We report on a rotaxane-like architecture secured by the in situ tying of an overhand knot in the tris(2,6-pyridyldicarboxamide) region of the axle through complexation with a lanthanide ion (Lu ). The increase in steric bulk caused by the knotting locks a crown ether onto the thread. Removal of the lutetium ion unties the knot, and when the axle binding site for the ring is deactivated, the macrocycle spontaneously dethreads. When the binding interaction is switched on again, the crown ether rethreads over the 10 nm length of the untangled strand. The overhand knot can be retied, relocking the threaded structure, by once again adding lutetium ions.
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http://dx.doi.org/10.1002/anie.201803871 | DOI Listing |
Front Robot AI
August 2024
Automatic Control and Systems Engineering, The University of Sheffield, Sheffield, United Kingdom.
Transforming planar structures into volumetric objects typically requires manual folding processes, akin to origami. However, manual intervention at sub-centimeter scales is impractical. Instead, folding is achieved using volume-changing smart materials that respond to physical or chemical stimuli, be it with direct contact such as hydration, pH, or remotely e.
View Article and Find Full Text PDFJ Phys Chem Lett
September 2024
Institute for Computational Molecular Science, Temple University, Philadelphia, Pennsylvania 19122, United States.
A neural network potential (NNP) has been developed by fitting to ab initio electronic structure data on hydrocarbons and is used to study failure of linear and knotted polyethylene (PE) chains. A linear PE chain must be highly strained before breaking as the stress is equally distributed across the chain. In contrast, the stress in a PE chain with a 3 or overhand knot, accumulates at the knot's entrance/exit.
View Article and Find Full Text PDFJ Am Chem Soc
August 2024
School of Chemistry and Molecular Engineering, East China Normal University, 200062 Shanghai, China.
J Orthop Res
November 2024
Department of Orthopedic Surgery, Orthopedic Biomechanics Research Laboratory, Mayo Clinic Rochester, Rochester, Minnesota, USA.
Nat Chem
August 2024
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, China.
Molecular knots and entanglements form randomly and spontaneously in both biological and synthetic polymer chains. It is known that macroscopic materials, such as ropes, are substantially weakened by the presence of knots, but until now it has been unclear whether similar behaviour occurs on a molecular level. Here we show that the presence of a well-defined overhand knot in a polymer chain substantially increases the rate of scission of the polymer under tension (≥2.
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