Topological Structure Evolution of Polymer Network Based on Star-shaped Multi-armed Precursors

Hui Li; Zi-Jian Xue; Yao-Hong Xue; Yingxiang Li; Hong Liu

doi:10.1007/s10118-025-3324-8

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Topological Structure Evolution of Polymer Network Based on Star-shaped Multi-armed Precursors

RESEARCH ARTICLE | Updated：2025-07-15

- Topological Structure Evolution of Polymer Network Based on Star-shaped Multi-armed Precursors
- Chinese Journal of Polymer Science Vol. 43, Issue 7, Pages: 1240-1252(2025)
- Affiliations：
  
  a.School of Material Science and Engineering, Lanzhou University of Technology, Lanzhou 730050, China
  b.Key Laboratory of Theoretical Chemistry of Environment Ministry of Education, School of Environment, South China Normal University, Guangzhou 510006, China
  c.Information Science School, Guangdong University of Finance and Economics, Guangzhou 510320, China
- Author bio：
  
  yingxiangli@m.scnu.edu.cn
- Funds：
- DOI：10.1007/s10118-025-3324-8
  CLC：
- Received：03 December 2024，
  
  Revised：2025-02-08，
  
  Accepted：20 February 2025，
  
  Online First：15 April 2025，
  
  Published：01 July 2025
- Accepted：
Scan QR Code
Li, H.; Xue, Z. J.; Xue, Y. H.; Li, Y. X.; Liu, H. Topological structure evolution of polymer network based on star-shaped multi-armed precursors. Chinese J. Polym. Sci. 2025, 43, 1240–1252

Hui Li, Zi-Jian Xue, Yao-Hong Xue, et al. Topological Structure Evolution of Polymer Network Based on Star-shaped Multi-armed Precursors[J]. Chinese Journal of Polymer Science, 2025, 43(7): 1240-1252.
Li, H.; Xue, Z. J.; Xue, Y. H.; Li, Y. X.; Liu, H. Topological structure evolution of polymer network based on star-shaped multi-armed precursors. Chinese J. Polym. Sci. 2025, 43, 1240–1252 DOI： 10.1007/s10118-025-3324-8.

Hui Li, Zi-Jian Xue, Yao-Hong Xue, et al. Topological Structure Evolution of Polymer Network Based on Star-shaped Multi-armed Precursors[J]. Chinese Journal of Polymer Science, 2025, 43(7): 1240-1252. DOI： 10.1007/s10118-025-3324-8.

摘要

This research focuses on the structure characteristics of polymer networks

including the number

and size dispersity of loops. We note that polydispersity of loop sizes is universal. While the size distribution is primarily related to the functionality of precursors

with fewer precursor arms system exhibiting larger average loop sizes.

Abstract

The performance of polymer network

is directly determined by their structure. Understanding the network structure offers insights into optimizing material performance

such as elasticity

toughness

and swelling behavior. Herein

in this study we introduce the Dijkstra algorithm from graph theory to characterize polymer networks based on star-shaped multi-armed precursors by employing coarse-grained molecular dynamics simulations coupled with stochastic reaction model. Our research focuses on the structure characteristics of the generated networks

including the number and size of loops

as well as network dispers

ity characterized by loops. Tracking the number of loops during network generation allows for the identification of the gel point. The size distribution of loops in the network is primarily related to the functionality of the precursors

and the system with fewer precursor arms exhibiting larger average loop sizes. Strain-stress curves indicate that materials with identical functionality and precursor arm lengths generally exhibit superior performance. This method of characterizing network structures helps to refine microscopic structural analysis and contributes to the enhancement and optimization of material properties.

关键词

Keywords

references

Hina, M.; Bashir, S.; Kamran, K.; Ramesh, S.; Ramesh, K. Synthesis and characterization of self-healable poly(acrylamide) hydrogel electrolytes and their application in fabrication of aqueous supercapacitors. Polymer 2020 , 210 , 123020..

Taghipour, Y. D.; Hokmabad, V. R.; Bakhshayesh, D.; Rahmani, A.; Asadi, N.; Salehi, R.;Nasrabadi, H. T. The application of hydrogels based on natural polymers for tissue engineering. Curr. Med. Chem. 2020 , 27 , 2658−2680..

Chen, Y.; Zhang, M.; Sun, Y.; Phuhongsung, P. Improving 3D/4D printing characteristics of natural food gels by novel additives: a review. Food Hydrocoll. 2022 , 123 , 107160..

