热氧老化对基于双重动态共价键的可降解树脂性能的影响

doi:10.19595/j.cnki.1000-6753.tces.240694

Abstract
Figure/Table
References (0)
Related Citation (7)

Download: PDF (1117 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract

Epoxy Resin (EP) possesses advantages such as low cost, high mechanical strength, robust chemical resistance, and excellent electrical insulation properties, making it extensively utilized in various epoxy cast electrical equipment like dry transformers and reactors. Nonetheless, the three-dimensional cross-linked network of resins exhibits non-melting characteristics, posing challenges in the degradation and recycling of retired epoxy electrical equipment. Nowadays, researchers have achieved epoxy resin recycling by incorporating dynamic covalent bonds into the epoxy resin crosslinking network to develop degradable Vitrimer epoxy resin materials. However, when applied to complex environments like high temperature, humidity, and intense electric fields, the internal crosslinking network of epoxy Vitrimers material may deteriorate, impacting its operational longevity. Therefore, besides ensuring favorable electrical, mechanical, and thermal properties, the enduring reliable performance of Vitrimer resin cannot be disregarded. This paper prepared dual-dynamic bonds Vitrimer resin with varying disulfide bond contents. The micromorphology, electrical characteristics, mechanical properties, dynamic thermodynamic properties, and degradation properties of Vitrimer resin at diverse aging stages were regularly investigated and the life evaluation model is constructed at last.
Firstly, dual dynamic crosslinked Vitrimer resin basded on ester bonds and varied disulfide bonds were prepared with 3,3’-Dithiodipropionic acid (DTDPA) and Hexahydro-4-methylphthalic anhydride (MHHPA) as the curing agent, with Triethanolamine acting as the catalyst. Subsequently, the accelerated thermo-oxygen aging tests were carried out, during which the microscopic morphology, electrical properties, bending characteristics, dynamic thermodynamic attributes, and degradation properties of vitrimer resin were periodically evaluated. Experiment results revealed alterations in the resin's microstructure under hot oxygen aging, leading to random internal cross-linked network fractures that generate abundant free radicals, ultimately causing resin failure. The resin's bending strength diminishes, rigidity increases, toughness notably decreases, and the bending fracture transitions to a brittle fracture pattern. As aging progresses, a denser cross-linked network forms on the resin's surface, elevating T_g. The integration of disulfide bonds makes the resin system more susceptible to oxidation and molecular chain breakage, resulting in reduced breakdown voltage, heightened dielectric loss factor, and increased insulation deterioration. Throughout the aging process, the degradation rate of Vitrimer resin in glycol solution decreases due to surface ester bond reduction and oxide layer formation, while the destruction of the disulfide crosslinking network prevents resin degradation in dithiothreitol solution. Lastly, a life evaluation model for the dual dynamic crosslinked Vitrimer resin was formulated based on the results of bending strength and TGA tests.
The dual dynamic crosslinked Vitrimer resin has excellent comprehensive properties and can realize the recycling of decommissioned epoxy electrical equipment. In this paper, the effect of thermal oxygen aging on the properties of dual dynamic crosslinked degradable resin was studied, which laid the experimental and theoretical foundation for the long-term service of vitrification epoxy resin in electrical equipment.

Key words： Vitrimer dual-dynamic bonds degradable epoxy resins thermal oxygen aging electrical equipment

Received: 06 May 2024

PACS:

TM21

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	Liu Hechen
	Liu Chang
	Sun Zhanglin
	Liu Yunpeng
	Jiang Yuzhe

Cite this article:

Liu Hechen,Liu Chang,Sun Zhanglin等. The Effect of Thermal Oxygen Aging on the Properties of Degradable Resin Based on Dual-Dynamic Bonds[J]. Transactions of China Electrotechnical Society, 0, (): 2492941-2492941.

URL:

https://dgjsxb.ces-transaction.com/EN/10.19595/j.cnki.1000-6753.tces.240694 OR https://dgjsxb.ces-transaction.com/EN/Y0/V/I/2492941

[1] Haque S M, Ardila-Rey J A, Umar Y, et al. Application and suitability of polymeric materials as insulators in electrical equipment[J]. Energies, 2021, 14(10): 2758.
[2] Alabiso W, Schlögl S.The impact of vitrimers on the industry of the future: chemistry, properties and sustainable forward-looking applications[J]. Polymers, 2020, 12(8): 1660.
[3] Chakma P, Konkolewicz D.Dynamic covalent bonds in polymeric materials[J]. Angewandte Chemie (International Edition in English), 2019, 58(29): 9682-9695.
[4] 伍云健, 丁大霖, 林慧, 等. 基于动态双硫键的本征自修复环氧绝缘材料性能研究[J]. 电工技术学报, 2024, 39(3): 836-843.
Wu Yunjian, Ding Dalin, Lin Hui, et al.Properties of intrinsic self-healing epoxy insulating materials based on dynamic disulfide bond[J]. Transactions of China Electrotechnical Society, 2024, 39(3): 836-843.
[5] Memon H, Wei Yi, Zhang Liying, et al.An imine-containing epoxy vitrimer with versatile recyclability and its application in fully recyclable carbon fiber reinforced composites[J]. Composites Science and Technology, 2020, 199: 108314.
[6] Ma Songqi, Wei Jingjing, Jia Zhen, et al.Readily recyclable, high-performance thermosetting materials based on a lignin-derived spiro diacetal trigger[J]. Journal of Materials Chemistry A, 2019, 7(3): 1233-1243.
[7] Lorero I, Rodríguez A, Campo M, et al.Thermally remendable, weldable, and recyclable epoxy network crosslinked with reversible Diels-alder bonds[J]. Polymer, 2022, 259: 125334.
[8] Wang Miaomiao, Gao Hong, Wang Zhen, et al.Rapid self-healed vitrimers via tailored hydroxyl esters and disulfide bonds[J]. Polymer, 2022, 248: 124801.
[9] Zhang Youhao, Yuan Li, Liang Guozheng, et al.Developing reversible self-healing and malleable epoxy resins with high performance and fast recycling through building cross-linked network with new disulfide-containing hardener[J]. Industrial & Engineering Chemistry Research, 2018, 57(37): 12397-12406.
[10] 王有元, 刘玉, 王施又, 等. 电热老化对干式变压器中环氧树脂特性的影响[J]. 电工技术学报, 2018, 33(16): 3906-3916.
Wang Youyuan, Liu Yu, Wang Shiyou, et al.The effect of electrothermal aging on the properties of epoxy resin in dry-type transformer[J]. Transactions of China Electrotechnical Society, 2018, 33(16): 3906-3916.
[11] 张福增, 王婷婷, 曾向君, 等. 阻燃剂对环氧树脂绝缘子护套材料耐热氧老化性能的影响[J]. 高压电器, 2023, 59(1): 154-160.
Zhang Fuzeng, Wang Tingting, Zeng Xiangjun, et al.Effect of flame retardant on thermal and oxidative aging properties of epoxy resin insulator sheath material[J]. High Voltage Apparatus, 2023, 59(1): 154-160.
[12] Adams J H, Goodrich J E.Analysis of nonvolatile oxidation products of polypropylene. II. Process degradation[J]. Journal of Polymer Science Part A-1: Polymer Chemistry, 1970, 8(5): 1269-1277.
[13] Wang Yongqiang, Zeng Zhuo, Gao Meng, et al.Hygrothermal aging characteristics of silicone-modified aging-resistant epoxy resin insulating material[J]. Polymers, 2021, 13(13): 2145.
[14] Zhang Fan, Yang Rui, Lu Diannan.Investigation of polymer aging mechanisms using molecular simulations: a review[J]. