Preparation and Characterization of Multilayered High-density Polyethylene with Tunable Crystalline Structure

Yi-Jie Ma; Jia-Wei Gong; Bin Chen; Ying Zhang; Gan-Ji Zhong; Zhong-Ming Li; Xue-Qin Gao

doi:10.1007/s10118-025-3363-1

Your Location：

Home >

Browse articles >

Preparation and Characterization of Multilayered High-density Polyethylene with Tunable Crystalline Structure

RESEARCH ARTICLE | Updated：2025-08-25

- Preparation and Characterization of Multilayered High-density Polyethylene with Tunable Crystalline Structure
- Chinese Journal of Polymer Science Vol. 43, Issue 9, Pages: 1616-1628(2025)
- Affiliations：
  
  a.College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, China
  b.Department of Mechanical Engineering, Pennsylvania State University, Erie, PA 16509, USA
- Author bio：
  
  gaoxueqin@scu.edu.cn
- Funds：
- DOI：10.1007/s10118-025-3363-1
  CLC：
- Received：20 February 2025，
  
  Revised：2025-04-06，
  
  Accepted：17 April 2025，
  
  Online First：23 July 2025，
  
  Published：05 September 2025
- Accepted：
Scan QR Code
Ma, Y. J.; Gong, J. W.; Chen, B.; Zhang, Y.; Zhong, G. J.; Li, Z. M.; Gao, X. Q. Preparation and characterization of multilayered high-density polyethylene with tunable crystalline structure. Chinese J. Polym. Sci. 2025, 43, 1616–1628

Yi-Jie Ma, Jia-Wei Gong, Bin Chen, et al. Preparation and Characterization of Multilayered High-density Polyethylene with Tunable Crystalline Structure[J]. Chinese Journal of Polymer Science, 2025, 43(9): 1616-1628.
Ma, Y. J.; Gong, J. W.; Chen, B.; Zhang, Y.; Zhong, G. J.; Li, Z. M.; Gao, X. Q. Preparation and characterization of multilayered high-density polyethylene with tunable crystalline structure. Chinese J. Polym. Sci. 2025, 43, 1616–1628 DOI： 10.1007/s10118-025-3363-1.

Yi-Jie Ma, Jia-Wei Gong, Bin Chen, et al. Preparation and Characterization of Multilayered High-density Polyethylene with Tunable Crystalline Structure[J]. Chinese Journal of Polymer Science, 2025, 43(9): 1616-1628. DOI： 10.1007/s10118-025-3363-1.

摘要

A novel rotational shear system (RSS) was used to fabricate multi-layer self-reinforced HDPE pipes featuring alternating shish-kebab and spherulite structures. Controlled mandrel rotation and cooling aligned molecular chains to form high-strength structures. The annular tensile strength of the TSK pipe increased from 26.7 MPa to 76.3 MPa

a 185.8% enhancement. SKS tubes maintained excellent tensile strength (73.4 MPa) and achieved 50.1% elongation due to smaller shish-kebab crystals and reduced interlocking. This improvement is supported by 2D-SAXS analysis

which confirmed that crystal size and amorphous region thickness critically affect the mechanical performance of these multi-layer pipes.

Abstract

In rotationally extruded fittings

high-density polyethylene (HDPE) pipes prepared using conventional processing methods often suffer from poor pressure resistance and low toughness. This study introduces an innovative rotary shear system (RSS) to address these deficiencies through controlled mandrel rotation and cooling rates. We successfully prepared self-reinforced HDPE pipes with a three-layer structure combining spherical and shish-kebab crystals. Rotational processing aligned the molecular chains in the ring direction and formed shish-kebab crystals. As a result

the annular tensile strength of the rotationally processed three-layer shish-kebab structure (TSK) pipe increased from 26.7 MPa to 76.3 MPa

an enhancement of 185.8%. Notably

while maintaining excellent tensile strength (73.4 MPa)

the elongation at break of the spherulite shish-kebab spherulite (SKS) tubes was improved to 50.1%

as compared to 33.8% in the case of shish-kebab spherulite shish-kebab (KSK) tubes. This improvement can be attributed to the changes in the micro-morphology and polymer structure within the SKS tubes

specifically due to the formation of small-sized shish-kebab crystals and the low degrees of interlocking.In addition

2D-SAXS analysis revealed that KSK tubes have higher tensile strength due to smaller crystal sizes and larger shish dimensions

forming dense interlocking structures. In contrast

the SKS and TSK tubes had thicker amorphous regions and smaller shish sizes

resulting in reduced interlocking and mechanical performance.

