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Kim, Jinhyun (author), Lee, S.H. (author), Tieves, F. (author), Choi, Da Som (author), Hollmann, F. (author), Paul, C.E. (author), Park, Chan Beum (author)Light-driven activation of redox enzymes is an emerging route for sustainable chemical synthesis. Among redox enzymes, the family of Old Yellow Enzyme (OYE) dependent on the nicotinamide adenine dinucleotide cofactor (NADH) catalyzes the stereoselective reduction of α,β-unsaturated hydrocarbons. Here, we report OYE-catalyzed asymmetric...journal article 2018
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Hobisch, Markus (author), van Schie, M.M.C.H. (author), Kim, Jinhyun (author), Røjkjær Andersen, Kasper (author), Alcalde, Miguel (author), Kourist, Robert (author), Park, Chan Beum (author), Hollmann, F. (author), Kara, S. (author)The use of neat reaction media, that is the avoidance of additional solvents, is the simplest and the most efficient approach to follow in biocatalysis. Here, we show that unspecific peroxygenase from Agrocybe aegerita (AaeUPO) can hydroxylate the neat model substrate cyclohexane. H<sub>2</sub>O<sub>2</sub> was photocatalytically generated in...journal article 2020
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Song, Ji Won (author), Baeg, Yoonjin (author), Jeong, Ha Yeon (author), Lee, Jinwon (author), Oh, Deok Kun (author), Hollmann, F. (author), Park, Jin Byung (author)Bacterial outer membrane vesicles (OMVs) are small unilamellar proteoliposomes, involved in various functions including cell-to-cell signalling and protein excretion. We have engineered the OMVs of Escherichia coli to nano-scaled bioreactors for the biotransformation of fatty acids by targeting a fatty acid double bond hydratase of...journal article 2021
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Hwang, Se Yeun (author), Song, Dayoon (author), Seo, Eun Ji (author), Hollmann, F. (author), You, Youngmin (author), Park, Jin Byung (author)Photobiocatalysis is a growing field of biocatalysis. Especially light-driven enzyme catalysis has contributed significantly to expanding the scope of synthetic organic chemistry. However, photoenzymes usually utilise a rather narrow wavelength range of visible (sun)light. Triplet–triplet annihilation-based upconversion (TTA-UC) of long...journal article 2022
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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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Kim, Chang Hyun (author), Kim, Jinhyun (author), Hollmann, F. (author), Park, Chan Beum (author)Solar-driven N<sub>2</sub> fixation offers a green alternative to the highly energy-intensive Haber-Bosch process that releases more than 300 million metric tons of CO<sub>2</sub> annually to form NH<sub>3</sub>. However, N<sub>2</sub>-reducing photoelectrochemical (PEC) studies have not elucidated how an oxidation reaction affects the N<sub...journal article 2023
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Yoon, Jaeho (author), Jang, Hanhwi (author), Oh, Min Wook (author), Hilberath, T. (author), Hollmann, F. (author), Jung, Yeon Sik (author), Park, Chan Beum (author)Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed...journal article 2022
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Kim, Jinhyun (author), Um, Yunna (author), Han, Seunghyun (author), Hilberath, T. (author), Kim, Yong Hwan (author), Hollmann, F. (author), Park, Chan Beum (author)The pulp and paper manufacturers generate approximately 50 million metric tons of lignin per annum, most of which has been abandoned or incinerated because of lignin's recalcitrant nature. Here, we report bias-free photoelectrochemical (PEC) oxidation of lignin coupled with asymmetric hydrogenation of C=C bonds. The PEC platform consists of a...journal article 2022
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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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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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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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Son, Eun Jin (author), Lee, Sahng Ha (author), Kuk, Su Keun (author), Pesic, M. (author), Choi, Da Som (author), Ko, Jong Wan (author), Kim, Kayoung (author), Hollmann, F. (author), Park, Chan Beum (author)In green plants, solar-powered electrons are transferred through sophistically arranged photosystems and are subsequently channelled into the Calvin cycle to generate chemical energy. Inspired by the natural photosynthetic scheme, a photoelectrochemical cell (PEC) is constructed configured with protonated graphitic carbon nitride (p-g-C<sub>3...journal article 2017
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Cofactor-Free, Direct Photoactivation of Enoate Reductases for the Asymmetric Reduction of C=C BondsLee, Sahng Ha (author), Choi, Da Som (author), Pesic, M. (author), Lee, Yang Woo (author), Paul, C.E. (author), Hollmann, F. (author), Park, Chan Beum (author)Enoate reductases from the family of old yellow enzymes (OYEs) can catalyze stereoselective trans-hydrogenation of activated C=C bonds. Their application is limited by the necessity for a continuous supply of redox equivalents such as nicotinamide cofactors [NAD(P)H]. Visible light-driven activation of OYEs through NAD(P)H-free, direct...journal article 2017
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Choi, Da Som (author), Ni, Y. (author), Fernandez Fueyo, E. (author), Lee, Minah (author), Hollmann, F. (author), Park, Chan Beum (author)Peroxygenases are very promising catalysts for oxyfunctionalization reactions. Their practical applicability, however, is hampered by their sensitivity against the oxidant (H<sub>2</sub>O<sub>2</sub>), therefore necessitating in situ generation of H<sub>2</sub>O<sub>2</sub>. Here, we report a photoelectrochemical approach to provide...journal article 2017
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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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Kim, Jinhyun (author), Lee, Sahng Ha (author), Tieves, F. (author), Paul, C.E. (author), Hollmann, F. (author), Park, Chan Beum (author)Nicotinamide adenine dinucleotide (NAD<sup>+</sup>) is a key redox compound in all living cells responsible for energy transduction, genomic integrity, life-span extension, and neuromodulation. Here, we report a new function of NAD<sup>+</sup> as a molecular photocatalyst in addition to the biological roles. Our spectroscopic and...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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Yun, Chul Ho (author), Kim, Jinhyun (author), Hollmann, F. (author), Park, Chan Beum (author)Enzymes are the catalyst of choice for highly selective reactions, offering nature-inspired approaches for sustainable chemical synthesis. Oxidative enzymes (e.g., monooxygenases, peroxygenases, oxidases, or dehydrogenases) catalyze a variety of enantioselective oxyfunctionalization and dehydrogenation reactions under mild conditions. To...review 2022