Unusually long polymers crosslinked by domains of physical bonds

Polymers crosslinked by covalent bonds suffer from a conflict: dense covalent crosslinks increase modulus but decrease fatigue threshold. Polymers crosslinked by physical bonds commonly have large hysteresis. Here we simultaneously achieve high modulus, high fatigue threshold, and low hysteresis in a network of unusually long polymer chains crosslinked by domains of physical bonds. When the network without precrack is pulled by a moderate stress, chains in the domains slip negligibly, so that the domains function like hard particles, leading to high modulus and low hysteresis. When the network with a precrack is stretched, the chains in the domains at the crack tip slip but do not pull out. This enables high tension to transmit over long segments of chains, leading to a high fatigue threshold.

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Publication Details

Journal
Nature Communications
Published
2025-05-22
DOI
https://doi.org/10.1038/s41467-025-59875-z
Citations
30
Primary Topic
Hydrogels: synthesis, properties, applications
Type
article
Field-Weighted Citation Impact
17.74

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article

Unusually long polymers crosslinked by domains of physical bonds

Zhigang Suo, Christine Heera Ahn, Xianyang Bao, Yakov Kutsovsky et al.
30 citations
Nature Communications
Hydrogels: synthesis, properties, applications
17.74
article

Unusually long polymers crosslinked by domains of physical bonds

Zhigang Suo, Christine Heera Ahn, Xianyang Bao, Yakov Kutsovsky, Zheqi Chen, Guodong Nian, Matthew Tan
article en
30 citations

Abstract

Polymers crosslinked by covalent bonds suffer from a conflict: dense covalent crosslinks increase modulus but decrease fatigue threshold. Polymers crosslinked by physical bonds commonly have large hysteresis. Here we simultaneously achieve high modulus, high fatigue threshold, and low hysteresis in a network of unusually long polymer chains crosslinked by domains of physical bonds. When the network without precrack is pulled by a moderate stress, chains in the domains slip negligibly, so that the domains function like hard particles, leading to high modulus and low hysteresis. When the network with a precrack is stretched, the chains in the domains at the crack tip slip but do not pull out. This enables high tension to transmit over long segments of chains, leading to a high fatigue threshold.

Nature CommunicationsVol. 16(1)
Harvard University (US), Nanyang Technological University (SG), Harvard University Press (US), Zhejiang University (CN)
National Science Foundation, Ministry of Education - Singapore, Nanyang Technological University, Materials Research Science and Engineering Center, Harvard University, Division of Materials Research, Air Force Office of Scientific Research
Openalex Percentile: Top 0%
Hydrogels: synthesis, properties, applications
17.74
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Unusually long polymers crosslinked by domains of physical bonds — Zhigang Suo, Christine Heera Ahn, et al. · Nature Communications (2025) | TGRS Research Map | TGRS