关键词

Keywords

references

Krushelnitzky, R. P.; Brachman, R. W. I. Buried high-density polyethylene pipe deflections at elevated temperatures. Geotext. Geomembr. 2013 , 40 , 69−77..

Hajibabaei, M.; Nazif, S.; Tavanaei Sereshgi F. Life cycle assessment of pipes and piping process in drinking water distribution networks to reduce environmental impact. Sustain. Cities Soc. 2018 , 43 , 538−549..

Kang, J.; Jung, Y.; Ahn, Y. Cover requirements of thermoplastic pipes used under highways. Compos. B. Eng. 2013 , 55 , 184−192..

Pearson, A.; Duncan, M.; Hammami, A.; Naguib H. E. Interfacial adhesion and thermal stability of high-density polyethylene glass fiber composites. Compos. Sci. Technol. 2022 , 227 , 109570..

Zhang, X. R.; Liu, C.; Liu, J. F.; Zhang, Z. Y.; Gong, Y. W.; Li, H. Y. Release of microplastics from typical rainwater facilities during aging process. Sci. Total Environ. 2022 , 813 , 152674..

Guidara, M. A.; Ali Bouaziz, M.; Schmitt, C.; Azari, Z.; Hadj-Taieb, E. A semi-empirical model for structural integrity assessment of defected high density polyethylene pipes. Eng. Fail. Anal. 2019 , 100 , 273−287..

Kwon, H. J.; Jar, P. Y. B. Toughness of high-density polyethylene in plane-strain fracture. Polym. Eng. Sci. 2006 , 46 , 1428−1432..

Dallali, M.; Azari, Z.; Schmitt, C.; Capelle, J.; Hadj-Taïeb, E. Experimental investigations of the critical values of J-integral and crack tip opening displacement (CTOD) of high-density poly-ethylene PE100 elbow. Eng. Fail. Anal. 2022 , 131 , 105834..

Yu, Y.; Yang, S.; Yu, H.; Li, J.; Guo, S. Temperature-dependent alternating α - or β -transcrystalline layersin coextruded isotactic polypropylene multilayered films. Macromolecules 2017 , 50 , 5098−5106..

Park, J. J.; Hong, S. M.; Lee, M. K.; Rhee, C. K.; Rhee, W. H. Enhancement in the microstructure and neutron shielding efficiency of sandwich type of 6061Al–B 4 C composite material via hot isostatic pressing. Nucl. Eng. Des. 2015 , 282 , 1−7..

Zhang, X. L.; Zhang, X. M.; Yang, M. T.; Yang, S.; Wu, H.; Guo,S. Y.; Wang, Y. Z. Ordered multilayer film of (graphene oxide/polymer and boron nitride/polymer) nanocomposites: an ideal EMI shielding material with excellent electrical insulation and high thermal conductivity. Compos. Sci. Technol. 2016 , 136 , 104−110..

Chen, B.; Gao, W.; Shen, J.; Guo, S. The multilayered distribution of intumescent flame retardants and its influence on the fire and mechanical properties of polypropylene. Compos. Sci. Technol. 2014 , 93 , 54−60..

Kazemzadeh Azad, S.; Akış, T. Automated selection of optimal material for pressurized multi-layer composite tubes based on an evolutionary approach. Neural Comput. Appl. 2018 , 29 , 405−416..

rávníček, L.; Poduška, J.; Messiha, M.; Arbeiter, F.; Pinter, G.; Náhlík, L.; Hutař, P. Effect of recycled material on failure by slow crack growth in multi-layer polyethylene pipes. Eng. Fract. Mech. 2023 , 289 , 109423..

He, Y. Y.; Vaz, M. A.; Caire, M.; Duan, M. L.; Su, J. Transient thermomechanical axisymmetric analysis of multilayer thermoplastic composite pipes. Appl. Math. Model. 2023 , 124 , 257−278..

