Metal-peptide rings form highly entangled topologically inequivalent frameworks with the same ring- and crossing-numbers

Nature Communications
Tomohisa SawadaMakoto Fujita

Abstract

With increasing ring-crossing number (c), knot theory predicts an exponential increase in the number of topologically different links of these interlocking structures, even for structures with the same ring number (n) and c. Here, we report the selective construction of two topologies of 12-crossing peptide [4]catenanes (n = 4, c = 12) from metal ions and pyridine-appended tripeptide ligands. Two of the 100 possible topologies for this structure are selectively created from related ligands in which only the tripeptide sequence is changed: one catenane has a T2-tetrahedral link and the other a three-crossed tetrahedral link. Crystallographic studies illustrate that a conformational difference in only one of the three peptide residues in the ligand causes the change in the structure of the final tetrahedral link. Our results thus reveal that peptide-based folding and assembly can be used for the facile bottom-up construction of 3D molecular objects containing polyhedral links.

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Citations

Nov 7, 2019·Chemistry : a European Journal·Guo-Xin JinSaud I Al-Resayes
Dec 14, 2019·Nature Communications·Tomohisa SawadaMakoto Fujita
Sep 2, 2020·Acta Crystallographica. Section A, Foundations and Advances·Michael O'Keeffe, Michael M J Treacy
Apr 30, 2019·Chemistry : a European Journal·Guo-Xin JinYue-Jian Lin
Nov 26, 2020·Journal of Materials Chemistry. B, Materials for Biology and Medicine·Zhonghui ChenZhenguo Chi
Jul 29, 2021·Bioconjugate Chemistry·Jacobo Gómez-GonzálezM Eugenio Vázquez
Aug 3, 2021·Journal of the American Chemical Society·Ye LuGuo-Xin Jin
May 24, 2019·Journal of the American Chemical Society·Wen-Xi GaoGuo-Xin Jin
Oct 1, 2020·Inorganic Chemistry·Prodip HowladerPartha Sarathi Mukherjee
Dec 29, 2020·The Journal of Physical Chemistry Letters·Carlos-Andres Palma
Jun 20, 2020·Chemical Reviews·Wen-Xi GaoGuo-Xin Jin
Oct 5, 2021·Journal of the American Chemical Society·Yuuki InomataMakoto Fujita
Oct 28, 2021·Chemical Reviews·Alexander V VirovetsManfred Scheer

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Methods Mentioned

BETA
peptide folding
X-ray
NMR
size-exclusion chromatography

Software Mentioned

SHELX
TwinRotMat
TL
SHELXL
PLATON
SHELXS
PyMOL

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