Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites

Xiao-Da Pan; Yun-Kui Song; Chong-Zhi Sun; Chao-Yang Yuan; Zong-Min Zhu; Jia-Ran Wang; Xian-Ze Yin; Hong-Tao Liu; Li Liu; Long Zheng

doi:10.1007/s10118-026-3580-2

Your Location：

Home >

Browse articles >

Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites

RESEARCH ARTICLE | Updated：2026-03-26

- Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites
- Chinese Journal of Polymer Science Vol. 44, Issue 4, Pages: 1186-1198(2026)
- Affiliations：
  
  a.Hubei Key Laboratory for New Textile Materials and Applications, College of Materials Science and Engineering, Wuhan Textile University, Wuhan 430200, China
  b.State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
  c.School of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 102202, China
- Author bio：
  
  lht@wtu.edu.cn (H.T.L.)
  liul@mail.buct.edu.cn (L.L.)
  lzheng@wtu.edu.cn (L.Z.)
- Funds：
- DOI：10.1007/s10118-026-3580-2
  CLC：
- Received：13 November 2025，
  
  Accepted：17 January 2026，
  
  Online First：10 March 2026，
  
  Published：05 April 2026
- Accepted：
Scan QR Code
Pan, X. D.; Song, Y. K.; Sun, C. Z.; Yuan, C. Y.; Zhu, Z. M.; Wang, J. R.; Yin, X. Z.; Liu, H. T.; Liu, L.; Zheng, L. Synergistic bioinspired interface and segregated graphene oxide networks enabling enhanced mechanical strength and chemical resistance in natural rubber latex composites. Chinese J. Polym. Sci. 2026, 44, 1186–1198

Xiao-Da Pan, Yun-Kui Song, Chong-Zhi Sun, et al. Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites[J]. Chinese Journal of Polymer Science, 2026, 44(4): 1186-1198.
Pan, X. D.; Song, Y. K.; Sun, C. Z.; Yuan, C. Y.; Zhu, Z. M.; Wang, J. R.; Yin, X. Z.; Liu, H. T.; Liu, L.; Zheng, L. Synergistic bioinspired interface and segregated graphene oxide networks enabling enhanced mechanical strength and chemical resistance in natural rubber latex composites. Chinese J. Polym. Sci. 2026, 44, 1186–1198 DOI： 10.1007/s10118-026-3580-2.

Xiao-Da Pan, Yun-Kui Song, Chong-Zhi Sun, et al. Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites[J]. Chinese Journal of Polymer Science, 2026, 44(4): 1186-1198. DOI： 10.1007/s10118-026-3580-2.

摘要

A mussel-inspired interfacial regulation strategy was developed by designing a catechol- and thiol-containing tannic acid-based modifier (TM) agent that induces graphene oxide (GO) to self-assemble on natural rubber (NR) latex particles into a segregated network

while Eu

coordination synergistically reinforces the interface. This struc

ture markedly promotes NR strain-induced crystallization and enhances mechanical

barrier

antibacterial

and chemical-resistant properties.

Abstract

Natural rubber (NR) latex is a renewable colloidal dispersion used in medical gloves

coatings

and flexible products. It is known for its excellent elasticity and film-forming ability but is limited by insufficient mechanical robustness and chemical resistance. Incorporating nanofillers

such as graphene oxide (GO)

is an effective approach to enhance its performance; however

achieving strong interfacial compatibility between hydrophilic GO and the nonpolar rubber matrix remains challenging. To overcome this issue

a multifunctional interf

acial design inspired by mussel adhesion chemistry was developed to construct a hierarchical and cohesive GO network within the NR latex matrix. A tannic acid-based modifier (TM) bearing catechol and thiol groups was synthesized and anchored onto latex particles

via

hydrogen bonding with surface proteins and phospholipids

enabling subsequent

–

interactions and hydrogen bonding with GO nanosheets. This guided the selective self-assembly of GO into a continuous segregated network along the latex particle boundaries. Hierarchical interface reinforcement was achieved through Eu

