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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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Chen, Shaohang (author), Zhang, Jiaan (author), Zeng, Zhigang (author), Dai, Zongjie (author), Wang, Qinhong (author), Wever, Ron (author), Hollmann, F. (author), Zhang, W. (author)A chemoenzymatic method for the synthesis of haloethers is presented. A combination of enzymatic hypohalite synthesis with spontaneous oxidation of alkenes and nucleophilic attack by various alcohols enabled the synthesis of a wide range of haloethers. The reaction system has been characterised and current imitations have been worked out. In...journal article 2022
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Naapuri, Janne M. (author), Wagner, Philip K. (author), Hollmann, F. (author), Deska, Jan (author)Vanadate-dependent chloroperoxidase from Curvularia inaequalis catalyzes 5-endo-trig bromocyclizations of α-allenols to produce valuable halofunctionalized furans as versatile synthetic building blocks. In contrast to other haloperoxidases, also the more challenging 5-exo-trig halocyclizations of γ-allenols succeed with this system even...journal article 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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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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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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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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Zippilli, C. (author), Bartolome, Miguel Jimenez (author), Hilberath, T. (author), Botta, Lorenzo (author), Hollmann, F. (author), Saladino, Raffaele (author)A photochemoenzymatic halodecarboxylation of ferulic acid was achieved using vanadate-dependent chloroperoxidase as (bio)catalyst and oxygen and organic solvent as sole stoichiometric reagents in a biphasic system. Performance and selectivity were improved through a phase transfer catalyst, reaching a turnover number of 660.000 for the enzyme...journal article 2022
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Hwang, Se Yeun (author), Song, Dayoon (author), Seo, Eun Ji (author), Hollmann, F. (author), You, Youngmin (author), Park, Jin Byung (author)Photobiocatalysis is a growing field of biocatalysis. Especially light-driven enzyme catalysis has contributed significantly to expanding the scope of synthetic organic chemistry. However, photoenzymes usually utilise a rather narrow wavelength range of visible (sun)light. Triplet–triplet annihilation-based upconversion (TTA-UC) of long...journal article 2022
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Ma, Yunjian (author), Liang, Hongjing (author), Zhao, Zexin (author), Wu, Bin (author), Lan, Dongming (author), Hollmann, F. (author), Wang, Yonghua (author)Unspecific peroxygenases (UPOs, EC 1.11.2.1) are promising oxyfunctionalization catalysts because of their unique stereoselectivity. However, so far only a few UPOs have been reported. In this study, gene mining was used to identify a gene from Galerina marginata that coded for a novel UPO (GmaUPO). GmaUPO was expressed in Pichia pastoris X...journal article 2022
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Domestici, C. (author), Wu, Y. (author), Hilberath, T. (author), Alcalde, Miguel (author), Hollmann, F. (author), Macchioni, Alceo (author)Unspecific peroxygenases (UPOs) are promising biocatalysts for oxyfunctionalisation reactions, owing to their simplicity of handling, stability and robustness. A limitation of using UPOs on a large scale is their deactivation in the presence of even rather modest concentrations of H<sub>2</sub>O<sub>2</sub>, requiring a constant and...journal article 2023
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Wu, Bin (author), Wang, S. (author), Ma, Yunjian (author), Yuan, Shuguang (author), Hollmann, F. (author), Wang, Yonghua (author)Alcohol oxidases (AOxs) catalyze the aerobic oxidation of alcohols to the corresponding carbonyl products (aldehydes or ketones), producing only H<sub>2</sub>O<sub>2</sub> as the byproduct. The majority of known AOxs, however, have a strong preference for small, primary alcohols, limiting their broad applicability, e.g., in the food industry....journal article 2023
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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