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Open AccessOpen Access JUSTC Engineering & Materials 08 November 2023

Design of novel double-layer wrapped ammonium polyphosphate and its application in aging-resistant and flame retardant crosslinked polyethylene composites

  • State Key Laboratory of Fire Science, University of Science and Technology of China, Hefei 230027, China

Cite this:
https://doi.org/10.52396/JUSTC-2023-0090
More Information
  • Author Bio:

    Pengfei Jia is currently a postgraduate student in the State Key Laboratory of Fire Science, University of Science and Technology of China. His research mainly focuses on application about aging-resistant and flame-retardant crosslinked polyethylene composites

    Yuan Hu is an Professor and master supervisor at the State Key Laboratory of Fire Science, University of Science and Technology of China (USTC). He received his Ph.D. degree in Chemistry from USTC in 1997. His research mainly focuses on the New environmentally friendly flame retardant materials and technologies, high-performance polymer-based nanocomposites, as well as fire safety material research methods and technologies

    Bibo Wang is an Associate Professor and master supervisor at the State Key Laboratory of Fire Science, the University of Science and Technology of China. His research mainly focuses on the surface modification and microencapsulation technology of flame retardants, electron beam irradiation cross-linked flame retardant cables, aging performance, durability testing, and evaluation of flame retardant materials

  • Corresponding author: E-mail: yuanhu@ustc.edu.cn; E-mail: wbibo@ustc.edu.cn
  • Received Date: 20 May 2023
  • Accepted Date: 06 August 2023
    • Available Online: 08 November 2023
    Abstract

  • Abstract

    In this study, double-layer wrapped ammonium polyphosphate (APP) is designed to enhance the mechanical properties, resistance and flame retardancy of crosslinked polyethylene (XLPE) composites. APP was wrapped with silica and then grafted with hindered phenol antioxidant 3-(3,5-di-tert-butyl-4 hydroxyphenyl) (AO) to prepare double-layer wrapped flame retardants (MCAPP). Due to the excellent compatibility between the MCAPP and XLPE matrix, the tensile strength and elongation at break of XLPE/MCAPP/CFA (XLPE-4) were improved. Moreover, the retention rate of elongation at break for the XLPE-4 composite reached 61.1%, significantly higher than that of XLPE-1 (2.6%) at 135 °C after aging for 14 d. This demonstrates that MCAPP could improve the aging resistance of XLPE cable composites. Compared with XLPE-1, the maximum smoke density and the peak heat release rate were reduced by 54.9% and 89.7%, respectively. Thus, the double-layer wrapping antioxidant strategy provides an excellent approach to obtain high-performance XLPE composites.

    Graphical abstract

    The double-layer wrapped ammonium polyphosphate (APP) enhances the fire safety, aging resistance, and mechanical property of crosslinked polyethylene (XLPE) composites.

    Abstract

    In this study, double-layer wrapped ammonium polyphosphate (APP) is designed to enhance the mechanical properties, resistance and flame retardancy of crosslinked polyethylene (XLPE) composites. APP was wrapped with silica and then grafted with hindered phenol antioxidant 3-(3,5-di-tert-butyl-4 hydroxyphenyl) (AO) to prepare double-layer wrapped flame retardants (MCAPP). Due to the excellent compatibility between the MCAPP and XLPE matrix, the tensile strength and elongation at break of XLPE/MCAPP/CFA (XLPE-4) were improved. Moreover, the retention rate of elongation at break for the XLPE-4 composite reached 61.1%, significantly higher than that of XLPE-1 (2.6%) at 135 °C after aging for 14 d. This demonstrates that MCAPP could improve the aging resistance of XLPE cable composites. Compared with XLPE-1, the maximum smoke density and the peak heat release rate were reduced by 54.9% and 89.7%, respectively. Thus, the double-layer wrapping antioxidant strategy provides an excellent approach to obtain high-performance XLPE composites.

    • Public Summary

    • The double-layer wrapped ammonium polyphosphate (APP) enhances the compatibility and mechanical property of crosslinked polyethylene (XLPE) composites.
    • The OIT value of XLPE-4 composite is 182.95 min, which is approximately 8 times than that of XLPE-1.
    • After aging at 135 °C for 14 d, the retention of EB for XLPE-1 and XLPE-4 reaches 2.6% and 61.1%, respectively.
    • The PHRR and Ds-max of XLPE-4 are reduced by 89.7% and 54.9%, respectively.

