Abstract

Combining coordination chemistry and peptide engineering offers extraordinary opportunities for developing novel molecular (supra)structures. Here, we demonstrate that the β-annulus motif is capable of directing the stereoselective assembly of designed peptides containing 2,2′-bipyridine ligands into parallel three-stranded chiral peptide helicates, and that these helicates selectively bind with high affinity to three-way DNA junctions.

Highlights

  • Peptides are ideal platforms for the programmed assembly of supramolecular structures, as they encode in their sequences precise structural and functional information in their sequence

  • One of the biggest challenges for the synthesis of helicates is their stereoselective assembly with controlled supramolecular chirality.[31−34] In this context, we wanted to test whether a small trimeric peptide motif could effectively control the selfassembly of three-stranded peptide helicates, selecting a particular orientation of the ligand chains and helical chirality

  • In contrast to our previous approach to helicate synthesis relying on the folding of a single peptide chain,[35,36] here we would rely on the assembly of three independent peptide monomers to template the formation of the desired helicate

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Summary

■ ACKNOWLEDGMENTS

Financial support from the Spanish grant RTI2018-099877-BI00, the Xunta de Galicia (Centro singular de Investigación de Galicia accreditation 2016−2019, ED431G/09, and ED431B 2018/04), and the European Union (European Regional Development Fund - ERDF) is gratefully acknowledged. J.G.G. thanks the Spanish MINECO for his FPI fellowship. D.B. thanks the CIQUS for his 2018 PhD fellowship. G.S. and J.D.M. thank Spanish MINECO (grant CTQ2017-87889-P) and Generalitat de Catalunya (2017SGR1323) for the financial support. Kazunori Matsuura at Tottori University for his valuable input during the preparation of this manuscript

■ REFERENCES
Supramolecular Cylinders Prescribe Helicity and Enhance DNA
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