New-to-nature chemistry from old protein machinery: carbene and nitrene transferases

Current Opinion in Biotechnology, Journal Year: 2020, Volume and Issue: 69, P. 43 - 51

Published: Dec. 25, 2020

Language: Английский

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Mimicking Enzymes: The Quest for Powerful Catalysts from Simple Molecules to Nanozymes

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(18), P. 11501 - 11509

Published: Sept. 5, 2021

ADVERTISEMENT RETURN TO ISSUEViewpointNEXTMimicking Enzymes: The Quest for Powerful Catalysts from Simple Molecules to NanozymesYanchao LyuYanchao LyuUniversity of Padova, Department Chemical Sciences, via Marzolo, 1, 35131 ItalyMore by Yanchao Lyu and Paolo Scrimin*Paolo ScriminUniversity Italy*Email P.S.: [email protected]More Scriminhttps://orcid.org/0000-0002-6741-3374Cite this: ACS Catal. 2021, 11, 18, 11501–11509Publication Date (Web):September 5, 2021Publication History Received16 March 2021Published online5 September inissue 17 2021https://pubs.acs.org/doi/10.1021/acscatal.1c01219https://doi.org/10.1021/acscatal.1c01219article-commentaryACS PublicationsCopyright © 2021 Authors. Published American Society. This publication is licensed under CC-BY 4.0. License Summary*You are free share (copy redistribute) this article in any medium or format adapt (remix, transform, build upon) the material purpose, even commercially within parameters below:Creative Commons (CC): a Creative license.Attribution (BY): Credit must be given creator.View full license*DisclaimerThis summary highlights only some key features terms actual license. It not license has no legal value. Carefully review before using these materials. Open Access indicated. Learn MoreACS Editors' Choice® collection designed feature scientific articles broad public interest. Read latest articlesArticle Views16469Altmetric-Citations31LEARN ABOUT THESE METRICSArticle Views COUNTER-compliant sum text downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other citing article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score quantitative measure attention that research received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail (1005 KB) Get e-AlertscloseSUBJECTS:Catalysts,Ions,Metal nanoparticles,Metals,Peptides proteins e-Alerts

Language: Английский

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Intracellular Reactions Promoted by Bis(histidine) Miniproteins Stapled Using Palladium(II) Complexes

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(23), P. 9149 - 9154

Published: March 12, 2020

The generation of catalytically active metalloproteins inside living mammalian cells is a major research challenge at the interface between catalysis and cell biology. Herein we demonstrate that basic domains bZIP transcription factors, mutated to include two histidine residues i i+4 positions, react with palladium(II) sources generate active, stapled pallado-miniproteins. resulting constrained peptides are efficiently internalized into cells, where they perform palladium-promoted depropargylation reactions without cellular fixation. Control experiments confirm requirement peptide scaffolding palladium staple for attaining intracellular reactivity.

Language: Английский

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The Time and Place for Nature in Drug Discovery

JACS Au, Journal Year: 2022, Volume and Issue: 2(11), P. 2400 - 2416

Published: Oct. 14, 2022

The case for a renewed focus on Nature in drug discovery is reviewed; not terms of natural product screening, but how and why biomimetic molecules, especially those produced by processes, should deliver the age artificial intelligence screening vast collections both vitro silico. declining product-likeness licensed drugs consequent physicochemical implications this trend context current practices are noted. To arrest these trends, logic seeking new bioactive agents with enhanced mimicry considered; notably that molecules constructed proteins (enzymes) more likely to interact other (e.g., targets transporters), notion validated products. Nature's finite number building blocks their interactions necessarily reduce potential numbers structures, yet enable expansion chemical space inherent diversity physical characteristics, pertinent property-based design. feasible variations motifs considered expanded encompass pseudo-natural products, leading further logical step harnessing bioprocessing routes access them. Together, offer opportunities enhancing mimicry, thereby bringing innovation synthesis exploiting characteristics recognition processes. computational guidance help identifying binding commonalities route map opportunity design tailored "organic/biological" rather than purely "synthetic" structures. prototype structures pay dividends disposition efficacy while inherently enabling greener sustainable manufacturing techniques.