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    • References(39)
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    [13]
    Liu Y, Wang D Y, Wang J S, et al. A novel intumescent flame-retardant LDPE system and its thermo-oxidative degradation and flame-retardant mechanisms. Polymers for Advanced Technologies, 2008, 19: 1566–1575. doi: 10.1002/pat.1171
    [14]
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    Ferdinánd M, Jerabek M, Várdai R, et al. Impact modification of wood flour reinforced PP composites: Problems, analysis, solution. Composites Part A: Applied Science and Manufacturing, 2023, 167: 107445. doi: 10.1016/j.compositesa.2023.107445
    [16]
    Li Y, Chen X, Liu Q, et al. Constructing cross-functional intumescent flame retardants with UV resistance for polypropylene composites. Materials Today Chemistry, 2022, 26: 101048. doi: 10.1016/j.mtchem.2022.101048
    [17]
    Xie H, Lai X, Li H, et al. Synthesis of a novel macromolecular charring agent with free-radical quenching capability and its synergism in flame retardant polypropylene. Polymer Degradation and Stability, 2016, 130: 68–77. doi: 10.1016/j.polymdegradstab.2016.05.029
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    Zhang L, Li H, Lai X, et al. Functionalized graphene as an effective antioxidant in natural rubber. Composites Part A: Applied Science and Manufacturing, 2018, 107: 47–54. doi: 10.1016/j.compositesa.2017.12.028
    [19]
    Wang J, Zheng Y, Ren W, et al. Intrinsic ionic confinement dynamic engineering of ionomers with low dielectric-k, high healing and stretchability for electronic device reconfiguration. Chemical Engineering Journal, 2023, 453: 139837. doi: 10.1016/j.cej.2022.139837
    [20]
    Zou Y, He J, Tang Z, et al. Structural and mechanical properties of styrene-butadiene rubber/silica composites with an interface modified in situ using a novel hindered phenol antioxidant and its samarium complex. Composites Science and Technology, 2020, 188: 107984. doi: 10.1016/j.compscitech.2019.107984
    [21]
    Li G, Wang F, Liu P, et al. Antioxidant functionalized silica-coated TiO2 nanorods to enhance the thermal and photo stability of polypropylene . Applied Surface Science, 2019, 476: 682–690. doi: 10.1016/j.apsusc.2019.01.116
    [22]
    Jiang S, Liu Y, Zou X, et al. Synthesis and application of new macromolecular hindered phenol antioxidants of polyamide 6. Journal of Applied Polymer Science, 2021, 138: 51184. doi: 10.1002/app.51184
    [23]
    Li R, Shi K, Ye L, et al. Polyamide 6/graphene oxide-g-hindered phenol antioxidant nano-composites: Intercalation structure and synergistic thermal oxidative stabilization effect. Composites Part B: Engineering, 2019, 162: 11–20. doi: 10.1016/j.compositesb.2018.10.091
    [24]
    Mousavi-Fakhrabadi S H, Ahmadi S, Arabi H. Mixing of hindered amine-grafted polyolefin elastomers with LDPE to enhance its long-term weathering and photo-stability. Polymer Degradation and Stability, 2022, 198: 109882. doi: 10.1016/j.polymdegradstab.2022.109882
    [25]
    Wang B, Tai Q, Nie S, et al. Electron beam irradiation cross linking of halogen-free flame-retardant ethylene vinyl acetate (EVA) copolymer by silica gel microencapsulated ammonium polyphosphate and char-forming agent. Industrial & Engineering Chemistry Research, 2011, 50: 5596–5605. doi: https://doi.org/10.1021/ie102394q
    [26]
    Jia P, Yu X, Lu J, et al. The Re2Sn2O7 (Re = Nd, Sm, Gd) on the enhancement of fire safety and physical performance of Polyolefin/IFR cable materials. Journal of Colloid and Interface Science, 2022, 608: 1652–1661. doi: 10.1016/j.jcis.2021.10.114
    [27]
    Xiao F, Fontaine G, Bourbigot S. Improvement of flame retardancy and antidripping properties of intumescent polybutylene succinate combining piperazine pyrophosphate and zinc borate. ACS Applied Polymer Materials, 2022, 4: 1911–1921. doi: 10.1021/acsapm.1c01755
    [28]
    Liu L, Zhu M, Shi Y, et al. Functionalizing MXene towards highly stretchable, ultratough, fatigue- and fire-resistant polymer nanocomposites. Chemical Engineering Journal, 2021, 424: 130338. doi: 10.1016/j.cej.2021.130338
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    Yu F, Jia P, Song L, Hu Y, Wang B, Wu R. Multifunctional fabrics based on copper sulfide with excellent electromagnetic interference shielding performance for medical electronics and physical therapy. Chemical Engineering Journal, 2023, 472: 145091. doi: https://doi.org/10.1016/j.cej.2023.145091
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    [36]
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    Figure  1.  (a) Schematic representation of the preparation process of MCAPP. (b) The corresponding WCA optical images. (c) SEM images of APP, SiAPP, and MCAPP. (d) EDX mapping images of MCAPP.

