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Paul, C.E. (author), Hanefeld, U. (author), Hollmann, F. (author), Qu, Ge (author), Yuan, Bo (author), Sun, Zhoutong (author)Contemporary Biocatalysis heavily relies on enzyme engineering as natural enzymes frequently lack the requisite attributes for effective organic synthesis. The inherent limitations in stability, catalytic activity, and selectivity of wild-type enzymes often hinder their suitability for chemical synthesis. Over the past 25 years, there has...journal article 2024
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Liu, Yunting (author), Ma, Teng (author), Guo, Zhongxu (author), Zhou, Liya (author), Liu, Guanhua (author), He, Ying (author), Ma, Li (author), Gao, Jing (author), Hollmann, F. (author)Chemoenzymatic cascade catalysis has emerged as a revolutionary tool for streamlining traditional retrosynthetic disconnections, creating new possibilities for the asymmetric synthesis of valuable chiral compounds. Here we construct a one-pot concurrent chemoenzymatic cascade by integrating organobismuth-catalyzed aldol condensation with ene...journal article 2024
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Jaroensuk, Juthamas (author), Sutthaphirom, Chalermroj (author), Phonbuppha, Jittima (author), Chinantuya, Wachirawit (author), Kesornpun, Chatchai (author), Akeratchatapan, Nattanon (author), Kittipanukul, Narongyot (author), Phatinuwat, Kamonwan (author), Hollmann, F. (author)Cofactor imbalance obstructs the productivities of metabolically engineered cells. Herein, we employed a minimally perturbing system, xylose reductase and lactose (XR/lactose), to increase the levels of a pool of sugar phosphates which are connected to the biosynthesis of NAD(P)H, FAD, FMN, and ATP in Escherichia coli. The XR/lactose system...journal article 2024
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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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- Hollmann, F. (author), Woodley, John M. (author) contribution to periodical 2023
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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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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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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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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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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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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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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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Wu, Y. (author), Paul, C.E. (author), Hollmann, F. (author)This review article critically compares two widely used types of catalysis, chemo- and biocatalysis, and provides insights on their greenness according to specified parameters. A comparative analysis of the environmental impact of chemo- and biocatalytic oxyfunctionalisation reactions based on published experimental data reveals that both...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