Early View e202510140
Forschungsartikel

Synergistic Covalently and Mechanically Interlocked Polymer

Yi Ding

Yi Ding

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Yuanhao Wang

Yuanhao Wang

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Changyao Liu

Changyao Liu

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Jingxi Deng

Jingxi Deng

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Shaolei Qu

Shaolei Qu

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Dr. Yongming Wang

Dr. Yongming Wang

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Dr. Ruixue Bai

Dr. Ruixue Bai

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Yuhang Liu

Yuhang Liu

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Guoquan Liu

Guoquan Liu

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Chuan Yue

Chuan Yue

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Prof. Wei Yu

Prof. Wei Yu

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

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Dr. Zhaoming Zhang

Corresponding Author

Dr. Zhaoming Zhang

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

E-mail: [email protected]; [email protected]

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Prof. Xuzhou Yan

Corresponding Author

Prof. Xuzhou Yan

State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P.R. China

E-mail: [email protected]; [email protected]

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First published: 21 July 2025

Abstract

Integrating different polymer types into a unified system in a thoughtful manner leverages their complementary advantages, providing a promising strategy for developing high-performance materials. Mechanically interlocked polymers (MIPs), characterized by their unique spatial entanglement, exhibit distinctive performance advantages, yet their potential to expand material properties through rational integration with other polymer architectures presents substantial opportunities for continued investigation. Herein, we report a coherent integration of covalent polymers (CPs) and mechanically interlocked polymers through sequential orthogonal polymerizations, developing a novel synergistic covalently and mechanically interlocked polymer (CMIP) featuring both structural stability and force-induced dynamics. Compared to its structurally similar but noninterlocked control sample, CMIP demonstrates markedly enhanced thermomechanical stability and performance recovery, achieving a 93.4% recovery efficiency at 100% strain after just 5 min of rest, in contrast to 59.7% for the control. This remarkable stability and recovery result from the synergistic interplay between the covalent polymer framework and the interlocked structure, which work in tandem to preserve network integrity and enable rapid host−guest reformation. Notably, despite this significant improvement, CMIP retains a comparable damping capacity (91% versus 87%) and material toughness (14.8 versus 15.1 MJ m−3), owing to the efficient energy dissipation mechanisms enabled by host−guest dissociation and subsequent sliding motion. This strategy imparts CMIP with unique characteristics, offering a prospective pathway for the development of a diverse array of advanced synergistic materials with enhanced, multifaceted properties.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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