Where Chemocatalysis Meets Biocatalysis: In Water

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(9), P. 5262 - 5296

Published: Dec. 6, 2022

Chemoenzymatic catalysis, by definition, involves the merging of sequential reactions using both chemocatalysis and biocatalysis, typically in a single reaction vessel. A major challenge, solution to which, however, is associated with numerous advantages, run such one-pot processes water: majority enzyme-catalyzed take place water as Nature's medium, thus enabling broad synthetic diversity when due option use virtually all types enzymes. Furthermore, cheap, abundantly available, environmentally friendly, making it, principle, an ideal medium. On other hand, most routinely performed today organic solvents (which might deactivate enzymes), appearing make it difficult combine biocatalysis toward cascades water. Several creative approaches solutions that enable combinations chemo- be realized applied problems are presented herein, reflecting state-of-the-art this blossoming field. Coverage has been sectioned into three parts, after introductory remarks: (1) Chapter 2 focuses on historical developments initiated area research; (2) 3 describes key post-initial discoveries have advanced field; (3) 4 highlights latest achievements provide attractive main question compatibility between (used predominantly aqueous media) (that remains solvents), Chapters covering mainly literature from ca. 2018 present. 5 6 brief overview where field stands, challenges lie ahead, ultimately, prognosis looking future chemoenzymatic catalysis synthesis.

Language: Английский

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Biocatalysed synthesis planning using data-driven learning

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Feb. 18, 2022

Abstract Enzyme catalysts are an integral part of green chemistry strategies towards a more sustainable and resource-efficient chemical synthesis. However, the use biocatalysed reactions in retrosynthetic planning clashes with difficulties predicting enzymatic activity on unreported substrates enzyme-specific stereo- regioselectivity. As now, only rule-based systems support using biocatalysis, while initial data-driven approaches limited to forward predictions. Here, we extend reaction as well pathway prediction models based Molecular Transformer architecture biocatalysis. The knowledge is learned from extensive data set publicly available biochemical aid new class token scheme enzyme commission classification number, which captures catalysis patterns among different enzymes belonging same hierarchy. model (top-1 accuracy 49.6%), single-step round-trip 39.6%) curated made facilitate adoption design greener processes.

Language: Английский

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Expanding chemistry through in vitro and in vivo biocatalysis

Nature, Journal Year: 2024, Volume and Issue: 631(8019), P. 37 - 48

Published: July 3, 2024

Language: Английский

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Learning from Protein Engineering by Deconvolution of Multi‐Mutational Variants

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 17, 2024

Abstract This review analyzes a development in biochemistry, enzymology and biotechnology that originally came as surprise. Following the establishment of directed evolution stereoselective enzymes organic chemistry, concept partial or complete deconvolution selective multi‐mutational variants was introduced. Early experiments led to finding mutations can interact cooperatively antagonistically with one another, not just additively. During past decade, this phenomenon shown be general. In some studies, molecular dynamics (MD) quantum mechanics/molecular mechanics (QM/MM) computations were performed order shed light on origin non‐additivity at all stages an evolutionary upward climb. Data used construct unique multi‐dimensional rugged fitness pathway landscapes, which provide mechanistic insights different from traditional landscapes. Along related line, biochemists have long tested result introducing two point enzyme for reasons, followed by comparison respective double mutant so‐called cycles, showed only additive effects, but more recently also uncovered cooperative antagonistic non‐additive effects. We conclude suggestions future work, call unified overall picture epistasis.

Language: Английский

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The fourth wave of biocatalysis is approaching

Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences, Journal Year: 2017, Volume and Issue: 376(2110), P. 20170063 - 20170063

Published: Nov. 25, 2017

Biocatalysis has undergone a tremendous development in the past few years. A plethora of methods enable rather rapid tailored-design an enzyme for targeted reaction such as asymmetric synthesis chiral building block by combination information from sequence and structure databases with modern molecular biology high-throughput screening tools. Moreover, novel non-natural reactions could be implemented into protein scaffolds new classes are emerging, both broadening repertoire now available organic synthesis. Furthermore, impressive examples metabolic engineering-the several newly introduced steps microbial host-have been developed, paving way large-scale processes pharmaceuticals bulk chemicals. This contribution highlights recent developments this area points out future challenges.This article is part discussion meeting issue 'Providing sustainable catalytic solutions rapidly changing world'.

Language: Английский

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