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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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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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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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Lacerda, Sara (author), Zhang, W. (author), T. M. De Rosales, Rafael (author), Da Silva, Isidro (author), Sobilo, Julien (author), Lerondel, Stéphanie (author), Tóth, Éva (author), Djanashvili, K. (author)Porous materials, such as zeolites, have great potential for biomedical applications, thanks to their ability to accommodate positively charged metal-ions and their facile surface functionalization. Although the latter aspect is important to endow the nanoparticles with chemical/colloidal stability and desired biological properties, the...journal article 2022
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Zhang, W. (author), Askarinejad, A. (author)Submarine slope instabilities are considered one of the major threats for offshore buried pipelines. This paper presents a novel method to evaluate the ultimate pressure acting on a buried pipeline during the liquefaction of an inclined seabed. Small-scale model tests with pipes buried at three different embedment ratios have been conducted...journal article 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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Zhang, W. (author)The assessment of the potentially destructive impacts of subaqueous landslides on offshore pipelines is required when the pipeline route passes through zones with a risk of mass movements. Therefore, quantifying and evaluating the ultimate load/pressure acting on the pipeline is one of the key factors in geotechnical safety design of the...doctoral thesis 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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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), 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
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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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Ma, Yunjian (author), Li, Yongru (author), Ali, Shahid (author), Li, Peilin (author), Zhang, W. (author), Rauch, M.C.R. (author), Willot, S.J. (author), Ribitsch, Doris (author), Hollmann, F. (author)Natural deep eutectic solvents (NADES) are proposed as alternative solvents for peroxygenase-catalysed oxyfunctionalization reactions. Choline chloride-based NADES are of particular interest as they can serve as solvent, enzyme-stabiliser and sacrificial electron donor for the in situ H<sub>2</sub>O<sub>2</sub> generation. This report...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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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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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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Zhang, W. (author), Ma, M. (author), Huijbers, M.M.E. (author), Filonenko, G.A. (author), Pidko, E.A. (author), van Schie, M.M.C.H. (author), de Boer, Sabrina (author), Smith, W.A. (author), Hollmann, F. (author)A recently discovered photodecarboxylase from Chlorella variabilis NC64A ( CvFAP) bears the promise for the efficient and selective synthesis of hydrocarbons from carboxylic acids. CvFAP, however, exhibits a clear preference for long-chain fatty acids thereby limiting its broad applicability. In this contribution, we demonstrate that the...journal article 2019
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Gacs, Jenő (author), Zhang, W. (author), Knaus, Tanja (author), Mutti, Francesco G. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)The consecutive photooxidation and reductive amination of various alcohols in a cascade reaction were realized by the combination of a photocatalyst and several enzymes. Whereas the photocatalyst (sodium anthraquinone-2-sulfonate) mediated the light-driven, aerobic oxidation of primary and secondary alcohols, the enzymes (various ω...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
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Ma, Yunjian (author), Li, Peilin (author), Li, Yongru (author), Willot, S.J. (author), Zhang, W. (author), Ribitsch, Doris (author), Choi, Young Hae (author), Verpoorte, Robert (author), Hollmann, F. (author)The use of natural deep eutectic solvents (NADES) as multifunctional solvents for limonene bioprocessing was reported. NADES were used for the extraction of limonene from orange peel wastes, as solvent for the chemoenzymatic epoxidation of limonene, and as sacrificial electron donor for the in situ generation of H <sub>2</sub> O <sub>2</sub>...journal article 2019
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Burek, Bastien O. (author), de Boer, Sabrina R. (author), Tieves, F. (author), Zhang, W. (author), van Schie, M.M.C.H. (author), Bormann, Sebastian (author), Alcalde, Miguel (author), Holtmann, Dirk (author), Hollmann, F. (author)Photoenzymatic cascades can be used for selective oxygenation of C−H-Bonds under mild conditions circumventing the hydrogen peroxide mediated peroxygenase inactivation via in situ H<sub>2</sub>O<sub>2</sub> generation. Here, we report the “on demand” production of hydrogen peroxide via methanol assisted reduction of molecular oxygen using UV...journal article 2019