    Figure  2.  (a) FTIR spectra of APP, SiAPP, and MCAPP. (b) The contents of C 1 s and Si 2p from APP, SiAPP, and MCAPP. (c) TGA curves of APP, SiAPP, MCAPP, and AO under N2 atmosphere. (d) Radical scavenging activity of APP, SiAPP, MCAPP, and AO.

    Figure  3.  (a) Tensile strength, (b) elongation at break and (c–j) cross-sectional SEM images of XLPE-1, XLPE-2, XLPE-3, XLPE-4, XLPE-5, and XLPE-6.

    Figure  4.  (a, b) The OIT curves of XLPE composites at 210 °C. (c) Retention rate of elongation at break of XLPE composites with different aging times at 135 °C. Electron spin resonance spectra of XLPE composites before (d) and after (e) aging at 135 °C for 14 d.

    Figure  5.  (a, b) TGA and DTG curves for XLPE composites from 50 °C to 800 °C under a N2 atmosphere, respectively. (c–f) HRR, THR curves, maximum smoke density, and smoke transmittance curve of XLPE composites respectively. (g, h) The absorbance at the maximum decomposition rate and Gram‒Schmidt curves for XLPE-1 and XLPE-4. (i–l) Typical volatile thermal decomposition products versus time: CO, CO2, hydrocarbons, and aromatic.

    Figure  6.  Schematic diagram of the flame retardant mechanism of the XLPE-4 composite.