ligand coordination. The incorporation of GO and enhancement of interfacial interactions promoted strain-induced crystallization

resulting in increased crystallinity and improved load transfer. The resulting composite film containing 0.5 part per hundred rubber GO and the bioinspired interface exhibited a tensile strength that was 107.8% higher than that of the pure NR latex film

while maintaining an elongation at break of 915%. Tear strength increased by 118.5%

toughness reached 61.7 MJ/m

nitrogen permeability decreased by 20.1%

and antibacterial efficiency against both

Escherichia coli

and

Staphylococcus aureus

reached 99.9%. The films also exhibited enhanced resistance to organic solvents

acids

and alkalis. This study provides a green and scalable strategy for fabricating high-performance NR latex-based products suitable for medical

protective

and engineering applications.

关键词

Keywords

references

Sriring, M.; Nimpaiboon, A.; Kumarn, S.; Higaki, K.; Higaki, Y.; Kojio, K.; Takahara, A.; Ho, C. C.; Sakdapipanich, J. Film formation process of natural rubber latex particles: roles of the particle size and distribution of non-rubber species on film microstructure. Colloid. Surfaces A 2020 , 592 , 124571..

Wei, Y. C.; Xia, J.H.; Zhang, L.; Zheng, T. T.; Liao, S. Influence of non-rubber components on film formation behavior of natural rubber latex. Colloid. Polym. Sci. 2020 , 298 , 1263−1271..

Ng, J. W.; Othman, N.; Yusof, N. H. Various coagulation techniques and their impacts towards the properties of natural rubber latex from Hevea brasiliensis—a comprehensive review related to tyre application. Ind. Crop. Prod. 2022 , 181 , 114835..

Zhang, G.; Guo, B.; Zhang, L. Significant trends in rubber research driven by environment, resource, and sustainability. Macromolecules 2025 , 58 , 5883−5903..

Whba, R.; Su'ait, M. S.; Whba, F.; Sahinbay, S.; Altin, S.; Ahmad, A. Intrinsic challenges and strategic approaches for enhancing the potential of natural rubber and its derivatives: a review. Int. J. Biol. Macromol. 2024 , 276 , 133796..

Sethulekshmi, A. S.; Saritha, A.; Joseph, K. A comprehensive review on the recent advancements in natural rubber nanocomposites. Int. J. Biol. Macromol. 2022 , 194 , 819−842..

Hou, J.R.; Huang, S. S.; Zhang, N.; Liu, D. Y.; Zhang, Z. J.; Yang, H. S.; Zong, L.; Duan, Y. X.; Zhang, J. M. Reinforcing natural rubber by amphiphilic graphene oxide for high-performance catheters. Polymer 2021 , 232 , 124142..

Yang, W.; Liu, J. J.; Wang, L. L.; Wang, W.; Yuen, A. C. Y.; Peng, S.; Yu, B.; Lu, H. D.; Yeoh, G. H.; Wang, C. H. Multifunctional MXene/natural rubber composite films with exceptional flexibility and durability. Compos. Part B-Eng. 2020 , 188 , 107875..

Hosseinmardi, A.; Amiralian, N.; Hayati, A. N.; Martin, D. J.; Annamalai, P. K. Toughening of natural rubber nanocomposites by the incorporation of nanoscale lignin combined with an industrially relevant leaching process. Ind. Crop. Prod. 2021 , 159 , 113063..

Li, J.; Liu, G.; Liu, Y.; Wu, Y.; He, M.; Li, Y. Cellulose fiber-assisted construction of multifunctional natural rubber latex sponges with excellent water-responsive shape memory behavior and oil absorption properties using ice template-vulcanization technology. Int. J. Biol. Macromol. 2025 , 308 , 142505..

Luo, C.; Xu, Y.; Jin, H. Preparation of biomass-oxidized natural rubber/cellulose nanofibers composites with enhanced mechani cal properties and self-healing properties based on hydrogen bonding network. Ind. Crop. Prod. 2025 , 226 , 120628..

