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Ebrecht, Ana C. (author), Mofokeng, Thato M. (author), Hollmann, F. (author), Smit, Martha S. (author), Opperman, Diederik J. (author)γ- and δ-lactones are valuable flavor and fragrance compounds. Their synthesis depends on the availability of suitable hydroxy fatty acid precursors. Three short unspecific peroxygenases were identified that selectively hydroxylate the C4 and C5 positions of C8-C12 fatty acids to yield after lactonization the corresponding γ- and δ-lactones....journal article 2023
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De Santos, Patricia Gomez (author), Mateljak, Ivan (author), Hoang, Manh Dat (author), Fleishman, Sarel J. (author), Hollmann, F. (author), Alcalde, Miguel (author)The generation of enantiodivergent biocatalysts for C-H oxyfunctionalizations is ever more important in modern synthetic chemistry. Here, we have applied the FuncLib algorithm based on phylogenetic and Rosetta calculations to design a diverse repertoire of active, stable, and enantiodivergent fungal peroxygenases. 24 designs, each carrying 4...journal article 2023
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Gomez de Santos, Patricia (author), González-Benjumea, Alejandro (author), Fernandez-Garcia, Angela (author), Aranda, Carmen (author), Wu, Y. (author), But, A. (author), Molina-Espeja, Patricia (author), Zhang, W. (author), Hollmann, F. (author)The hydroxylation of fatty acids is an appealing reaction in synthetic chemistry, although the lack of selective catalysts hampers its industrial implementation. In this study, we have engineered a highly regioselective fungal peroxygenase for the ω-1 hydroxylation of fatty acids with quenched stepwise over-oxidation. One single mutation near...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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- Hollmann, F. (author), Woodley, John M. (author) contribution to periodical 2023
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Dirks, Tim (author), Yayci, Abdulkadir (author), Klopsch, Sabrina (author), Krewing, Marco (author), Zhang, Wuyuan (author), Hollmann, F. (author), Bandow, Julia E. (author)Non-thermal plasmas are used in various applications to inactivate biological agents or biomolecules. A complex cocktail of reactive species, (vacuum) UV radiation and in some cases exposure to an electric field together cause the detrimental effects. In contrast to this disruptive property of technical plasmas, we have shown previously that...journal article 2023
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Domestici, C. (author), Wu, Y. (author), Hilberath, T. (author), Alcalde, Miguel (author), Hollmann, F. (author), Macchioni, Alceo (author)Unspecific peroxygenases (UPOs) are promising biocatalysts for oxyfunctionalisation reactions, owing to their simplicity of handling, stability and robustness. A limitation of using UPOs on a large scale is their deactivation in the presence of even rather modest concentrations of H<sub>2</sub>O<sub>2</sub>, requiring a constant and...journal article 2023
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Younes, S.H.H. (author), Hollmann, F. (author)A simple, solvent-free method for the synthesis of (thio)esters from simple acid chlorides at room temperature is reported. Simple FeCl<sub>3</sub> (5 mol%) enables facile, near complete conversion of equimolar starting materials in high selectivity. Recycling of the catalyst has been demonstrated.journal article 2023
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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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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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Wu, Bin (author), Wang, S. (author), Ma, Yunjian (author), Yuan, Shuguang (author), Hollmann, F. (author), Wang, Yonghua (author)Alcohol oxidases (AOxs) catalyze the aerobic oxidation of alcohols to the corresponding carbonyl products (aldehydes or ketones), producing only H<sub>2</sub>O<sub>2</sub> as the byproduct. The majority of known AOxs, however, have a strong preference for small, primary alcohols, limiting their broad applicability, e.g., in the food industry....journal article 2023
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Wu, Y. (author), Paul, C.E. (author), Hilberath, T. (author), Jongkind, E.P.J. (author), Zhang, Wuyuan (author), Alcalde, Miguel (author), Hollmann, F. (author)Utilisation of fatty acids generally relies on pre-existing functional groups such as the carboxylate group or C=C-double bonds. Addition of new functionalities into the hydrocarbon part opens up new possibilities for fatty acid valorisation. In this contribution we demonstrate the synthetic potential of a peroxygenase mutant AaeUPO−Fett for...journal article 2023
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Zhou, Jianle (author), Hollmann, F. (author), He, Qi (author), Chen, Wen (author), Ma, Yunjian (author), Wang, Yonghua (author)The realm of photobiocatalytic alkane biofuel synthesis has burgeoned recently; however, the current dearth of well-established and scalable production methodologies in this domain remains conspicuous. In this investigation, we engineered a modified form of membrane-associated fatty acid photodecarboxylase sourced from Micractinium conductrix...journal article 2023
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Zhong, Xuanru (author), Ma, Yunjian (author), Zhang, Xizhen (author), Zhang, Jiahui (author), Wu, Bin (author), Hollmann, F. (author), Wang, Yonghua (author)Hydrocarbon synthesis from (waste)oils enabled by a cascade of lipase-catalysed hydrolysis and decarboxylase-catalysed decarboxylation has become an active area of research en route to alternative, biobased fuels. However, Poor substrate transport efficiency is a major issue causing low reaction rates. This study focused on a protein self...journal article 2022
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Yoon, Jaeho (author), Jang, Hanhwi (author), Oh, Min Wook (author), Hilberath, T. (author), Hollmann, F. (author), Jung, Yeon Sik (author), Park, Chan Beum (author)Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed...journal article 2022
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Sang, Xianke (author), Tong, Feifei (author), Zeng, Zhigang (author), Wu, Minghu (author), Yuan, Bo (author), Sun, Zhoutong (author), Sheng, Xiang (author), Hollmann, F. (author), Zhang, W. (author)Propargylic alcohols and amines are versatile building blocks in organic synthesis. We demonstrate a straightforward enzymatic cascade to synthesize enantiomerically pure propargylic alcohols and amines from readily available racemic starting materials. In the first step, the peroxygenase from Agrocybe aegerita converted the racemic...journal article 2022
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Li, Zongquan (author), Ma, Yunjian (author), Hollmann, F. (author), Wang, Yonghua (author)Carvol and carvone are oxidation products from the natural product limonene. They are important raw materials for the flavours and fragrances industry and also act as pharmaceutical active ingredients. Orange waste peels possibly represent an attractive source for limonene, but studies on valorizing orange peel wastes are rare. In this study,...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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- Han, Jeong Woo (author), Hollmann, F. (author), Luque, Rafael (author), Song, In Kyu (author), Talarico, Giovanni (author), Tatsumi, Takashi (author), Yan, Ning (author) 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