    [1]
    Chen J, Wang J, Ding A, et al. Flame retardancy and mechanical properties of glass fibre reinforced polyethylene composites filled with novel intumescent flame retardant. Composites Part B: Engineering, 2019, 179: 107555. doi: 10.1016/j.compositesb.2019.107555
    [2]
    Lau S, Gonchikzhapov M, Paletsky A, et al. Aluminum diethylphosphinate as a flame retardant for polyethylene: Investigation of the pyrolysis and combustion behavior of PE/AlPi-mixtures. Combustion and Flame, 2022, 240: 112006. doi: 10.1016/j.combustflame.2022.112006
    [3]
    Salasinska K, Mizera K, Celiński M, et al. Thermal properties and fire behavior of polyethylene with a mixture of copper phosphate and melamine phosphate as a novel flame retardant. Fire Safety Journal, 2020, 115: 103137. doi: 10.1016/j.firesaf.2020.103137
    [4]
    Wang C, Liu J, Wang Y, et al. Enhanced flame retardance in polyethylene/magnesium hydroxide/polycarbosilane blends. Materials Chemistry and Physics, 2020, 253: 123373. doi: 10.1016/j.matchemphys.2020.123373
    [5]
    Xie C, Leng F, Dong Z, et al. Synthesis of 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide derivative grafted polyethylene films for improving the flame retardant and anti-dripping properties. Polymer Engineering & Science, 2020, 60: 2804–2813. doi: https://doi.org/10.1002/pen.25512
    [6]
    Yan J, Xu M. Design, synthesis and application of a highly efficient mono-component intumescent flame retardant for non-charring polyethylene composites. Polymer Bulletin, 2021, 78: 643–662. doi: 10.1007/s00289-020-03130-6
    [7]
    Zhang T, Wang C, Wang Y, et al. Effects of modified layered double hydroxides on the thermal degradation and combustion behaviors of intumescent flame retardant polyethylene nanocomposites. Polymers, 2022, 14: 1616. doi: 10.3390/polym14081616
    [8]
    Birnbaum L S, Staskal D F. Brominated flame retardants: Cause for concern? Environmental Health Perspectives, 2004, 112: 9–17. doi: https://doi.org/10.1289/ehp.6559
    [9]
    Rault F, Giraud S, Salaün F. Flame retardant/resistant based nanocomposites in textile. In: Visakh P, Arao Y, editors. Flame Retardants. Cham: Springer, 2015: 131–165.
    [10]
    Hu X P, Li Y L, Wang Y Z. Synergistic effect of the charring agent on the thermal and flame retardant properties of polyethylene. Macromolecular Materials and Engineering, 2004, 289: 208–212. doi: 10.1002/mame.200300189
    [11]
    Li X, Yang B. Synergistic effects of pentaerythritol phosphate nickel salt (PPNS) with ammonium polyphosphate in flame retardant of polyethylene. Journal of Thermal Analysis and Calorimetry, 2015, 122: 359–368. doi: 10.1007/s10973-015-4683-0
    [12]
    Barczewski M, Hejna A, Sałasińska K, et al. Thermomechanical and fire properties of polyethylene-composite-filled ammonium polyphosphate and inorganic fillers: An evaluation of their modification efficiency. Polymers, 2022, 14: 2501. doi: 10.3390/polym14122501
    [13]
    Liu Y, Wang D Y, Wang J S, et al. A novel intumescent flame-retardant LDPE system and its thermo-oxidative degradation and flame-retardant mechanisms. Polymers for Advanced Technologies, 2008, 19: 1566–1575. doi: 10.1002/pat.1171
    [14]
    Martín Z, Jiménez I, Gómez M Á, et al. Interfacial interactions in PP/MMT/SEBS nanocomposites. Macromolecules, 2010, 43: 448–453. doi: 10.1021/ma901952p
    [15]
    Ferdinánd M, Jerabek M, Várdai R, et al. Impact modification of wood flour reinforced PP composites: Problems, analysis, solution. Composites Part A: Applied Science and Manufacturing, 2023, 167: 107445. doi: 10.1016/j.compositesa.2023.107445
    [16]
    Li Y, Chen X, Liu Q, et al. Constructing cross-functional intumescent flame retardants with UV resistance for polypropylene composites. Materials Today Chemistry, 2022, 26: 101048. doi: 10.1016/j.mtchem.2022.101048
    [17]
    Xie H, Lai X, Li H, et al. Synthesis of a novel macromolecular charring agent with free-radical quenching capability and its synergism in flame retardant polypropylene. Polymer Degradation and Stability, 2016, 130: 68–77. doi: 10.1016/j.polymdegradstab.2016.05.029
    [18]
    Zhang L, Li H, Lai X, et al. Functionalized graphene as an effective antioxidant in natural rubber. Composites Part A: Applied Science and Manufacturing, 2018, 107: 47–54. doi: 10.1016/j.compositesa.2017.12.028
    [19]
    Wang J, Zheng Y, Ren W, et al. Intrinsic ionic confinement dynamic engineering of ionomers with low dielectric-k, high healing and stretchability for electronic device reconfiguration. Chemical Engineering Journal, 2023, 453: 139837. doi: 10.1016/j.cej.2022.139837
    [20]
    Zou Y, He J, Tang Z, et al. Structural and mechanical properties of styrene-butadiene rubber/silica composites with an interface modified in situ using a novel hindered phenol antioxidant and its samarium complex. Composites Science and Technology, 2020, 188: 107984. doi: 10.1016/j.compscitech.2019.107984
    [21]