Gong, H.; Zhong, K.; Chen, F.; Yi, M.; Wan, L.; Wang, Z.; Liao, J. Preparation of modified hydroxyapatite and its effect on natural latex film. J. Appl. Polym. Sci. 2023 , 140 , e54019..

Liu, C.; Huang, S.; Hou, J.; Zhang, W.; Wang, J.; Yang, H.; Zhang, J. Natural rubber latex reinforced by graphene oxide/zwitterionic chitin nanocrystal hybrids for high-performance elastomers without sulfur vulcanization. ACS Sustain. Chem. Eng. 2021 , 9 , 6470−6478..

Szadkowski, B.; Rybiński, P.; Sarlin, E.; Marzec, A. Bio-functionalization of fillers with natural phytic acid for sustainable flame-retardant agents for natural rubber composites. Ind. Crop. Prod. 2024 , 222 , 119504..

Kargarzadeh, H.; Mariano, M.; Huang, J.; Lin, N.; Ahmad, I.; Dufresne, A.; Thomas, S. Recent developments on nanocellulose reinforced polymer nanocomposites: a review. Polymer 2017 , 132 , 368−393..

Wang, L.; Zhang, J.; Yang, G.; Sun, Y.; Liang, Y.; Wang, Y.; Li, C. Self-crosslinking of graphene oxide/natural rubber nanocomposite film under assistance of protein for enhancing gas barrier performance. Surf. Interfaces 2021 , 26 , 101359..

Xing, W.; Wu, J.; Huang, G.; Li, H.; Tang, M.; Fu, X. Enhanced mechanical properties of graphene/natural rubber nanocomposites at low content. Polym. Int. 2014 , 63 , 1674−1681..

George, N.; C. S, J. C.; Mathiazhagan, A.; Joseph, R. High performance natural rubber composites with conductive segregated network of multiwalled carbon nanotubes. Compos. Sci. Technol. 2015 , 116 , 33−40..

George, N.; Varghese, G. A.; Joseph, R. Improved mechanical and barrier properties of Natural rubber-Multiwalled carbon nanotube composites with segregated network structure. Mater. Today: Proc. 2019 , 9 , 13−20..

George, N.; Bipinbal, P.; Bhadran, B.; Mathiazhagan, A.; Joseph, R. Segregated network formation of multiwalled carbon nanotubes in natural rubber through surfactant assisted latex compounding: A novel technique for multifunctional properties. Polymer 2017 , 112 , 264−277..

Zhu, Y.; Wei, L.Y.; Fu, X.; Zhang, J. Q.; Kong, L. M.; Huang, G. S.; Wu, J. R. Super strong and tough elastomers enabled by sacrificial segregated network. Chinese J.Polym. Sci. 2020 , 39 , 377−386..

Zheng, S.; Wang, Y.; Zhu, Y.; Zheng, C. Recent advances in the construction and properties of carbon-based nanofillers/polymer composites with segregated network structures. Mater. Today Commun. 2023 , 36 , 106773..

Pan, G.; Li, B. A dynamic biointerface controls mussel adhesion. Science 2023 , 382 , 763−764..

Zhang, C.; Xiang, L.; Zhang, J.; Liu, C.; Wang, Z.; Zeng, H.; Xu, Z.-K. Revisiting the adhesion mechanism of mussel-inspired chemistry. Chem. Sci. 2022 , 13 , 1698−1705..

Huang, S.; Zhang, J.; Kong, L.; Li, W.; Xie, Z. T.; Wu, J. Fully biosourced, vulcanization-free, and thermal-responsive natural rubber material. Macromolecules 2024 , 57 , 1642−1652..

Wei, Y. C.; Liu, G. X.; Zhang, L.; Xu, W. Z.; Liao, S.; Luo, M. C. Mimicking the mechanical robustness of natural rubber based on a sacrificial network constructed by phospholipids. ACS Appl. Mater. Interfaces 2020 , 12 , 14468−14475..

Zhu, S.; Zhao, F.; Sun, Y.; Wang, C.; Yuan, Z.; Liao, S. Fluorinated natural rubber with enhanced strength and excellent resistance to ozone, organic solvent, and acid and alkali via in situ reactive melt extrusion. Polym. Degrad. Stabil. 2024 , 228 , 110916..

