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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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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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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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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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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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Mahor, Durga (author), Cong, Zhiqi (author), Weissenborn, Martin J. (author), Hollmann, F. (author), Zhang, Wuyuan (author)The oxidation of alkanes into valuable chemical products is a vital reaction in organic synthesis. This reaction, however, is challenging, owing to the inertness of C−H bonds. Transition metal catalysts for C−H functionalization are frequently explored. Despite chemical alternatives, nature has also evolved powerful oxidative enzymes (e. g.,...review 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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Song, Ji Won (author), Baeg, Yoonjin (author), Jeong, Ha Yeon (author), Lee, Jinwon (author), Oh, Deok Kun (author), Hollmann, F. (author), Park, Jin Byung (author)Bacterial outer membrane vesicles (OMVs) are small unilamellar proteoliposomes, involved in various functions including cell-to-cell signalling and protein excretion. We have engineered the OMVs of Escherichia coli to nano-scaled bioreactors for the biotransformation of fatty acids by targeting a fatty acid double bond hydratase of...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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Hagedoorn, P.L. (author), Hollmann, F. (author), Hanefeld, U. (author)Oleate hydratase catalyses the addition of water to the CC double bond of oleic acid to produce (R)-10-hydroxystearic acid. The enzyme requires an FAD cofactor that functions to optimise the active site structure. A wide range of unsaturated fatty acids can be hydrated at the C10 and in some cases the C13 position. The substrate scope can be...review 2021
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van Gelder, P.H.A.J.M. (author), Taebi, B. (author), van Ommen, J.R. (author), van de Poel, I.R. (author), Asveld, L. (author), Balkenende, R. (author), Hollmann, F. (author), van Kampen, E. (author), Krebbers, R.J. (author), de Lange, J. (author), Terwel, K.C. (author), Visser, Eelco (author)In this paper, we provide an overview of how Safe-by-Design is conceived and applied in practice in a large number of engineering disciplines. We discuss the differences, commonalities, and possibilities for mutual learning found in those practices and identify several ways of putting those disciplinary outlooks in perspective. The considered...journal article 2021
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Nintzel, Friederike E.H. (author), Wu, Y. (author), Planchestainer, Matteo (author), Held, Martin (author), Alcalde, Miguel (author), Hollmann, F. (author)Oxyfunctionalisation reactions in neat substrate still pose a challenge for biocatalysis. Here, we report an alginate-confined peroxygenase-CLEA to catalyse the enantioselective epoxidation of cis-β-methylstyrene in a solvent-free reaction system achieving turnover numbers of 96 000 for the biocatalyst and epoxide concentrations of 48 mM.journal article 2021
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Santner, Paul (author), Szabó, László Krisztián (author), Chanquia, Santiago Nahuel (author), Merrild, Aske Høj (author), Hollmann, F. (author), Kara, S. (author), Eser, Bekir Engin (author)Fatty acid photodecarboxylase (FAP) is one of the few photoenzymes in nature. The ability of FAP to convert fatty acids into alka(e)nes without the need for reducing equivalents put this enzyme into spotlight for biocatalytic applications. Although it has been discovered only a few years ago, many studies already emerged demonstrating its...journal article 2021
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Luan, Pengqian (author), Liu, Yunting (author), Li, Yongxing (author), Chen, Ran (author), Huang, Chen (author), Gao, Jing (author), Hollmann, F. (author), Jiang, Yanjun (author)An aqueous chemoenzymatic cascade reaction combining Pd-catalyzed C-C formation and enzymatic C=C asymmetric hydrogenation (AH) was developed for enantioselective synthesis of tertiary α-aryl cycloketones in good yields and excellent enantioselectivities. The stereopreference of the enzyme in AH of α-aryl cyclohexenones was studied. An...journal article 2021
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Amoroso, Rosa (author), Hollmann, F. (author), Maccallini, Cristina (author)DES are mixtures of two or more compounds, able to form liquids upon mixing, with lower freezing points when compared to the individual constituents (eutectic mixtures). This attitude is due to the specific hydrogen-bond interactions network between the components of the mixture. A notable characteristic of DES is the possibility to develop...review 2021
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Calderini, Elia (author), Süss, Philipp (author), Hollmann, F. (author), Wardenga, Rainer (author), Schallmey, Anett (author)Multi-step cascade reactions have gained increasing attention in the biocatalysis field in recent years. In particular, multi-enzymatic cascades can achieve high molecular complexity without workup of reaction intermediates thanks to the enzymes’ intrinsic selectivity; and where enzymes fall short, organo-or metal catalysts can further expand...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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Lin, Richen (author), Deng, Chen (author), Zhang, Wuyuan (author), Hollmann, F. (author), Murphy, Jerry D. (author)Bioelectrochemical technologies such as electro-fermentation and microbial CO<sub>2</sub> electrosynthesis are emerging interdisciplinary technologies that can produce renewable fuels and chemicals (such as carboxylic acids). The benefits of electrically driven bioprocesses include improved production rate, selectivity, and carbon conversion...review 2021
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Hobisch, Markus (author), Holtmann, Dirk (author), Gomez de Santos, Patricia (author), Alcalde, Miguel (author), Hollmann, F. (author), Kara, Selin (author)Peroxygenases are an emerging new class of enzymes allowing selective oxyfunctionalisation reactions in a cofactor-independent way different from well-known P450 monooxygenases. Herein, we focused on recent developments from organic synthesis, molecular biotechnology and reaction engineering viewpoints that are devoted to bring these enzymes...review 2021
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Erol, Özlem (author), Hollmann, F. (author)Following ionic liquids, (natural) deep eutectic solvents ((NA)DES) are receiving significant attention as performance additives for biocatalytic reactions. (NA)DES are increasingly evaluated as solvents to replace water in hydrolase-catalyzed esterification reactions thereby shifting the reaction equilibrium. They also frequently outperform...book chapter 2021