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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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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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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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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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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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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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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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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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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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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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Ma, Yunjian (author), Zhang, Xizhen (author), Zhang, W. (author), Li, Peilin (author), Li, Yongru (author), Hollmann, F. (author), Wang, Yonghua (author)A photobiocatalytic cascade transforming natural triglycerides into alkanes/alkenes is proposed. Starting from natural triglycerides, free fatty acids have been obtained using lipases. The free fatty acids were then, in a photoenzymatic step, decarboxylated into the C1-shortened alkanes using a recently described photodecarboxylase from...journal article 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)The use of a microscale atmospheric pressure plasma jet (μAPPJ) was investigated for its potential to supply hydrogen peroxide in biocatalysis. Compared to a previously employed dielectric barrier discharge (DBD), the μAPPJ offered significantly higher H<sub>2</sub>O<sub>2</sub> production rates and better handling of larger reaction volumes....journal article 2020
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Bormann, Sebastian (author), van Schie, M.M.C.H. (author), Pedroso de Almeida, T. (author), Zhang, W. (author), Stöckl, Markus (author), Ulber, Roland (author), Hollmann, F. (author), Holtmann, Dirk (author)Various enzymes utilize hydrogen peroxide as an oxidant. Such “peroxizymes” are potentially very attractive catalysts for a broad range of oxidation reactions. Most peroxizymes, however, are inactivated by an excess of H<sub>2</sub>O<sub>2</sub>. The electrochemical reduction of oxygen can be used as an in situ generation method for hydrogen...journal article 2019
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Willot, S.J. (author), Fernandez Fueyo, E. (author), Tieves, F. (author), Pesic, M. (author), Alcalde, Miguel (author), Arends, I.W.C.E. (author), Park, Chan Beum (author), Hollmann, F. (author)Peroxygenases require a controlled supply of H<sub>2</sub>O<sub>2</sub> to operate efficiently. Here, we propose a photocatalytic system for the reductive activation of ambient O<sub>2</sub> to produce H<sub>2</sub>O<sub>2</sub> which uses the energy provided by visible light more efficiently based on the combination of wavelength...journal article 2019
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