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Paul, C.E. (author), Hanefeld, U. (author), Hollmann, F. (author), Qu, Ge (author), Yuan, Bo (author), Sun, Zhoutong (author)Contemporary Biocatalysis heavily relies on enzyme engineering as natural enzymes frequently lack the requisite attributes for effective organic synthesis. The inherent limitations in stability, catalytic activity, and selectivity of wild-type enzymes often hinder their suitability for chemical synthesis. Over the past 25 years, there has...journal article 2024
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Heckmann, C.M. (author), Bürgler, Moritz (author), Paul, C.E. (author)The unmatched chemo-, regio-, and stereoselectivity of enzymes renders them powerful catalysts in the synthesis of chiral active pharmaceutical ingredients (APIs). Inspired by the discovery route toward the LPA<sub>1</sub>-antagonist BMS-986278, access to the API building block (1S,3R)-3-hydroxycyclohexanecarbonitrile was envisaged using an...journal article 2024
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Paul, A. (author), Rafigh Doost, J. (author), Dou, X. (author), Pereira, S.F. (author)Nanostructures with steep side wall angles (swa) play a pivotal role in various technological applications. Accurate characterization of these nanostructures is crucial for optimizing their performance. In this study, we propose a far-field detection method based on coherent Fourier scatterometry (CFS) for accurate quantification of steep swa...journal article 2024
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Heckmann, C.M. (author), Paul, C.E. (author)Chiral N-heterocycles are a common motif in many active pharmaceutical ingredients; however, their synthesis often relies on the use of heavy metals. In recent years, several biocatalytic approaches have emerged to reach enantiopurity. Here, we describe the asymmetric synthesis of 2-substituted pyrrolidines and piperidines, starting from...journal article 2023
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Medipally, Hitesh (author), Guarneri, Alice (author), Pospisil, Lars (author), Franssen, Maurice C.R. (author), van Berkel, Willem J.H. (author), Paul, C.E. (author), Nowaczyk, Marc M. (author)Biocatalytic asymmetric reduction of C=C and C=O bonds is highly attractive to produce valuable (chiral) chemicals for the fine and pharmaceutical industry, yet occurs at the expense of reduced nicotinamide adenine dinucleotide coenzyme NADPH that requires recycling. Established methods each have their challenges. Here we developed a light...journal article 2023
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Wu, Y. (author), Paul, C.E. (author), Hollmann, F. (author)This review article critically compares two widely used types of catalysis, chemo- and biocatalysis, and provides insights on their greenness according to specified parameters. A comparative analysis of the environmental impact of chemo- and biocatalytic oxyfunctionalisation reactions based on published experimental data reveals that both...journal article 2023
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Röllig, Robert (author), Paul, C.E. (author), Rousselot-Pailley, Pierre (author), Kara, Selin (author), Alphand, Véronique (author)Taking advantage of the unique properties of two-component flavo-monooxygenases and the ability of [Cp*Ir(bpy-OMe)H]<sup>+</sup> to transfer hydrides to reduce flavins, we extended the scope of the pH- and oxygen-robust iridium(iii)-complex to drive the enzymatic reaction of a FMN-dependent Baeyer-Villiger monooxygenase and a FAD-dependent...journal article 2023
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Villa Aroca, R. (author), Ferrer Carbonell, C. (author), Paul, C.E. (author)Biocatalytic asymmetric reduction of alkenes in organic solvent is attractive for enantiopurity and product isolation, yet remains under developed. Herein we demonstrate the robustness of an ene reductase immobilised on Celite for the reduction of activated alkenes in micro-aqueous organic solvent. Full conversion was obtained in methyl t...journal article 2023
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Xu, X. (author), van Hengst, J.M.A. (author), Mao, Yejia (author), Martinez, Mireia (author), Roda, Sergi (author), Floor, Martin (author), Guallar, Victor (author), Paul, C.E. (author), Alcalde, Miguel (author), Hollmann, F. (author)A peroxygenase-catalysed hydroxylation of organosilanes is reported. The recombinant peroxygenase from Agrocybe aegerita (AaeUPO) enabled efficient conversion of a broad range of silane starting materials in attractive productivities (up to 300 mM h<sup>−1</sup>), catalyst performance (up to 84 s<sup>−1</sup> and more than 120 000 catalytic...journal article 2023
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Alphand, Véronique (author), van Berkel, Willem J.H. (author), Jurkaš, Valentina (author), Kara, Selin (author), Kourist, Robert (author), Kroutil, Wolfgang (author), Mascia, Francesco (author), Nowaczyk, Marc M. (author), Paul, C.E. (author)The recent increase of interest in photocatalysis spread to biocatalysis and triggered a rush for the development of light-dependent enzyme-mediated or enzyme-coupled processes. After several years of intense research on photobiocatalysis, it is time to evaluate the state of the field in a structured manner. In this Perspective, we suggest to...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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Paul, A. (author), Kolenov, D. (author), Scholte, T.C. (author), Pereira, S.F. (author)Detecting defects on diffraction gratings is crucial for ensuring their performance and reliability. Practical detection of these defects poses challenges due to their subtle nature.We performnumerical investigations and demonstrate experimentally the capability of coherent Fourier scatterometry (CFS) to detect particles as small as 100 nm...journal article 2023
