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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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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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Acevedo-Rocha, Carlos G. (author), Hollmann, F. (author), Sanchis, Joaquin (author), Sun, Zhoutong (author)In this invited Account, we highlight the enormous scientific breadth of our mentor Professor Manfred T. Reetz. It stretches from the development of organometallic reagents and transition metal catalysts to the adventurous idea of directed evolution of chemo-, stereo-, and regioselective enzymes, which he considered to be most important. We...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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Evolved Peroxygenase-Aryl Alcohol Oxidase Fusions for Self-Sufficient Oxyfunctionalization ReactionsGomez De Santos, Patricia (author), Lazaro, Sofia (author), Viña-Gonzalez, Javier (author), Hoang, Manh Dat (author), Sánchez-Moreno, Israel (author), Glieder, Anton (author), Hollmann, F. (author), Alcalde, Miguel (author)Fungal peroxygenases are deemed emergent biocatalysts for selective C-H bond oxyfunctionalization reactions. In this study, we have engineered a functional and stable self-sufficient chimeric peroxygenase-oxidase fusion. The bifunctional biocatalyst carried a laboratory-evolved version of the fungal peroxygenase fused to an evolved fungal...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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Zhang, Tianyu (author), Ma, Yunjian (author), Tan, Chin Ping (author), Hollmann, F. (author), Wang, Jianrong (author), Yang, Bo (author), Wang, Yonghua (author)Poor H <sub>2</sub> O <sub>2</sub> -resistance by enzymes is a key bottleneck in the epoxidation process of oil by enzymatic methods. In this study, the stability of three lipases, from Aspergillus oryzae lipase (AOL), Aspergillus fumigatus lipase B (AflB), and marine Janibacter (MAJ1), in the presence of H <sub>2</sub> O <sub>2</sub> was...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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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