Yao, P.; Bao, Q.; Yao, Y.; Xiao, M.; Xu, Z.; Yang, J.; Liu, W. Environmentally stable, robust, adhesive, and conductive supramolecular deep eutectic gels as ultrasensitive flexible temperature sensor. Adv. Mater. 2023 , 35 , 2300114..

Yan, A.; Luo, Y.; Tian, H.; Pan, H.; Cao, Y.; Niu, B.; Long, D. Ultrahigh-strength silicone aerogels reinforced by an armor-like epoxy framework via a temperature-controlled sequential reaction strategy. J. Colloid Interface Sci. 2024 , 663 , 665−673..

Zhou, X.; Zhao, X.; Wang, Y.; Wang, P.; Jiang, X.; Song, Z.; Xu, W. Gel-based strain/pressure sensors for underwater sensing: sensing mechanisms, design strategies and applications. Compos. Part B. Eng. 2023 , 255 , 110631..

Zhao, H.; Chen, X.; Yuk, H.; Lin, S.; Liu, X.; Parada, G. Soft materials by design: unconventional polymer networks give extreme properties. Chem. Rev. 2021 , 121 , 4309−4372..

Danielsen, S. P.; Beech, H. K.; Wang, S.; El-Zaatari, B. M.; Wang, X.; Sapir, L.; Rubinstein, M. Molecular characterization of polymer networks. Chem. Rev. 2021 , 121 , 5042−5092..

Xie, D.; Hou, W.; Wang, X.; Fan, W.; Zhang, X.; Wang, D.; Sui, K. Chain folding double-network hydrogels leads to ultra-strong, stretchabl e and tough sensors. Compos. Commun. 2023 , 43 , 101692..

Liu, C.; Morimoto, N.; Jiang, L.; Kawahara, S.; Noritomi, T.; Yokoyama, H.; Ito, K. Tough hydrogels with rapid self-reinforcement. Science 2021 , 372 , 1078−1081..

Ghiassinejad, S.; Kumar Sharma, A.; Fustin, C. A.; van Ruymbeke, E. Effect of ring mobility on the dynamics of the slide-ring gels. Chem. Mater. 2024 , 36 , 8311−8322..

Wu, Z.; Zhang, P.; Zhang, H.; Li; X.; He; Y.; Qin, P.; Yang, C. Tough porous nanocomposite hydrogel for water treatment. J. Hazard. Mater. 2022 , 421 , 126754..

Tanpichai, S.; Oksman, K. Cross-linked nanocomposite hydrogels based on cellulose nanocrystals and PVA: mechanical properties and creep recovery. Compos. Part Appl. Sci. Manuf. 2016 , 88 , 226−233..

Gravelle, A. J.; Marangoni, A. G. A new fractal structural-mechanical theory of particle-filled colloidal networks with heterogeneous stress translation. J. Colloid Interface Sci. 2021 , 598 , 56−68..

Sakai, T.; Matsunaga, T.; Yamamoto, Y.; Ito, C.; Yoshida, R.; Suzuki, S.; Chung, U. I. Design and fabrication of a high-strength hydrogel with ideally homogeneous network structure from tetrahedron-like macromonomers. Macromolecules 2008 , 41 , 5379−5384..

Panyukov, S. Theory of flexible polymer networks: Elasticity and heterogeneities. Polymers 2020 , 12 , 767..

Luo, L.; Zhang, F.; Liu, Y.; Leng, J. Super-tough, self-sensing and shape-programmable polymers via topological structure crosslinking networks. Chem. Eng. J. 2023 , 457 , 141282..

Apostolides, D. E.; Sakai, T.; & Patrickios, C. S. Dynamic covalent star poly(ethylene glycol) model hydrogels: A new platform for mechanically robust, multifunctional materials. Macromolecules 2017 , 50 , 2155−2164..

Okaya, Y.; Jochi, Y.; Seki, T.; Satoh, K.; Kamigaito, M.; Hoshino, T.; Takeoka, Y. Precise synthesis of a homogeneous thermoresponsive polymer network composed of four-branched star polymers with a narrow molecular weight distribution. Macromolecules 2019 , 53 , 374−386..

Doehler, D.; Peterlik, H.; Binder, W. H. A dual crosslinked self-healing system: supramolecular and covalent network formation of four-arm star polymers. Polymer 2015 , 69 , 264−273..

Liu, H.; Mohsin, N.; Kim, S.; Chung, H. Lignin, a biomass crosslinker, in a shape memory polycaprolactone network. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57 , 2121−2130..