Zhou, Z.; Liu, T.; Zhou, W.; Chen, H.; Bian, Y.; Gong, S.; Shi, S. Q.; Li, J. A strong and biodegradable wood particles-based bioplastic modified by synergistically dynamic cross-linking with tannic acid and Fe3+. Compos. Part B-Eng. 2022 , 247 , 110349..

Li, Z.; Liu, R.; Zhang, Y.; Yang, K.; Zhang, Z.; Zhao, Y.; Yan, H. Designing schiff-based hyperbranched polysiloxane for simultaneously enhancing epoxy resin with mechanical properties, thermal stability, and recyclability. ACS Appl. Polym. Mater. 2024 , 6 , 3115−3127..

Li, H.; Gao, C.; Tang, L.; Wang, C.; Chen, Q.; Zheng, Q.; Yang, S.; Sheng, S.; Zan, X. Lysozyme (Lys), tannic acid (TA), and graphene oxide (GO) thin coating for antibacterial and enhanced osteogenesis. ACS Appl. Bio Mater. 2020 , 3 , 673−684..

Boro, U.; Karak, N. Tannic acid based hyperbranched epoxy/reduced graphene oxide nanocomposites as surface coating materials. Prog. Org. Coat. 2017 , 104 , 180−187..

Quevedo, B. V.; Komatsu, D.; de Lourdes Rezende, M.; de Rezende Duek, E. A. Synthesis of epoxidized natural rubber grafted with hyaluronic acid for the development of biomaterials. Int. J. Biol. Macromol. 2023 , 244 , 125359..

Qiu, H.; Ni, W.; Yang, L.; Zhang, Q. Remarkable ability of Pb(II) capture from water by self-assembled metal-phenolic networks prepared with tannic acid and ferric ions. Chem. Eng. J. 2022 , 450 , 138161..

Li, S.; Liang, F.; Zhou, J.; Shi, B. Bio-inspired dual crosslinked network mediated by plant polyphenols for toughening natural rubber latex-based elastomeric composites. Ind. Crop. Prod. 2024 , 210 , 118027..

Dong, G.; Liu, H.; Yu, X.; Zhang, X.; Lu, H.; Zhou, T.; Cao, J. Antimicrobial and anti-biofilm activity of tannic acid against Staphylococcus aureus. Nat. Prod. Res. 2018 , 32 , 2225−2228..

Sethulekshmi, A. S.; Joseph, K.; Aprem, A. S.; Sisupal, S. B.; Punetha, V. D.; Saritha, A. Green synthesis of tannic acid-modified tungsten disulfide nanosheets: a cost effective pathway towards tailoring the properties of natural rubber. Tungsten 2025 , 1−14..

Views

131

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Processing-integrated Machine Learning Models for Predicting and Optimizing Mechanical Properties of Polyimides

Dislocation Propagation and Mechanical Properties in Poly(p-phenylene terephthalamide) Fibers: An All-atom Molecular Dynamics Simulation

High-performance Polydimethylsiloxane Composites Based on Ordered Three-dimensional PVA-MMT Aerogel Network: Network Structure Regulation and Mechanical Enhancement Mechanism

Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation

A Paradigm for BF3 Co-initiated Cationic Polymerization with Low Dispersity: Introducing Acetonitrile and Lowering the Reaction Temperature

Related Author

Wei-Long Hu

Hao-Ke Qiu

En-Zhe Jing

Wan-Chen Zhao

Hai-Yang Huo

Zhao-Yan Sun

Jia Wan

Ran Chen

Related Institution

School of Applied Chemistry and Engineering, University of Science and Technology of China

State Key Laboratory of Polymer Physics and Chemistry & Key Laboratory of Polymer Science and Technology, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences

Jilin Provincial International Cooperation Key Laboratory for Polymer Processing Physics

State Key Laboratory of Polymer Science and Technology, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences

CAS Key Laboratory of High-Performance Synthetic Rubber and Its Composite Materials, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences

⁰