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Hüppi, S.N. (author)Our ability to tailor enzymatic properties is a critical factor for biocatalyst application in the industrial sector. Although many wild-type enzymes have been found capable of promiscuously catalysing desired anthropogenic reactions, their activity and selectivity for non-natural transformations is often poor. Consequently, it is crucial to...doctoral thesis 2024
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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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Ingram, A.A. (author), Oike, K. (author)Astonishing progress has been achieved in unlocking new-to-nature biocatalysis in the past decades. The progress in protein engineering enabled research to efficiently incorporate artificial structural elements into enzyme design. Recent trends include cofactor mimetics, artificial metalloenzymes and non-canonical amino acids. In this...journal article 2024
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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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Kim, Chang Hyun (author), Kim, Jinhyun (author), Hollmann, F. (author), Park, Chan Beum (author)Solar-driven N<sub>2</sub> fixation offers a green alternative to the highly energy-intensive Haber-Bosch process that releases more than 300 million metric tons of CO<sub>2</sub> annually to form NH<sub>3</sub>. However, N<sub>2</sub>-reducing photoelectrochemical (PEC) studies have not elucidated how an oxidation reaction affects the N<sub...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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Xu, X. (author), Hilberath, T. (author), Hollmann, F. (author)Heme-dependent oxygenases (i.e. P450 monooxygenases and peroxygenases) are highly selective catalysts for the selective oxyfunctionalisation or organic compounds. Both enzyme classes exhibit mechanistic similarities (i.e. using so-called compound I (CpdI) as active oxidation species) and differences in how CpdI is formed. From the differences...review 2023
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Li, Huanhuan (author), Shen, Qianqian (author), Zhou, Xiaoying (author), Duan, Peigao (author), Hollmann, F. (author), Huang, Yawen (author), Zhang, Wuyuan (author)Chiral sulfoxides are valuable building blocks in asymmetric synthesis. However, the biocatalytic synthesis of chiral sulfoxides is still challenged by low product titres. Herein, we report the use of peroxygenase as a catalyst for asymmetric sulfoxidation under non-aqueous conditions. Upon covalent immobilisation, the peroxygenase showed...journal article 2023
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Schober, Lukas (author), Tonin, F. (author), Hanefeld, U. (author), Gröger, Harald (author)A sequential-type as well as a tandem-type chemoenzymatic flow cascade combining an organocatalytic aldol reaction and a biocatalytic reduction to form stereoselectively a 1,3-diol with two stereogenic centers were developed. Initially, a comprehensive screening of 24 alcohol dehydrogenases was carried out and the identified candidates were...journal article 2022
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Benincá, Luiza A.D. (author), França, Alexandre S. (author), Brêda, Gabriela C. (author), Leão, Raquel A.C. (author), Almeida, Rodrigo V. (author), Hollmann, F. (author), de Souza, Rodrigo O.M.A. (author)The fatty acid photodecarboxylase from Chlorella variabilis NC64A (CvFAP) promotes the elimination of CO<sub>2</sub> from fatty acids (C<sub>n</sub>) producing the corresponding hydrocarbon (<sub>Cn-1</sub>). Therefore, this enzyme is of great biotechnological interest since it can be used in alternative biofuel production routes matching the...journal article 2022
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Synthesis of Chiral Amines via a Bi-Enzymatic Cascade Using an Ene-Reductase and Amine DehydrogenaseJongkind, E.P.J. (author), Fossey-Jouenne, Aurélie (author), Mayol, Ombeline (author), Zaparucha, Anne (author), Vergne-Vaxelaire, Carine (author), Paul, C.E. (author)Access to chiral amines with more than one stereocentre remains challenging, although an increasing number of methods are emerging. Here we developed a proof-of-concept bi-enzymatic cascade, consisting of an ene reductase and amine dehydrogenase (AmDH), to afford chiral diastereomerically enriched amines in one pot. The asymmetric reduction...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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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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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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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
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Mestrom, L. (author)Enzymes are nature’s catalyst of choice for the highly selective and efficient coupling of carbohydrates. Enzymatic sugar coupling is a competitive technology for industrial glycosylation reactions, since chemical synthetic routes require extensive use of laborious protection group manipulations and often lack regio- and stereoselectivity.doctoral thesis 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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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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Tonin, F. (author), Marti, E. (author), Arends, I.W.C.E. (author), Hanefeld, U. (author)The specific oxidation of 12α-OH group of hydroxysteroids is required for the preparation of cheno-and ursodeoxycholic acid (CDCA and UDCA, respectively). The C<sub>12</sub> oxidation of hydroxysteroids into their 12-oxo derivatives can selectively be performed by employing 12α-hydroxysteroid dehydrogenases. These enzymes use NAD(P)<sup>+<...journal article 2020