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Allosteric release of cucurbit[6]uril from a rotaxane using a molecular signal.
Chem Sci
December 2024
Department of Chemistry, Faculty of Technology, Tomas Bata University in Zlín Vavrečkova 5669 760 01 Zlín Czech Republic
Rotaxanes can be regarded as storage systems for their wheel components, which broadens their application potential as a complement to the supramolecular systems that retain a mechanically interlocked structure. However, utilising rotaxanes in this way requires a method to release the wheel while preserving the integrity of all molecular constituents. Herein, we present simple rotaxanes based on cucurbit[6]uril (CB6), with an axis equipped with an additional binding motif that enables the binding of another macrocycle, cucurbit[7]uril (CB7).
View Article and Find Full Text PDFMechanistic basis for the allosteric activation of NADase activity in the Sir2-HerA antiphage defense system.
Nat Commun
October 2024
Kev Laboratory of Microbial Pathogenesis and Interventions of Fuian Province University, the Key Laboratory of inmate lmmune Biology of Fuijian Province, Biomedical Research Center of South China, Key Laboratory of Opto Electronic Science and Technology for Medicine of the Ministry of Education, College of Life Sciences, Fujian Normal University, Fuzhou, 350117, China.
Article Synopsis
- Sir2-HerA is an antiphage system found in some bacteria, composed of an ATPase (HerA) and an effector (Sir2) that may have NADase activity.
- The mechanism of how Sir2-HerA defends against phage infections involves Sir2-dependent NAD depletion, which halts the growth of infected cells, but specifics were unclear until this study.
- Researchers discovered that SaHerA activates SaSir2’s NADase function through allosteric effects, leading to the formation of a complex that allows NAD to be cleaved by uncovering its active site.
Anion Recognition-Directed Supramolecular Catalysis with Functional Macrocycles and Molecular Cages.
Acc Chem Res
November 2024
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Molecular Recognition and Function, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Article Synopsis
- The text discusses the advancements in supramolecular chemistry, particularly focusing on how host molecules and noncovalent interactions can enhance catalytic processes through supramolecular catalysis.
- It highlights the significance of macrocyclic and cage-like compounds which mimic enzymes and possess unique recognition features, emphasizing the underutilization of directional binding sites in traditional host molecules.
- The study introduces a novel approach using tailor-made functionalized macrocycles and cages specifically designed for anion recognition, which enhances catalytic efficiency and stereocontrol in reactions by leveraging strong anion binding and cooperative interactions.
Ternary π-π Stacking Complexes by Allosteric Regulation in Multilayer Nanographenes.
J Am Chem Soc
October 2024
Institut für Organische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany.
Construction of π-π stacking supramolecular complexes with more than two different components is challenging due to the weak and directionless nature of dispersion interactions. Here, we report ternary complexes of a ditopic nanographene tetraimide (), α-substituted phthalocyanine (), and polyaromatic hydrocarbons (PAHs) in solution and the crystalline state via allosteric regulation. Binding of one gives rise to significant distortion and conformational changes in that in turn lead to the inhibition of the second binding of .
View Article and Find Full Text PDFAllosteric Control of the Catalytic Properties of Dipeptide-Based Supramolecular Assemblies.
J Am Chem Soc
August 2024
Department of Chemical Sciences and Centre for Advanced Functional Materials, Indian Institute of Science Education and Research (IISER) Kolkata, Mohanpur 741246, India.
Allostery, as seen in extant biology, governs the activity regulation of enzymes through the redistribution of conformational equilibria upon binding an effector. Herein, a minimal design is demonstrated where a dipeptide can exploit dynamic imine linkage to condense with simple aldehydes to access spherical aggregates as catalytically active states, which facilitates an orthogonal reaction due to the closer proximity of catalytic residues (imidazoles). The allosteric site (amine) of the minimal catalyst can concomitantly bind to an inhibitor via a dynamic exchange, which leads to the alternation of the energy landscape of the self-assembled state, resulting in downregulation of catalytic activity.
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