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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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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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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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Ma, Yunjian (author), Zhong, Xuanru (author), Wu, Bin (author), Lan, Dongming (author), Zhang, Hao (author), Hollmann, F. (author), Wang, Yonghua (author)Hydrocarbons are essential base chemicals as energy carriers and starting materials for chemical manufacture. So-called fatty acid photodecarboxylases (FAPs) represent interesting catalysts for the conversion of natural fatty acids into hydrocarbons thereby giving access to alkanes from renewable feedstock. Today, however, only few FAPs are...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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Ma, Yunjian (author), Li, Zongquan (author), Zhang, Hao (author), Wong, Vincent Kam Wai (author), Hollmann, F. (author), Wang, Yonghua (author)Aromatic aldehydes are important aromatic compounds for the flavour and fragrance industry. In this study, a parallel cascade combining aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) and unspecific peroxygenase from the basidiomycete Agrocybe aegerita (AaeUPO) to convert aromatic primary alcohols into high-value aromatic aldehydes is...journal article 2023
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Wang, Y. (author), Teetz, Niklas (author), Holtmann, Dirk (author), Alcalde, Miguel (author), van Hengst, J.M.A. (author), Liu, Xiaoxiao (author), Wang, Mengfan (author), Qi, Wei (author), Zhang, Wuyuan (author), Hollmann, F. (author)Biocatalytic oxidation reactions of toluene derivates to the corresponding aldehydes are typically challenged by regio- and chemoselectivity issues. In this contribution we address both challenges by a combined reactant- and reaction engineering approach. We demonstrate that the peroxygenase-catalysed transformation of ring-substituted...journal article 2023
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Chen, Shaohang (author), Zhang, Jiaan (author), Zeng, Zhigang (author), Dai, Zongjie (author), Wang, Qinhong (author), Wever, Ron (author), Hollmann, F. (author), Zhang, W. (author)A chemoenzymatic method for the synthesis of haloethers is presented. A combination of enzymatic hypohalite synthesis with spontaneous oxidation of alkenes and nucleophilic attack by various alcohols enabled the synthesis of a wide range of haloethers. The reaction system has been characterised and current imitations have been worked out. In...journal article 2022
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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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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, 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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Alagumalai, Avinash (author), Mahian, Omid (author), Hollmann, F. (author), Zhang, Wuyuan (author)Versatile bio-derived catalysts have been under dynamic investigation as potential substitutes to conventional chemical catalysts for sustainable biodiesel production. This is because of their unique, low-cost benefits and production processes that are environmentally and economically acceptable. This critical review aspires to present a...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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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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Lin, Richen (author), Deng, Chen (author), Zhang, Wuyuan (author), Hollmann, F. (author), Murphy, Jerry D. (author)Bioelectrochemical technologies such as electro-fermentation and microbial CO<sub>2</sub> electrosynthesis are emerging interdisciplinary technologies that can produce renewable fuels and chemicals (such as carboxylic acids). The benefits of electrically driven bioprocesses include improved production rate, selectivity, and carbon conversion...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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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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Ma, Yunjian (author), Zhang, Xizhen (author), Li, Yongru (author), Li, Peilin (author), Hollmann, F. (author), Wang, Yonghua (author)A biocatalytic cascade transforming castor oil into (R,Z)-octadec-9-en-7-ol is presented by combining a lipase catalysed hydrolysis of castor oil into ricinoleic acid followed by a photoenzymatic decarboxylation into (R,Z)-octadec-9-en-7-ol. Conversion of up to 41.7% and overall product concentrations of up to 60 mM, this new bienzymatic and...journal article 2020
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Zhang, W. (author), Lee, Jeong Hoo (author), Younes, S.H.H. (author), Tonin, F. (author), Hagedoorn, P.L. (author), Pichler, Harald (author), Baeg, Yoonjin (author), Park, Jin-Buang (author), Hollmann, F. (author), Kourist, Robert (author)En route to a bio-based chemical industry, the conversion of fatty acids into building blocks is of particular interest. Enzymatic routes, occurring under mild conditions and excelling by intrinsic selectivity, are particularly attractive. Here we report photoenzymatic cascade reactions to transform unsaturated fatty acids into...journal article 2020