Highly robust supramolecular polymer networks crosslinked by a tiny amount of metallacycles

Lang He, Yu Jiang, Jialin Wei, Zibin Zhang, Tao Hong, Zhiqiang Ren, Jianying Huang (), Feihe Huang (), Peter J. Stang () and Shijun Li ()
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Lang He: Hangzhou Normal University
Yu Jiang: Zhejiang Gongshang University
Jialin Wei: Hangzhou Normal University
Zibin Zhang: Hangzhou Normal University
Tao Hong: Zhejiang Gongshang University
Zhiqiang Ren: Peking University
Jianying Huang: Zhejiang Gongshang University
Feihe Huang: Zhejiang University
Peter J. Stang: University of Utah
Shijun Li: Hangzhou Normal University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Supramolecular polymeric materials have exhibited attractive features such as self-healing, reversibility, and stimuli-responsiveness. However, on account of the weak bonding nature of most noncovalent interactions, it remains a great challenge to construct supramolecular polymeric materials with high robustness. Moreover, high usage of supramolecular units is usually necessary to promote the formation of robust supramolecular polymeric materials, which restrains their applications. Herein, we describe the construction of highly robust supramolecular polymer networks by using only a tiny amount of metallacycles as the supramolecular crosslinkers. A norbornene ring-opening metathesis copolymer with a 120° dipyridine ligand is prepared and self-assembled with a 60° or 120° Pt(II) acceptor to fabricate the metallacycle-crosslinked polymer networks. With only 0.28 mol% or less pendant dipyridine units to form the metallacycle crosslinkers, the mechanical properties of the polymers are significantly enhanced. The tensile strengths, Young’s moduli, and toughness of the reinforced polymers reach up to more than 20 MPa, 600 MPa, and 150 MJ/m3, respectively. Controllable destruction and reconstruction of the metallacycle-crosslinked polymer networks are further demonstrated by the sequential addition of tetrabutylammonium bromide and silver triflate, indicative of good stimuli-responsiveness of the networks. These remarkable performances are attributed to the thermodynamically stable, but dynamic metallacycle-based supramolecular coordination complexes that offer strong linkages with good adaptive characteristics.

Date: 2024
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DOI: 10.1038/s41467-024-47333-1

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