Multistep enzyme cascades as a route towards green and sustainable pharmaceutical syntheses

Nature Chemistry, Год журнала: 2022, Номер 14(5), С. 489 - 499

Опубликована: Май 1, 2022

Язык: Английский

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State-of-the-Art Biocatalysis

ACS Central Science, Год журнала: 2021, Номер 7(7), С. 1105 - 1116

Опубликована: Июнь 25, 2021

The use of enzyme-mediated reactions has transcended ancient food production to the laboratory synthesis complex molecules. This evolution been accelerated by developments in sequencing and DNA technology, bioinformatic protein engineering tools, increasingly interdisciplinary nature scientific research. Biocatalysis become an indispensable tool applied academic industrial spheres, enabling synthetic strategies that leverage exquisite selectivity enzymes access target In this Outlook, we outline technological advances have led field's current state. Integration biocatalysis into mainstream chemistry hinges on increased well-characterized permeation retrosynthetic logic. Ultimately, anticipate is poised enable molecules at new levels efficiency throughput.

Язык: Английский

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Dearomative logic in natural product total synthesis

Natural Product Reports, Год журнала: 2022, Номер 39(12), С. 2231 - 2291

Опубликована: Янв. 1, 2022

This review explores the strategies and tactics of effective dearomative retrosynthetic logic, illustrated through numerous outstanding examples contemporary natural product total synthesis.

Язык: Английский

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Flow chemistry in the multi-step synthesis of natural products

Green Synthesis and Catalysis, Год журнала: 2022, Номер 3(3), С. 243 - 258

Опубликована: Авг. 1, 2022

The total synthesis of natural products is constantly facing many challenges derived from the complexed chemical structures, lengthy synthetic routes, time-consuming workup procedures and large environmental footprint. In past two decades, performing transformations in continuous flow using various types microreactors in-line auxiliary technologies have been demonstrated effectively respects enhanced reaction yield selectivity, excellent reproducibility easy scale-up, safe proceeding hazardous reaction. And rapid products, which has enabled based upon significant improvement overall within a short residence time via processing intensification systematic automation, essential to furnish sufficient quantity for bioactivity investigation structural diversity modification, structure-activity relationship during drug discovery increasing consumption medical treatment. this review, multi-step highlighted provide comprehensive recognization on intrinsic merits chemistry organic chemists purposefully develop approaches future.

Язык: Английский

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Synthesis of Natural Products by C−H Functionalization of Heterocycless

Chemistry - A European Journal, Год журнала: 2022, Номер 28(22)

Опубликована: Янв. 28, 2022

Total synthesis is considered by many as the finest combination of art and science. During last decades, several concepts were proposed for achieving perfect vision total synthesis, such atom economy, step or redox economy. In this context, C-H functionalization represents most powerful platform that has emerged in years, empowering rapid complex natural products enabling diversification bioactive scaffolds based on product architectures. review, we present an overview recent strategies towards heterocyclic enabled functionalization. Heterocycles represent common motifs drug discovery marketed drugs. The implementation heterocycles enables novel tactics construction core architectures, but also changes logic design retrosynthetic permits access to with enhanced biological activities.

Язык: Английский

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Merging enzymatic and synthetic chemistry with computational synthesis planning

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Дек. 14, 2022

Synthesis planning programs trained on chemical reaction data can design efficient routes to new molecules of interest, but are limited in their ability leverage rare transformations. This challenge is acute for enzymatic reactions, which valuable due selectivity and sustainability few number. We report a retrosynthetic search algorithm using two neural network models retrosynthesis-one covering 7984 transformations one 163,723 synthetic transformations-that balances the exploration reactions identify hybrid synthesis plans. approach extends space moves by thousands uniquely one-step transformations, discovers or searches find none, designs shorter others. Application (-)-Δ9 tetrahydrocannabinol (THC) (dronabinol) R,R-formoterol (arformoterol) illustrates how our strategy facilitates replacement metal catalysis, high step counts, costly enantiomeric resolution with more elegant proposals.

Язык: Английский

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Chemoenzymatic synthesis of C14-functionalized steroids

Nature Synthesis, Год журнала: 2023, Номер 2(8), С. 729 - 739

Опубликована: Апрель 17, 2023

Язык: Английский

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The Key Effect of Carboxyl Group and CuN₂O₂ Coordinate Structure for Cu, N Co‐Doped Carbon Dots with Peroxidase‐Like Property

Small, Год журнала: 2023, Номер 19(31)

Опубликована: Апрель 8, 2023

Abstract Carbon dots (CDs) with good water solubility and biocompatibility have become a research hotspot in the nano‐enzyme biomedical field. However, problems of low catalytic activity ambiguous site CDs as nanozymes still need to be addressed. In this work, loaded Cu single atoms are obtained through pyrolysis, coordination structure surface functional groups regulated by adjusting pyrolysis temperature. at 300 °C (named Cu‐CDs‐300) most carboxyl content is coordinated form CuN 2 O , which can better decompose H produce free radical beneficial catalyze oxidation 3,3′,5,5′‐tetramethylbenzidine (TMB). The v max 6.56*10 −7 m s −1 6.56 times higher than that horseradish peroxidase (HRP). Moreover, Cu‐CDs‐300 effectively lead CT26 apoptosis generating much radicals. This work demonstrates synergistic effect oxygen‐containing metal structures on peroxide‐like provides new ideas for design clear active high efficiency atom catalyst.

Язык: Английский

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Enabling Broader Adoption of Biocatalysis in Organic Chemistry

JACS Au, Год журнала: 2023, Номер 3(8), С. 2073 - 2085

Опубликована: Июль 19, 2023

Biocatalysis is becoming an increasingly impactful method in contemporary synthetic chemistry for target molecule synthesis. The selectivity imparted by enzymes has been leveraged to complete previously intractable chemical transformations and improve routes toward complex molecules. However, the implementation of biocatalysis mainstream organic gradual this point. This partly due a set historical technological barriers that have prevented chemists from using as tool with utility parallels alternative modes catalysis. In Perspective, we discuss these how they hindered adoption enzyme catalysts into strategies. We also summarize tools resources already enable use biocatalysts. Furthermore, ways further lower broader community through dissemination resources, demystifying biocatalytic reactions, increasing collaboration across field.

Язык: Английский

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The Transformative Power of Biocatalysis in Convergent Synthesis

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(12), С. 5214 - 5225

Опубликована: Март 15, 2022

Achieving convergent synthetic strategies has long been a gold standard in constructing complex molecular skeletons, allowing for the rapid generation of complexity comparatively streamlined routes. Traditionally, biocatalysis not played prominent role laboratory synthesis, with application biocatalysts primarily limited to synthesis chiral fragments. Although use enzymes enable approaches is relatively new and emerging, combining efficiency transformations selectivity achievable through creates opportunities efficient strategies. This Perspective provides an overview recent developments biocatalytic offers insights into advantages these methods compared their small molecule-based counterparts.

Язык: Английский

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