Language: Английский

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Synthetic prodrug design enables biocatalytic activation in mice to elicit tumor growth suppression

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

Published: Jan. 10, 2022

Considering the intrinsic toxicities of transition metals, their incorporation into drug therapies must operate at minimal amounts while ensuring adequate catalytic activity within complex biological systems. As a way to address this issue, study investigates design synthetic prodrugs that are not only tuned be harmless, but can robustly transformed in vivo reach therapeutically relevant levels. To accomplish this, retrosynthetic prodrug highlights potential naphthylcombretastatin-based prodrugs, which form highly active cytostatic agents via sequential ring-closing metathesis and aromatization. Structural adjustments will also done improve aspects related reactivity, bioactivity, hydrolytic stability. The developed therapy is found possess excellent anticancer activities cell-based assays. Furthermore, activation by intravenously administered glycosylated artificial metalloenzymes induce significant reduction implanted tumor growth mice.

Language: Английский

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Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

Topics in Catalysis, Journal Year: 2022, Volume and Issue: 65(1-4), P. 6 - 39

Published: Jan. 13, 2022

Autonomous computations that rely on automated reaction network elucidation algorithms may pave the way to make computational catalysis a par with experimental research in field. Several advantages of this approach are key catalysis: (i) Automation allows one consider orders magnitude more structures systematic and open-ended fashion than what would be accessible by manual inspection. Eventually, full resolution terms structural varieties conformations as well respect type number potentially important elementary steps (including decomposition reactions determine turnover numbers) achieved. (ii) Fast electronic structure methods uncertainty quantification warrant high efficiency reliability order not only deliver results quickly, but also allow for predictive work. (iii) A degree autonomy reduces amount human work, processing errors, bias. Although being inherently unbiased, it is still steerable specific regions an emerging addition new reactant species. This fidelity formalization some catalytic process surprising silico discoveries. In we first review state art embed autonomous explorations into general field from which draws its ingredients. We then elaborate conceptual issues arise context procedures, discuss at example system.

Language: Английский

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Hydrolase mimic via second coordination sphere engineering in metal-organic frameworks for environmental remediation

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 25, 2023

Enzymes achieve high catalytic activity with their elaborate arrangements of amino acid residues in confined optimized spaces. Nevertheless, when exposed to complicated environmental implementation scenarios, including acidity, organic solvent and ionic strength, enzymes exhibit low operational stability poor activity. Here, we report a metal-organic frameworks (MOFs)-based artificial enzyme system via second coordination sphere engineering hydrolytic under mild conditions. Experiments theoretical calculations reveal that amide cleavage catalyzed by MOFs follows two distinct mechanisms, Lewis acid- hydrogen bonding-mediated processes. The bond formed the secondary exhibits 11-fold higher than acidic zinc ions. satisfactory degradation performance toxins extreme working conditions, fermentation broth ethanol environments, display broad substrate specificity. These findings hold great promise for designing remediation.

Language: Английский

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Artificial metalloenzyme assembly in cellular compartments for enhanced catalysis

Nature Chemical Biology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Language: Английский

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Bridging the gap between theory and treatment: Transition metal complexes as successful candidates in medicine

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 531, P. 216477 - 216477

Published: Feb. 8, 2025

Language: Английский

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Controlling the optical and catalytic properties of artificial metalloenzyme photocatalysts using chemogenetic engineering

Chemical Science, Journal Year: 2022, Volume and Issue: 13(5), P. 1459 - 1468

Published: Jan. 1, 2022

Artificial metalloenzyme visible light photocatalysts possess enhanced optical properties and are competent towards single electron energy transfer organic transformations.

Language: Английский

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