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Mehta, Piyush M. (author), Paul, Smriti N. (author), Crisp, Nicholas H. (author), Sheridan, Philip L. (author), Siemes, C. (author), March, G. (author), Bruinsma, Sean (author)Satellite drag modeling remains the largest source of uncertainty affecting space operations in low Earth orbit. The uncertainty stems from inaccurate models for mass density and drag coefficient. Drag coefficient modeling also impacts scientific knowledge on the physics and dynamics of the upper atmosphere through the estimation of high...journal article 2022
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Zhang, Linyue (author), King, Edward (author), Black, William B. (author), Heckmann, C.M. (author), Wolder, A.E. (author), Cui, Youtian (author), Nicklen, Francis (author), Siegel, Justin B. (author), Paul, C.E. (author)Noncanonical redox cofactors are attractive low-cost alternatives to nicotinamide adenine dinucleotide (phosphate) (NAD(P)<sup>+</sup>) in biotransformation. However, engineering enzymes to utilize them is challenging. Here, we present a high-throughput directed evolution platform which couples cell growth to the in vivo cycling of a...journal article 2022
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Ottun, Abdul Rasheed (author), Mane, Pramod C. (author), Yin, Zhigang (author), Paul, Souvik (author), Liyanage, Mohan (author), Pridmore, Jason (author), Ding, Aaron Yi (author), Sharma, Rajesh (author), Nurmi, Petteri (author), Flores, Huber (author)Federated learning (FL) is a promising privacy-preserving solution to build powerful AI models. In many FL scenarios, such as healthcare or smart city monitoring, the user's devices may lack the required capabilities to collect suitable data, which limits their contributions to the global model. We contribute social-aware federated learning...journal article 2022
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Röllig, Robert (author), Paul, C.E. (author), Duquesne, Katia (author), Kara, Selin (author), Alphand, Véronique (author)Temperature is a crucial parameter for biological and chemical processes. Its effect on enzymatically catalysed reactions has been known for decades, and stereo- and enantiopreference are often temperature-dependent. For the first time, we present the temperature effect on the Baeyer-Villiger oxidation of rac-bicyclo[3.2.0]hept-2-en-6-one by...journal article 2022
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Reeve, Holly A. (author), Nicholson, Jake (author), Altaf, Farieha (author), Lonsdale, Thomas H. (author), Preissler, Janina (author), Lauterbach, Lars (author), Lenz, Oliver (author), Leimkühler, Silke (author), Hollmann, F. (author), Paul, C.E. (author), Vincent, Kylie A. (author)We demonstrate a recycling system for synthetic nicotinamide cofactor analogues using a soluble hydrogenase with turnover number of >1000 for reduction of the cofactor analogues by H2. Coupling this system to an ene reductase, we show quantitative conversion of N-ethylmaleimide to N-ethylsuccinimide. The biocatalyst system retained >50%...journal article 2022
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Xu, X. (author), Brasselet, H.L.Y. (author), Jongkind, E.P.J. (author), Alcalde, Miguel (author), Paul, C.E. (author), Hollmann, F. (author)In this study, we developed a new bienzymatic reaction to produce enantioenriched phenylethanols. In a first step, the recombinant, unspecific peroxygenase from Agrocybe aegerita (rAaeUPO) was used to oxidise ethylbenzene and its derivatives to the corresponding ketones (prochiral intermediates) followed by enantioselective reduction into the...journal article 2022
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Ribeaucourt, David (author), Höfler, G.T. (author), Yemloul, Mehdi (author), Bissaro, Bastien (author), Lambert, Fanny (author), Berrin, Jean Guy (author), Lafond, Mickael (author), Paul, C.E. (author)Biocatalytic pathways for the synthesis of (-)-menthol, the most sold flavor worldwide, are highly sought-after. To access the key intermediate (R)-citronellal used in current major industrial production routes, we established a one-pot bienzymatic cascade from inexpensive geraniol, overcoming the problematic biocatalytic reduction of the...journal article 2022
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Synthesis of Chiral Amines via a Bi-Enzymatic Cascade Using an Ene-Reductase and Amine DehydrogenaseJongkind, E.P.J. (author), Fossey-Jouenne, Aurélie (author), Mayol, Ombeline (author), Zaparucha, Anne (author), Vergne-Vaxelaire, Carine (author), Paul, C.E. (author)Access to chiral amines with more than one stereocentre remains challenging, although an increasing number of methods are emerging. Here we developed a proof-of-concept bi-enzymatic cascade, consisting of an ene reductase and amine dehydrogenase (AmDH), to afford chiral diastereomerically enriched amines in one pot. The asymmetric reduction...journal article 2021