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解锁手性超分子螺旋聚合物的生物界面

Unlocking a Biological Interface of Chiral Supramolecular Helical Polymers.

作者信息

Alcalde-Ordóñez Ana, Sarmiento Axel, Gómez-González Jacobo, Bouzada David, Núñez-Martínez Manuel, Fernández-Míguez Manuel, Rodríguez Rafael, Freire Félix, Vázquez M Eugenio, Vázquez López Miguel

机构信息

Departamento de Química Inorgánica, Universidade de Santiago de Compostela, Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS), Rúa Jenaro de la Fuente s/n, 15782 Santiago de Compostela, Spain.

Departamento de Química Orgánica, Universidade de Santiago de Compostela, Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS), Rúa Jenaro de la Fuente s/n, 15782 Santiago de Compostela, Spain.

出版信息

J Am Chem Soc. 2025 Jul 23;147(29):25254-25263. doi: 10.1021/jacs.5c02902. Epub 2025 Jun 9.

DOI:10.1021/jacs.5c02902
PMID:40491063
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12291456/
Abstract

Here we report a C-symmetric metal-binding tripeptide, , that self-assembles in water into either a chiral supramolecular helical polymer or a discrete Co peptide helicate, depending on metal coordination. The Co peptide helicate exhibits high affinity and selectivity toward DNA three-way junctions (3WJ), a class of noncanonical DNA structures with emerging biological relevance. Importantly, we demonstrate that the recognition process can be triggered dynamically by adding Co ions to a dispersion of the supramolecular polymer, which acts as an inert precursor reservoir in physiological media. In this way, our strategy shows that chiral supramolecular helical polymers can form temporarily inactive aggregates that release discrete helicates for biomolecular recognition, such as 3WJ binding, upon metal ion coordination. Overall, this mechanism reveals a previously unexplored capability of this class of materials and offers a new approach for the design of responsive supramolecular systems for nucleic acid recognition and anticancer therapy.

摘要

在此，我们报道了一种C对称金属结合三肽，其在水中根据金属配位情况自组装成手性超分子螺旋聚合物或离散的钴肽螺旋配合物。钴肽螺旋配合物对DNA三链体（3WJ）表现出高亲和力和选择性，3WJ是一类具有新兴生物学相关性的非经典DNA结构。重要的是，我们证明了通过向超分子聚合物分散体中添加钴离子可以动态触发识别过程，该超分子聚合物在生理介质中充当惰性前体库。通过这种方式，我们的策略表明手性超分子螺旋聚合物可以形成暂时无活性的聚集体，在金属离子配位时释放离散的螺旋配合物用于生物分子识别，如3WJ结合。总体而言，这种机制揭示了这类材料以前未被探索的能力，并为设计用于核酸识别和抗癌治疗的响应性超分子系统提供了一种新方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/285d357c8098/ja5c02902_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/2e44ce1156ad/ja5c02902_0001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/c71301098e62/ja5c02902_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/d5ff53709aa4/ja5c02902_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/62a6b956e31d/ja5c02902_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/285d357c8098/ja5c02902_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/2e44ce1156ad/ja5c02902_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/243006eb42f7/ja5c02902_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/b7a3683823f1/ja5c02902_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/c71301098e62/ja5c02902_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/d5ff53709aa4/ja5c02902_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/62a6b956e31d/ja5c02902_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e3f2/12291456/285d357c8098/ja5c02902_0006.jpg

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本文引用的文献

1
Bottom-up construction of chiral metal-peptide assemblies from metal cluster motifs.从金属团簇基元出发，通过自下而上的方法构建手性金属-肽组装体。
Nat Commun. 2024 Oct 19;15(1):9034. doi: 10.1038/s41467-024-53320-3.
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Stimuli-responsive synthetic helical polymers.刺激响应性合成螺旋聚合物
Chem Soc Rev. 2024 Jan 22;53(2):793-852. doi: 10.1039/d3cs00952a.
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A copper(ii) peptide helicate selectively cleaves DNA replication foci in mammalian cells.一种铜（II）肽螺旋体可选择性地切割哺乳动物细胞中的DNA复制位点。
Chem Sci. 2023 Oct 27;14(48):14082-14091. doi: 10.1039/d3sc03303a. eCollection 2023 Dec 13.
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Screw sense and screw sensibility: communicating information by conformational switching in helical oligomers.拧转理智，拧转感知：通过螺旋寡聚物的构象转变来传递信息。
Chem Soc Rev. 2023 Apr 3;52(7):2480-2496. doi: 10.1039/d2cs00982j.
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Selective recognition of A/T-rich DNA 3-way junctions with a three-fold symmetric tripeptide.利用具有三重对称性的三肽对富含A/T的DNA三向接头进行选择性识别。
Chem Commun (Camb). 2022 Jul 12;58(56):7769-7772. doi: 10.1039/d2cc02874c.
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Solvent Drives Switching between Λ and Δ Metal Center Stereochemistry of ML Cubic Cages.溶剂驱动 ML 立方笼中金属中心 Λ 和 Δ 立体化学的转变。
J Am Chem Soc. 2022 Apr 13;144(14):6136-6142. doi: 10.1021/jacs.2c00245. Epub 2022 Apr 1.
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DNA folds threaten genetic stability and can be leveraged for chemotherapy.DNA折叠会威胁基因稳定性，可用于化疗。
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Stereoselective Self-Assembly of DNA Binding Helicates Directed by the Viral β-Annulus Trimeric Peptide Motif.手性选择性 DNA 结合螺旋体的自组装由病毒 β-环三聚肽基序指导。
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Dynamic Stereoselection of Peptide Helicates and Their Selective Labeling of DNA Replication Foci in Cells*.动态立体选择性肽螺旋及其对细胞中 DNA 复制焦点的选择性标记*。
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