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Jang, Jinha (author), Aurangzeb Khan, Waseela (author), Hollmann, F. (author), Won, Keehoon (author), Park, Chan Beum (author)Lignin is the most abundant renewable and sustainable source of aromatic compounds to replace fossil resources, causing environmental issues. However, most lignin generated from pulping and biorefinery processes is combusted or discarded as waste. In this work, we first propose a photocatalytic artificial wood platform consisting of lignin and...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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Xu, X. (author)H2O2 is a relatively 'green' oxidant because its by-products are only H2O. In recent years, an increasing number of enzymatic synthesis methods based on H2O2 have been estab-lished. H2O2-driven reactions are usually applied as an alternative to NAD(P)H-dependent reactions to avoid complicated cofactor regeneration systems.<br/><br/>The aim of...doctoral thesis 2022
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Hilberath, T. (author), van Troost, A.G.L. (author), Alcalde, Miguel (author), Hollmann, F. (author)The use of water-miscible organic co-solvents in biocatalysis is a simple procedure for obtaining higher enzymatic activities toward hydrophobic substrates. However, effects on activity and stability have to be carefully evaluated, also with regard to the type and concentration of the respective co-solvent. In this contribution, we investigated...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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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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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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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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Yoon, Jaeho (author), Kim, Jinhyun (author), Tieves, F. (author), Zhang, W. (author), Alcalde, Miguel (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases have long inspired the selective oxyfunctionalization of various aliphatic and aromatic compounds, because of their broad substrate spectrum and simplicity of catalytic mechanism. This study provides a proof-of-concept of piezobiocatalysis by demonstrating peroxygenase-catalyzed oxyfunctionalization reactions fueled by...journal article 2020
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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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van Schie, M.M.C.H. (author), Zhang, W. (author), Tieves, F. (author), Choi, Da Som (author), Park, Chan Beum (author), Burek, Bastien O. (author), Bloh, Jonathan Z. (author), Arends, I.W.C.E. (author), Paul, C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H<sub>2</sub>O<sub>2</sub> can be addressed via in situ generation of H<sub>2</sub>O<sub>2<...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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Zhang, W. (author), Burek, Bastien O. (author), Fernandez Fueyo, E. (author), Alcalde, Miguel (author), Bloh, Jonathan Z. (author), Hollmann, F. (author)Selective oxyfunctionalizations of inert C−H bonds can be achieved under mild conditions by using peroxygenases. This approach, however, suffers from the poor robustness of these enzymes in the presence of hydrogen peroxide as the stoichiometric oxidant. Herein, we demonstrate that inorganic photocatalysts such as gold–titanium dioxide...journal article 2017
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Martínez, Angel T. (author), Ruiz-Dueñas, Francisco J. (author), Camarero, Susana (author), Serrano, Ana (author), Linde, Dolores (author), Lund, Henrik (author), Vind, Jesper (author), Tovborg, Morten (author), Herold-Majumdar, Owik M. (author), Hofrichter, Martin (author), Liers, Christiane (author), Ullrich, René (author), Scheibner, Katrin (author), Sannia, Giovanni (author), Piscitelli, Alessandra (author), Pezzella, Cinzia (author), Sener, Mehmet E. (author), Kılıç, Sibel (author), van Berkel, Willem J.H. (author), Guallar, Victor (author), Lucas, Maria Fátima (author), Zuhse, Ralf (author), Ludwig, Roland (author), Hollmann, F. (author), Fernandez Fueyo, E. (author), Record, Eric (author), Faulds, Craig B. (author), Tortajada, Marta (author), Winckelmann, Ib (author), Rasmussen, Jo Anne (author), Gelo-Pujic, Mirjana (author), Gutiérrez, Ana (author), del Río, José C. (author), Rencoret, Jorge (author), Alcalde, Miguel (author)Fungi produce heme-containing peroxidases and peroxygenases, flavin-containing oxidases and dehydrogenases, and different copper-containing oxidoreductases involved in the biodegradation of lignin and other recalcitrant compounds. Heme peroxidases comprise the classical ligninolytic peroxidases and the new dye-decolorizing peroxidases, while...review 2017
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Choi, Da Som (author), Ni, Y. (author), Fernandez Fueyo, E. (author), Lee, Minah (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases are very promising catalysts for oxyfunctionalization reactions. Their practical applicability, however, is hampered by their sensitivity against the oxidant (H<sub>2</sub>O<sub>2</sub>), therefore necessitating in situ generation of H<sub>2</sub>O<sub>2</sub>. Here, we report a photoelectrochemical approach to provide...journal article 2017
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Zhang, W. (author), Gacs, Jenő (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The aerobic organocatalytic oxidation of alcohols was achieved by using water-soluble sodium anthraquinone sulfonate. Under visible-light activation, this catalyst mediated the aerobic oxidation of alcohols to aldehydes and ketones. The photo-oxyfunctionalization of alkanes was also possible under these conditions.journal article 2017
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Holtmann, Dirk (author), Hollmann, F. (author)Monooxygenases are promising catalysts because they in principle enable the organic chemist to perform highly selective oxyfunctionalisation reactions that are otherwise difficult to achieve. For this, monooxygenases require reducing equivalents, to allow reductive activation of molecular oxygen at the enzymes' active sites. However, these...journal article 2016
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Fernandez Fueyo, E. (author), Ni, Y. (author), Gomez Baraibar, A. (author), Alcalde, Miguel (author), van Langen, L.M. (author), Hollmann, F. (author)The peroxygenase from Agrocybe aegerita (AaeUPO) has been evaluated for stereoselective oxyfunctionalization chemistry under non-aqueous reaction conditions. The stereoselective hydroxylation of ethylbenzene to (R)-1-phenylethanol was performed in neat substrate as reaction medium together with the immobilized biocatalyst and <sup>tert</sup...journal article 2016