Li, Y.; Lu, H.; Zhang, Z. Y.; Liu, H.; Sun, Z. Y. Network formation and mechanical stretching of nanocomposite fabricated by crosslinking reaction of polymer-grafted nanoparticles. Compos. Sci. Technol. 2022 , 227 , 109605..

Bilal, M. H.; Mahmood, N.; Samiullah, M. H.; Busse, K.; Kressler, J. Physico-mechanical properties of poly(ethylene glycol)-based polymer networks. J. Appl. Polym. Sci. 2023 , 140 , e54726..

Samiullah, M. H.; Reichert, D.; Zinkevich, T.; Kressler, J. NMR characterization of PEG networks synthesized by CuAAC using reactive oligomers. Macromolecules 2013 , 46 , 6922−6930..

Sorichetti, V., Ninarello, A., Ruiz-Franco, J. M., Hugouvieux, V., Kob, W., Zaccarelli, E., & amp; Rovigatti, L. Effect of chain polydispersity on the elasticity of disordered polymer networks. Macromolecules 2021 , 54 , 3769−3779..

Furuya, T.; Koga, T. Molecular simulation of networks formed by end-linking of tetra-arm star polymers: Effects of network structures on mechanical properties. Polymer 2020 , 189 , 122195..

Kamata, H.; Akagi, Y.; Kayasuga-Kariya, Y.; Chung, U. I.; Sakai, T. “Nonswellable” hydrogel without mechanical hysteresis. Science 2014 , 343 , 873-875..

Dhamankar, S.; Webb, M. A. Chemically specific coarse-graining of polymers: Methods and prospects. J. Polym. Sci. 2021 , 59 , 2613−2643..

Li, X.; Hirosawa, K.; Sakai, T.; Gilbert, E. P.; Shibayama, M. SANS study on critical polymer clusters of tetra-functional polymers. Macromolecules 2017 , 50 , 3655−3661..

Svaneborg, C.; Everaers, R. Characteristic time and length scales in melts of Kremer–Grest bead–spring polymers with wormlike bending stiffness. Macromolecules 2020 , 53 , 1917−1941..

Liu, H.; Li, M.; Lu, Z. Y.; Zhang, Z. G.; Sun, C. C. Influence of surface-initiated polymerization rate and initiator density on the properties of polymer brushes. Macromolecules 2009 , 42 , 2863−2872..

Groot, R. D.; Warren, P. B. Dissipative particle dynamics: Bridging the gap between atomistic and mesoscopic simulation. J. Chem. Phys. 1997 , 107 , 4423−4435..

Espanol, P.; Warren, P. Statistical mechanics of dissipative particle dynamics. EPL 1995 , 30 , 191..

Li, Y.; Zhao, W.; Cheng, Z.; Sun, Z. Y.; Liu, H. Structural heterogeneity in tetra-armed gels revealed by computer simulation: evidence from a graph theory assisted characterization. J. Chem. Phys. 2024 , 160 , 144902..

Lang, M.; Michalke, W.; Kreitmeier, S. A statistical model for the length distribution of meshes in a polymer network. J. Chem. Phys. 2001 , 114 , 7627−7632..

Hutchinson, R. A. Modeling of chain length and long-chain branching distributions in free-radical polymerization. Macromol. Theory Simul. 2001 , 10 , 144−157..

Gavrilov, A. A.; Komarov, P. V.; Khalatur, P. G. Thermal properties and topology of epoxy networks: a multiscale simulation methodology. Macromolecules 2015 , 48 , 206−212..

Lang, M.; Kreitmeier, S.; Göritz, D. Trapped entanglements in polymer networks. Rubber Chem. Technol. 2007 , 80 , 873−894..

Deng, Y.; Chen, Y.; Zhang, Y.; Mahadevan, S. Fuzzy Dijkstra algorithm for shortest path problem under uncertain environment. Appl. Soft Comput. 2012 , 12 , 1231−1237..

Cail, J. I.; Stepto, R. F. T. The gel point and network formation–theory and experiment. Polym. Bull. 2007 , 58 , 15−25..

Yasuda, Y.; Morita, H. Structural Analysis of the Linear Elasticity of End-Cross-Linked Star Elastomers with a Number of Trapped Entanglements via Coarse-Grained Molecular Dynamics Simulations. Macromolecules 2024 , 57 , 4804−4816..

Uehara, S.; Wang, Y.; Ootani, Y.; Ozawa, N.; Kubo M. Molecular-level elucidation of a fracture process in slide-ring gels via coarse-grained molecular dynamics simulations. Macromolecules 2022 , 55 , 1946−1956..

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