Pei, C. Y.; Zhang, H. J.; Li, Y. W.; Gu, Z. P.; Chen, X. C.; Kuang, T. R. Robust and durable biodegradable polymer-based triboelectric nanogenerators enabled by trace amounts of melanin-like nanoparticles. Nano Energy 2025 , 135 , 110643..

Kua ng, T. R.; Guo, H. X.; Guo, W.; Liu, W. X.; Li, W.; Saeb, M. R.; Vatankhah-Varnosfaderani, M.; Sheiko, S. S. Boosting the strength and toughness of polymer blends via ligand-modulated MOFs. Adv. Sci. 2024 , 11 , 2407593..

Bai, Y.; Yuan, S.; Cheng, P.; Han, P. H.; Ruan, W. D.; Tang, G. Confined collapse of unbonded multi-layer pipe subjected to external pressure. Compos. Struct. 2016 , 158 , 1−10..

Pourmansouri, M.; Mosalmani, R.; Yaghootian, A.; Ghanbarzadeh, A. Detecting and locating delamination defect in multilayer pipes using torsional guided wave. Arch. Appl. Mech. 2022 , 92 , 1037−1052..

Zhu, F.; Pan, E. N.; Qian, Z. H.; Luo, Z. Waves in a generally anisotropic viscoelastic composite laminated bilayer: Impact of the imperfect interface from perfect to complete delamination. Int. J. Solids Struct. 2020 , 202 , 262−277..

Huang, J.; Gilbert, M.; Bowman J. The effect of a polypropylene skin on the structure and properties of PE/PP dual layer pressure pipe. Polym. Eng. Sci. 2012 , 52 , 1081−1088..

Lämmel, M.; Jaschinski, E.; Merkel, R.; Kroy, K. Microstructure of sheared entangled solutions of semiflexible polymers. Polymers 2016 , 8 , 353..

Guseva, M. A.; Gerasin, V. A.; Shklyaruk, B. F.; Dubinskiy, V. A. Relation between thermal effects and structural changes under deformation of thermoplastics. Polymer 2018 , 144 , 18−32..

Nie, Y. J.; Zhao, Y. F.; Matsuba, G.; Hu, W. B. Shish-kebab crystallites initiated by shear fracture in bulk polymers. Macromolecules 2018 , 51 , 480−487..

Foster, R. J.; Hine, P. J.; Ward, I. M. The effect of draw ratio on the mechanical properties and crystalline structure of single polymer polypropylene composites. Polymer 2016 , 91 , 156−161..

Yang, H.; Luo, X. H.; Shen, K. Z.; Yuan, Y.; Fu, Q.; Gao, X. Q.; Jiang, L. The role of mandrel rotation speed on morphology and mechanical properties of polyethylene pipes produced by rotational shear. Polymer 2019 , 184 , 121915..

Han, R.; Nie, M.; Bai, S.; Wang, Q . Control over crystalline form in polypropylene pipe via mandrel rotation extrusion. Polym. Bull. 2013 , 70 , 2083−2096..

Nie, M.; Wang, Q.; Bai, S. B. The effect of cooling mode on slow crack growth resistance of polyethylene pipe. J. Macromol. Sci. B 2010 , 49 , 640−651..

Nie, M.; Li, X.; Hu, X. Y.; Wang, Q. Effect of die temperature on morphology and performance of polyethylene pipe prepared via mandrel rotation extrusion. J. Macromol. Sci. B 2014 , 53 , 1442−1452..

Nie, M.; Bai, S. B.; Wang, Q. Effect of the inner wall cooling rate on the structure and properties of a polyethylene pipe extruded at a high rotation speed. J. Appl. Polym. Sci. 2011 , 119 , 1659−1666..

Wu, J. J.; Xie, Z. X.; Yang, H.; Yang, M. H.; Shen, K. Z.; Fu, Q.; Gao, X. Q. Effect of mandrel rotation speed on morphology and mechanical properties of polypropylene pipes produced by rotational shear. J. Polym. Res. 2021 , 28 , 25..

