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Yin, Xinjian (author), Gong, Wenzhong (author), Zeng, Yujing (author), Qiu, Hulin (author), Liu, Lan (author), Hollmann, F. (author), Chen, Bishuang (author)The biocatalytic oxidative deamination of β-amino alcohols holds significant practical potential in kinetic resolution and/or deracemization process to access (R)-β-amino alcohols. This study exemplifies a notable instance of acquisition and utilization of this valuable oxidative deamination activity. Initially, the mutation N261M (M0) was...journal article 2024
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Li, Huanhuan (author), Duan, Peigao (author), Huang, Yawen (author), Cui, Chengsen (author), Hollmann, F. (author), Ma, Yunjian (author), Wang, Yonghua (author), Zhang, Jie (author), Liu, Weidong (author), Zhang, Wuyuan (author)The downstream product transformation of lignin depolymerization is of great interest in the production of high-value aromatic chemicals. However, this transformation is often impeded by chemical oxidation under harsh reaction conditions. In this study, we demonstrate that hypohalites generated in situ by the vanadium-containing...journal article 2024
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Heckmann, C.M. (author), Bürgler, Moritz (author), Paul, C.E. (author)The unmatched chemo-, regio-, and stereoselectivity of enzymes renders them powerful catalysts in the synthesis of chiral active pharmaceutical ingredients (APIs). Inspired by the discovery route toward the LPA<sub>1</sub>-antagonist BMS-986278, access to the API building block (1S,3R)-3-hydroxycyclohexanecarbonitrile was envisaged using an...journal article 2024
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França, Alexandre S. (author), Brêda, Gabriela C. (author), De Oliveira, Kleber T. (author), Almeida, Rodrigo V. (author), Hollmann, F. (author), de Souza, Rodrigo O.M.A. (author)A visible-light-driven photocatalytic decarboxylation of palmitic acid and related fatty acids is described in this study. Remarkable decarboxylation rates have been observed with full conversion in less than 20 min. In this study, we have<br/>demonstrated that sunlight irradiation, even on cloudy days, can deliver similar results to traditional...journal article 2023
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Nieto, Susana (author), Bernal, Juana M. (author), Villa Aroca, R. (author), Garcia-Verdugo, Eduardo (author), Donaire, Antonio (author), Lozano, Pedro (author)A sustainable scaling-up process for the biocatalytic production of new bioactive provitamin-B<sub>5</sub> monoacyl esters has been demonstrated. A solvent-free reaction protocol, based on the formation of eutectic mixtures between neat substrates, renders highly efficient direct esterification of free fatty acids (i.e., from C<sub>6</sub> to...journal article 2023
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Heckmann, C.M. (author), Paul, C.E. (author)Chiral N-heterocycles are a common motif in many active pharmaceutical ingredients; however, their synthesis often relies on the use of heavy metals. In recent years, several biocatalytic approaches have emerged to reach enantiopurity. Here, we describe the asymmetric synthesis of 2-substituted pyrrolidines and piperidines, starting from...journal article 2023
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Alphand, Véronique (author), van Berkel, Willem J.H. (author), Jurkaš, Valentina (author), Kara, Selin (author), Kourist, Robert (author), Kroutil, Wolfgang (author), Mascia, Francesco (author), Nowaczyk, Marc M. (author), Paul, C.E. (author)The recent increase of interest in photocatalysis spread to biocatalysis and triggered a rush for the development of light-dependent enzyme-mediated or enzyme-coupled processes. After several years of intense research on photobiocatalysis, it is time to evaluate the state of the field in a structured manner. In this Perspective, we suggest to...journal article 2023
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Burek, Bastien O. (author), Dawood, A.W.H. (author), Hollmann, F. (author), Liese, Andreas (author), Holtmann, Dirk (author)Enzyme catalysis, made tremendous progress over the last years in identification of new enzymes and new enzymatic reactivity’s as well as optimization of existing enzymes. However, the performance of the resulting processes is often still limited, e.g., in regard of productivity, realized product concentrations and the stability of the enzymes....journal article 2022
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Silva de Miranda, Amanda (author), Milagre, C.D.D.F. (author), Hollmann, F. (author)Alcohol dehydrogenases (ADHs) have become important catalysts for stereoselective oxidation and reduction reactions of alcohols, aldehydes and ketones. The aim of this contribution is to provide the reader with a timely update on the state-of-the-art of ADH-catalysis. Mechanistic basics are presented together with practical information about the...journal article 2022
