Stacked or folded? impact of chelate cooperativity on the self-assembly pathway to helical nanotubes from dinucleobase monomers
Entity
UAM. Departamento de Química OrgánicaPublisher
American Chemical SocietyDate
2023-08-02Citation
10.1021/jacs.3c04773
Journal of the American Chemical Society 145.232 (2023): 17805–17818
ISSN
0002-7863 (print); 1520-5126 (online)DOI
10.1021/jacs.3c04773Funded by
Funding from the European Research Council (ERC-Starting Grant 279548 PROGRAM-NANO) MCIN (RED2018- 102331-T, PID2020-116921GB-I00, and TED2021-132602BI00), the Italian Ministry of Education, University and Research (PRIN project prot. 2017A4XRCA_003), the Ministry of Education, Youth, and Sports of the Czech Republic (CZ.02.1.01/0.0/0.0/16_019/0000754, e-INFRA CZ (ID:90254)), the Swedish Research Council (2018- 4343), and the Swedish e-Science Research Centre (SeRC) is gratefully acknowledged. The authors also acknowledge the provision of supercomputer resources from the Swedish National Infrastructure for Computing (SNIC). F.A. is grateful to MCIN and Next Generation EU funding for a “Ramon-yCajal” fellowship (RyC-2021-031538-I). A.dJ. is grateful to EU funding from a MSCA-IEF action (897507-SuprAlloCat)Project
info:eu-repo/grantAgreement/EC/PROGRAM-NANO/279548; Gobierno de España. RED2018-102331-T; info:eu-repo/grantAgreement/EC/SuprAlloCat/ES/897507Editor's Version
https://doi.org/10.1021/jacs.3c04773Subjects
QuímicaRights
© 2023 The AuthorsAbstract
Self-assembled nanotubes exhibit impressive biological functions that have always inspired supramolecular scientists in their efforts to develop strategies to build such structures from small molecules through a bottom-up approach. One of these strategies employs molecules endowed with self-recognizing motifs at the edges, which can undergo either cyclization-stacking or folding-polymerization processes that lead to tubular architectures. Which of these self-assembly pathways is ultimately selected by these molecules is, however, often difficult to predict and even to evaluate experimentally. We show here a unique example of two structurally related molecules substituted with complementary nucleobases at the edges (i.e., G:C and A:U) for which the supramolecular pathway taken is determined by chelate cooperativity, that is, by their propensity to assemble in specific cyclic structures through Watson-Crick pairing. Because of chelate cooperativities that differ in several orders of magnitude, these molecules exhibit distinct supramolecular scenarios prior to their polymerization that generate self-assembled nanotubes with different internal monomer arrangements, either stacked or coiled, which lead at the same time to opposite helicities and chiroptical properties
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Google Scholar:González Sánchez, Marina
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Mayoral, María J.
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Vázquez González, Violeta
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Paloncýová, Markéta
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Sancho Casado, Irene
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Aparicio Hernández, Fátima
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Juan Garrudo, Alberto de
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Longhi, Giovanna
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Norman, Patrick
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Linares, Mathieu
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González Rodríguez, David
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