and structural properties of the vanadium chloroperoxidases will be discussed with an emphasis on their superb activity and stability under operational conditions. These properties make these enzymes attractive catalysts in organic synthesis and allow a number of applications. Some of the more recent findings are...book chapter 2020
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Zhang, W. (author), Liu, H. (author), van Schie, M.M.C.H. (author), Hagedoorn, P.L. (author), Alcalde, Miguel (author), Denkova, A.G. (author), Djanashvili, K. (author), Hollmann, F. (author)It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenases utilize H2O2 as an oxidant to promote highly selective...journal article 2020
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Acevedo-Rocha, Carlos G. (author), Hollmann, F. (author), Sanchis, Joaquin (author), Sun, Zhoutong (author)In this invited Account, we highlight the enormous scientific breadth of our mentor Professor Manfred T. Reetz. It stretches from the development of organometallic reagents and transition metal catalysts to the adventurous idea of directed evolution of chemo-, stereo-, and regioselective enzymes, which he considered to be most important. We...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
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Ma, Yunjian (author), Zhang, Xizhen (author), Li, Yongru (author), Li, Peilin (author), Hollmann, F. (author), Wang, Yonghua (author)A biocatalytic cascade transforming castor oil into (R,Z)-octadec-9-en-7-ol is presented by combining a lipase catalysed hydrolysis of castor oil into ricinoleic acid followed by a photoenzymatic decarboxylation into (R,Z)-octadec-9-en-7-ol. Conversion of up to 41.7% and overall product concentrations of up to 60 mM, this new bienzymatic and...journal article 2020