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Hagedoorn, P.L. (author)Isothermal titration calorimetry (ITC) is a popular chemical analysis technique that can be used to measure macromolecular interactions and chemical and physical processes. ITC involves the measurement of heat flow to and from a measurement cell after each injection during a titration experiment. ITC has been useful to measure the thermodynamics...journal article 2022
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Puchľová, Eva (author), Hilberath, T. (author), Vranková, Kvetoslava (author), Hollmann, F. (author)Non-enantioselective alcohol dehydrogenases (ADHs) are rarely found in the biocatalysis portfolio. Generally, highly enantioselective ADHs are sought for. Using such ADHs for the oxidation of racemic alcohols generally results in a kinetic resolution of the starting material, which is unfavourable if the ketone represents the product of interest...journal article 2022
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Ribeaucourt, David (author), Höfler, G.T. (author), Yemloul, Mehdi (author), Bissaro, Bastien (author), Lambert, Fanny (author), Berrin, Jean Guy (author), Lafond, Mickael (author), Paul, C.E. (author)Biocatalytic pathways for the synthesis of (-)-menthol, the most sold flavor worldwide, are highly sought-after. To access the key intermediate (R)-citronellal used in current major industrial production routes, we established a one-pot bienzymatic cascade from inexpensive geraniol, overcoming the problematic biocatalytic reduction of the...journal article 2022
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Li, Huanhuan (author), Younes, S.H.H. (author), Chen, Shaohang (author), Duan, Peigao (author), Cui, Chengsen (author), Wever, Ron (author), Zhang, Wuyuan (author), Hollmann, F. (author)In this contribution, we report chemoenzymatic bromodecarboxylation (Hunsdiecker-type) of α,ß-unsaturated carboxylic acids. The extraordinarily robust chloroperoxidase from Curvularia inaequalis (CiVCPO) generated hypobromite from H2O2 and bromide, which then spontaneously reacted with a broad range of unsaturated carboxylic acids and yielded...journal article 2022
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Kim, Jinhyun (author), Um, Yunna (author), Han, Seunghyun (author), Hilberath, T. (author), Kim, Yong Hwan (author), Hollmann, F. (author), Park, Chan Beum (author)The pulp and paper manufacturers generate approximately 50 million metric tons of lignin per annum, most of which has been abandoned or incinerated because of lignin's recalcitrant nature. Here, we report bias-free photoelectrochemical (PEC) oxidation of lignin coupled with asymmetric hydrogenation of C=C bonds. The PEC platform consists of a...journal article 2022
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Voss, Moritz (author), Hüppi, S.N. (author), Schaub, Daniela (author), Hayashi, Takahiro (author), Ligibel, Mathieu (author), Sager, Emine (author), Schroer, Kirsten (author), Snajdrova, Radka (author), Buller, Rebecca (author)Enzymatic late-stage diversification of small molecules has the potential to rapidly generate diversity in compound libraries dedicated to drug discovery. In this context, freestanding Fe(II)/α-ketoglutarate-dependent halogenases have raised particular interest as this enzyme family allows the otherwise difficult regio- and stereoselective...journal article 2022
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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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Chatzipanagiotou, Konstantina Roxani (author), Soekhoe, Virangni (author), Jourdin, L. (author), Buisman, Cees J.N. (author), Bitter, J. Harry (author), Strik, David P.B.T.B. (author)Electrocatalytic metals and microorganisms can be combined for CO2 conversion in microbial electrosynthesis (MES). However, a systematic investigation on the nature of interactions between metals and MES is still lacking. To investigate this nature, we integrated a copper electrocatalyst, converting CO2 to formate, with microorganisms,...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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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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Joseph Srinivasan, Shiny (author), Cleary, Sarah E. (author), Ramirez, Miguel A. (author), Reeve, Holly A. (author), Paul, C.E. (author), Vincent, Kylie A. (author)A new activity for the [NiFe] uptake hydrogenase 1 of Escherichia coli (Hyd1) is presented. Direct reduction of biological flavin cofactors FMN and FAD is achieved using H<sub>2</sub> as a simple, completely atom-economical reductant. The robust nature of Hyd1 is exploited for flavin reduction across a broad range of temperatures (25–70 °C)...journal article 2021