    Li G, Wang F, Liu P, et al. Antioxidant functionalized silica-coated TiO2 nanorods to enhance the thermal and photo stability of polypropylene . Applied Surface Science, 2019, 476: 682–690. doi: 10.1016/j.apsusc.2019.01.116
    [22]
    Jiang S, Liu Y, Zou X, et al. Synthesis and application of new macromolecular hindered phenol antioxidants of polyamide 6. Journal of Applied Polymer Science, 2021, 138: 51184. doi: 10.1002/app.51184
    [23]
    Li R, Shi K, Ye L, et al. Polyamide 6/graphene oxide-g-hindered phenol antioxidant nano-composites: Intercalation structure and synergistic thermal oxidative stabilization effect. Composites Part B: Engineering, 2019, 162: 11–20. doi: 10.1016/j.compositesb.2018.10.091
    [24]
    Mousavi-Fakhrabadi S H, Ahmadi S, Arabi H. Mixing of hindered amine-grafted polyolefin elastomers with LDPE to enhance its long-term weathering and photo-stability. Polymer Degradation and Stability, 2022, 198: 109882. doi: 10.1016/j.polymdegradstab.2022.109882
    [25]
    Wang B, Tai Q, Nie S, et al. Electron beam irradiation cross linking of halogen-free flame-retardant ethylene vinyl acetate (EVA) copolymer by silica gel microencapsulated ammonium polyphosphate and char-forming agent. Industrial & Engineering Chemistry Research, 2011, 50: 5596–5605. doi: https://doi.org/10.1021/ie102394q
    [26]
    Jia P, Yu X, Lu J, et al. The Re2Sn2O7 (Re = Nd, Sm, Gd) on the enhancement of fire safety and physical performance of Polyolefin/IFR cable materials. Journal of Colloid and Interface Science, 2022, 608: 1652–1661. doi: 10.1016/j.jcis.2021.10.114
    [27]
    Xiao F, Fontaine G, Bourbigot S. Improvement of flame retardancy and antidripping properties of intumescent polybutylene succinate combining piperazine pyrophosphate and zinc borate. ACS Applied Polymer Materials, 2022, 4: 1911–1921. doi: 10.1021/acsapm.1c01755
    [28]
    Liu L, Zhu M, Shi Y, et al. Functionalizing MXene towards highly stretchable, ultratough, fatigue- and fire-resistant polymer nanocomposites. Chemical Engineering Journal, 2021, 424: 130338. doi: 10.1016/j.cej.2021.130338
    [29]
    Yu F, Jia P, Song L, Hu Y, Wang B, Wu R. Multifunctional fabrics based on copper sulfide with excellent electromagnetic interference shielding performance for medical electronics and physical therapy. Chemical Engineering Journal, 2023, 472: 145091. doi: https://doi.org/10.1016/j.cej.2023.145091
    [30]
    Jiang X, Chu F, Liu W, et al. An individualized core–shell architecture derived from covalent triazine frameworks: Toward enhancing the flame retardancy, smoke release suppression, and toughness of bismaleimide resin. ACS Materials Letters, 2023, 5: 630–637. doi: 10.1021/acsmaterialslett.2c01173
    [31]
    Yin Z, Lu J, Hong N, et al. Functionalizing Ti3C2Tx for enhancing fire resistance and reducing toxic gases of flexible polyurethane foam composites with reinforced mechanical properties. Journal of Colloid and Interface Science, 2022, 607: 1300–1312. doi: 10.1016/j.jcis.2021.09.027
    [32]
    Jia P, Zhu Y, Lu J, et al. Multifunctional fireproof electromagnetic shielding polyurethane films with thermal management performance. Chemical Engineering Journal, 2022, 439: 135673. doi: 10.1016/j.cej.2022.135673
    [33]
    Wang J, Zhang D, Zhang Y, et al. Construction of multifunctional boron nitride nanosheet towards reducing toxic volatiles (CO and HCN) generation and fire hazard of thermoplastic polyurethane. Journal of Hazardous Materials, 2019, 362: 482–494. doi: 10.1016/j.jhazmat.2018.09.009
    [34]
    Zhang Y, Tian W, Liu L, et al. Eco-friendly flame retardant and electromagnetic interference shielding cotton fabrics with multi-layered coatings. Chemical Engineering Journal, 2019, 372: 1077–1090. doi: 10.1016/j.cej.2019.05.012
    [35]
    Jia P, Yu F, Jin Z, et al. Multifunctional Additive: A novel regulate strategy for improving mechanical property, aging life and fire safety of EVA composites. Chemical Engineering Journal, 2023, 473: 145283. doi: 10.1016/j.cej.2023.145283
    [36]
    Chen H R, Meng W M, Wang R Y, et al. Engineering highly graphitic carbon quantum dots by catalytic dehydrogenation and carbonization of Ti3C2Tx-MXene wrapped polystyrene spheres. Carbon, 2022, 190: 319–328. doi: 10.1016/j.carbon.2022.01.028
    [37]
    Wang N N, Wang H, Wang Y Y, et al. Robust, lightweight, hydrophobic, and fire-retarded polyimide/MXene aerogels for effective oil/water separation. ACS Applied Materials & Interfaces, 2019, 11: 40512–40523. doi: https://doi.org/10.1021/acsami.9b14265
    [38]
    Yin Z, Wang B, Tang Q, et al. Inspired by placoid scale to fabricate MXene derivative biomimetic structure on the improvement of interfacial compatibility, mechanical property, and fire safety of epoxy nanocomposites. Chemical Engineering Journal, 2022, 431: 133489. doi: 10.1016/j.cej.2021.133489
    [39]
    He W, Song P, Yu B, et al. Flame retardant polymeric nanocomposites through the combination of nanomaterials and conventional flame retardants. Progress in Materials Science, 2020, 114: 100687. doi: 10.1016/j.pmatsci.2020.100687
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