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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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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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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
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Paul, C.E. (author), Eggerichs, Daniel (author), Westphal, Adrie H. (author), Tischler, Dirk (author), van Berkel, Willem J.H. (author)Flavoprotein monooxygenases (FPMOs) are single- or two-component enzymes that catalyze a diverse set of chemo-, regio- and enantioselective oxyfunctionalization reactions. In this review, we describe how FPMOs have evolved from model enzymes in mechanistic flavoprotein research to biotechnologically relevant catalysts that can be applied for...review 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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Sheldon, R.A. (author)The role of bio- and chemo-catalytic aerobic oxidations in the production of commodity chemicals in a bio-refinery is reviewed. The situation is fundamentally different to that in a petrochemicals refinery where the feedstocks are gaseous or liquid hydrocarbons that are oxidized at elevated temperatures in the vapor or liquid phase under...review 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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Tischler, Dirk (author), Gädke, Eric (author), Eggerichs, Daniel (author), Gomez Baraibar, Alvaro (author), Mügge, Carolin (author), Scholtissek, Anika (author), Paul, C.E. (author)Ene-reductases allow regio- and stereoselective reduction of activated C=C double bonds at the expense of nicotinamide adenine dinucleotide cofactors [NAD(P)H]. Biological NAD(P)H can be replaced by synthetic mimics to facilitate enzyme screening and process optimization. The ene-reductase FOYE-1, originating from an acidophilic iron oxidizer...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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Choi, Da Som (author), Lee, Hojin (author), Tieves, F. (author), Lee, Yang Woo (author), Son, Eun Jin (author), Zhang, W. (author), Shin, Byungha (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases catalyze selective oxyfunctionalization of hydrocarbons with high conversion efficiencies using H<sub>2</sub>O<sub>2</sub> as a key cosubstrate. Here, we report an unbiased photoelectrochemical (PEC) tandem structure consisting of a FeOOH/BiVO<sub>4</sub> photoanode, a Cu(In,Ga)Se<sub>2</sub> solar absorber, and a graphitic...journal article 2019
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Pedroso de Almeida, T. (author), van Schie, M.M.C.H. (author), Ma, A. (author), Tieves, F. (author), Younes, S.H.H. (author), Fernandez Fueyo, E. (author), Arends, I.W.C.E. (author), Riul, A. (author), Hollmann, F. (author)The selective oxidation of trans-2-hexen-1-ol to the corresponding aldehyde using a recombinant aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) is reported. Especially using the two liquid phase system to overcome solubility and product inhibition issues enabled to achieve more than 2.200.000 catalytic turnovers for the production enzyme...journal article 2019
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Younes, S.H.H. (author), Tieves, F. (author), Lan, Dongming (author), Wang, Yonghua (author), Süss, Philipp (author), Brundiek, Henrike (author), Wever, Ron (author), Hollmann, F. (author)A chemoenzymatic method for the halocyclization of unsaturated alcohols and acids by using the robust V-dependent chloroperoxidase from Curvularia inaequalis (CiVCPO) as catalyst has been developed for the in situ generation of hypohalites. A broad range of halolactones and cyclic haloethers are formed with excellent performance of the...journal article 2019
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Tieves, F. (author), Willot, S.J. (author), van Schie, M.M.C.H. (author), Rauch, M.C.R. (author), Younes, S.H.H. (author), Zhang, W. (author), Dong, J. (author), Gomez de Santos, P. (author), Hollmann, F. (author)An increasing number of biocatalytic oxidation reactions rely on H <sub>2</sub> O <sub>2</sub> as a clean oxidant. The poor robustness of most enzymes towards H <sub>2</sub> O <sub>2</sub> , however, necessitates more efficient systems for in situ H <sub>2</sub> O <sub>2</sub> generation. In analogy to the well-known formate dehydrogenase to...journal article 2019