Xie, Z.; Gao, N.; Du, Z.; Yang, H.; Shen, K.; Fu, Q.; Gao, X. Role of melt pla sticizing temperature in morphology and properties of PE100 pipes prepared by a rotational shear system. ACS Omega 2020 , 5 , 12660−12671..

Guo J.; Zhang C.; Nie M.; Wang Q. The effect of soluble β-nucleator’s content on crystalline structure and performance of polypropylene pipe. J. Vinyl Addit. Technol. 2021 , 27 , 174−182..

Chen, B.; Gong, J.; Huang, W.; Gao, N.; Deng, C.; Gao, X. Constructing a parallel aligned shish kebab structure of HDPE/BN composites: toward improved two-way thermal conductivity and tensile strength. Compos. B. Eng. 2023 , 259 , 110699..

Wu, J. J.; Gao, N.; Jiang, L.; Zhong, G. J.; Deng, C.; Gao, X. Q. The coupling effect of cellulose nanocrystal and strong shear field achieved the strength and toughness balance of Polylactide. Int. J. Biol. Macromol. 2022 , 207 , 927−940..

Jiang, Z. Y.; Tang, Y. J.; Men, Y. F.; Enderle, H. F.; Lilge, D.; Roth, S. V.; Gehrke, R.; Rieger, J. Structural evolution of tensile-deformed high-density polyethylene during annealing: Scanning synchrotron small-angle X-ray scattering study. Macromolecules 2007 , 40 , 7263−7269..

Murthy, N. S.; Bednarczyk, C.; Moore, R. A. F.; Grubb, D. T. Analysis of small-angle X-ray scattering from fibers: Structural changes in nylon 6 upon drawing and annealing. J. Polym. Sci. B Polym. Phys. 1996 , 34 , 821−835..

Jiang, Z. Y.; Tang, Y. J.; Rieger, J.; Enderle, H. F.; Lilge, D.; Roth, S. V.; Gehrke, R.; Wu, Z. H.; Li, Z. H.; Li, X. H.; Men, Y. F. Structural evolution of melt-drawn transparent high-density polyethylene during heating and annealing: synchrotron small-angle X-ray scattering study. Eur. Polym. J. 2010 , 46 , 1866−1877..

Keum, J. K.; Zuo, F.; Hsiao, B. S. Formation and stability of shear-induced shish-kebab structure in highly entangled melts of UHMWPE/HDPE blends. Macromolecules 2008 , 41 , 4766−4776..

Zhu, P. wei; Tung, J.; Edward, G.; Nichols, L. Effects of different colorants on morphological development of sheared isotactic polypropylene: a study using synchrotron wide-angle X-ray scattering. J. Appl. Phys. 2008 , 103 , 124906..

Perret, R.; Ruland, W. Single and multiple X-ray small-angle scattering of carbon fibres. J. Appl. Crystallogr. 1969 , 2 , 209−218..

Views

1206

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Effect of Different Shear Modes on Morphology and Mechanical Properties of Polypropylene Pipes Produced by Rotational Shear

The Role of Mold Temperature on Morphology and Mechanical Properties of PE Pipe Produced by Rotational Shear

Constructing High-content, Highly Ordered Shish-Kebab Crystals during Hot-stretching via Varying Contents of Reserved Shish in Ultra-long Chain Ultra-high Molecular Weight Polyethylene Gel Systems

The Influence of Ethyl Branch on Formation of Shish-Kebab Crystals in Bimodal Polyethylene under Shear at Low Temperature

Distribution of α-, β-, and γ-Phases in a Multi-flow Injection-molded Hierarchical Structure

Related Author

Wei-Chen Zhou

Zu-Chen Du

Hao Yang

Jun-Jie Li

Qiang Fu

Ze-Xiang Xie

Xie-Huai Luo

Related Institution

School of Materials Science and Chemical Engineering, Ningbo University

SCG Chemicals Co., Ltd., Siam Cement Group (SCG). 1 Siam Cement Rd., Bangsue

USA Department of Chemistry, Stony Brook University, Stony Brook

NIST Center for Neutron Research, National Institute of Standards and Technology

Department of Materials Science and Engineering, University of Maryland, College Park

⁰