Citation: Chengyuan Yu, Huiyao Lin, Le Li, Ruirui Gu, Qi Zhang, Chenyu Shi, Chenchen Zhang, Fei Tong. Ion-cluster-optimized microphase separation in shape-memory polydisulfides for enhanced mechanical performance[J]. Chinese Chemical Letters, ;2026, 37(2): 111946. doi: 10.1016/j.cclet.2025.111946 shu

Ion-cluster-optimized microphase separation in shape-memory polydisulfides for enhanced mechanical performance

Chengyuan Yu ^{a, b, 1,*,} ,
Huiyao Lin ^{a, 1} ,
Le Li ^a ,
Ruirui Gu ^a ,
Qi Zhang ^a ,
Chenyu Shi ^a ,
Chenchen Zhang ^a ,
Fei Tong ^{a, *,}

a.
Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China
b.
Strait Institute of Flexible Electronics (SIFE, Future Technologies), Fujian Key Laboratory of Flexible Electronics, Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE), Fuzhou 350117, China

ifechyyu@fjnu.edu.cn

feitong@ecust.edu.cn

Received Date: 12 June 2025
Revised Date: 8 October 2025
Accepted Date: 12 October 2025
Available Online: 12 October 2025

Figures(4)

Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science. Recently, supramolecular polymeric materials (SPMs) have drawn increased attention due to their unique properties and potential applications in self-healing, shape memory, sensors, and flexible electronics. Here, we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers. The mechanical properties, including Young’s modulus and toughness, are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone (UPy) induced microphase separation with iron(Ⅲ)-to-carboxylate ionic clusters. By combining established chemical approaches with adjustable polymer phase ratios, it is revealed that the synergistic effect of these factors expands the interchain spacing, facilitates the formation of microphase domains, and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli, meeting the practical requirements for industrial plastic applications. Moreover, the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature. Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.
- Polydisulfides,
- Network toughening,
- Ionic clusters,
- Microphase separation,
- Shape-memory supramolecular polymers
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