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Yayci, Abdulkadir (author), Baraibar, Álvaro Gómez (author), Krewing, Marco (author), Fernandez Fueyo, E. (author), Hollmann, F. (author), Alcalde, Miguel (author), Kourist, Robert (author), Bandow, Julia E. (author)Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one-electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a...journal article 2020
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Willot, S.J. (author), Hoang, Manh Dat (author), Paul, C.E. (author), Alcalde, Miguel (author), Arends, I.W.C.E. (author), Bommarius, Andreas S. (author), Bommarius, Bettina (author), Hollmann, F. (author)The novel formate oxidase from Aspergillus oryzae (AoFOx) is a useful catalyst to promote H<sub>2</sub>O<sub>2</sub>-dependent oxyfunctionalisation reactions. In this contribution we exploit the substrate promiscuity of AoFOx to fully oxidise methanol and formaldehyde to CO<sub>2</sub> and drive peroxygenase-catalysed stereoselective...journal article 2020
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Choi, Da Som (author), Kim, Jinhyun (author), Hollmann, F. (author), Park, Chan Beum (author)Inspired by natural photosynthesis, biocatalytic photoelectrochemical (PEC) platforms are gaining prominence for the conversion of solar energy into useful chemicals by combining redox biocatalysis and photoelectrocatalysis. Herein, we report a dual biocatalytic PEC platform consisting of a molybdenum (Mo)-doped BiVO<sub>4</sub> (Mo:BiVO<sub...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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Perz, Frederic (author), Bormann, Sebastian (author), Ulber, Roland (author), Alcalde, Miguel (author), Bubenheim, Paul (author), Hollmann, F. (author), Holtmann, Dirk (author), Liese, Andreas (author)Unspecific peroxygenases have recently gained significant interest due to their ability to catalyse the hydroxylation of non-activated C−H bonds using only hydrogen peroxide as a co-substrate. However, the development of preparative processes has so far mostly concentrated on benzylic hydroxylations using liquid substrates. Herein, we...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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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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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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Rauch, M.C.R. (author), Huijbers, M.M.E. (author), Pabst, Martin (author), Paul, C.E. (author), Pesic, M. (author), Arends, I.W.C.E. (author), Hollmann, F. (author)Direct, NAD(P)H-independent regeneration of Old Yellow Enzymes represents an interesting approach for simplified reaction schemes for the stereoselective reduction of conjugated C=C-double bonds. Simply by illuminating the reaction mixtures with blue light in the presence of sacrificial electron donors enables to circumvent the costly and...journal article 2020
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Yuan, Bo (author), Mahor, Durga (author), Fei, Qiang (author), Wever, Ron (author), Alcalde, Miguel (author), Zhang, Wuyuan (author), Hollmann, F. (author)Peroxyzymes simply use H2O2 as a cosubstrate to oxidize a broad range of inert C-H bonds. The lability of many peroxyzymes against H2O2 can be addressed by a controlled supply of H2O2, ideally in situ. Here, we report a simple, robust, and water-soluble anthraquinone sulfonate (SAS) as a promising organophotocatalyst to drive both...journal article 2020
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Yayci, Abdulkadir (author), Dirks, Tim (author), Kogelheide, Friederike (author), Alcalde, Miguel (author), Hollmann, F. (author), Awakowicz, Peter (author), Bandow, Julia E. (author)The use of a microscale atmospheric pressure plasma jet (μAPPJ) was investigated for its potential to supply hydrogen peroxide in biocatalysis. Compared to a previously employed dielectric barrier discharge (DBD), the μAPPJ offered significantly higher H<sub>2</sub>O<sub>2</sub> production rates and better handling of larger reaction volumes....journal article 2020
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Gomez de Santos, P. (author), Cervantes, Fadia V. (author), Tieves, F. (author), Plou, Francisco J. (author), Hollmann, F. (author), Alcalde, Miguel (author)By mimicking the role of human liver P450 monooxygenases, fungal unspecific peroxygenases (UPOs) can perform a range of highly selective oxyfunctionalization reactions on pharmacological compounds, including O-dealkylations and hydroxylations, thereby simulating drug metabolism. Here we have benchmarked human drug metabolite (HDM) synthesis...journal article 2019
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Aslan-Üzel, Aşkın S. (author), Beier, Andy (author), Kovář, David (author), Cziegler, Clemens (author), Padhi, Santosh K. (author), Schuiten, Eva D. (author), Dörr, Mark (author), Böttcher, Dominique (author), Hollmann, F. (author)Halide assays are important for the study of enzymatic dehalogenation, a topic of great industrial and scientific importance. Here we describe the development of a very sensitive halide assay that can detect less than a picomole of bromide ions, making it very useful for quantifying enzymatic dehalogenation products. Halides are oxidised...journal article 2019
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Yoon, Jaeho (author), Lee, S.H. (author), Tieves, F. (author), Rauch, M.C.R. (author), Hollmann, F. (author), Park, Chan Beum (author)We report visible light-driven, asymmetric hydrogenation of C=C bonds using an ene-reductase from Thermus scotoductus SA-01 (TsOYE) and a light-harvesting dye (rose bengal, RB) co-immobilized in an alginate hydrogel. Highly efficient encapsulation of RB in alginate hydrogel was achieved using the intrinsic affinity between TsOYE and RB,...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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Tieves, F. (author), Tonin, F. (author), Fernandez Fueyo, E. (author), Robbins, John M. (author), Bommarius, Bettina (author), Bommarius, Andreas S. (author), Alcalde, Miguel (author), Hollmann, F. (author)The E-factor has become an important measure for the environmental impact of (bio)chemical reactions. However, summing up the obvious wastes generated in the laboratory neglects energy-related wastes (mostly greenhouse gases) which are generated elsewhere. To estimate these wastes, we propose to extend the E-factor by an energy-term (E<sup>+<...journal article 2019
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Vignali, Valentina (author), S. Miranda, Barbara (author), Lodoso-Torrecilla, Irene (author), Van Nisselroy, Cathelijn A.J. (author), Hoogenberg, Bas Jan (author), Dantuma, Sybren (author), Hollmann, F. (author), De Vries, Jan Willem (author)Engineered viruses are finding an increasing number of applications in basic, translational research and materials science. Genetic and chemical engineering of capsids represents a key point for tailoring the properties of viral particles, but the synthetic efforts and limits accompanying these processes still hinder their usability. Here, a...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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Höfler, G.T. (author), But, A. (author), Hollmann, F. (author)Haloperoxidases are very active catalysts for the in situ generation of electrophilic halide species for oxidative halogenation reactions. In the synthetic community, these catalysts, however, are not widely used. The aim of this mini-review is to critically summarise the current state-of-the-art of haloperoxidase catalysis for organic...journal article 2019
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Leemans, Laura (author), Walter, Marc D. (author), Hollmann, F. (author), Schallmey, Anett (author), van Langen, L.M. (author)Enantiopure β-amino alcohols constitute one of the most significant building blocks for the synthesis of active pharmaceutical ingredients. Despite the availability of a range of chiral β-amino alcohols from a chiral pool, there is a growing demand for new enantioselective synthetic routes to vicinal amino alcohols and their derivatives. In...journal article 2019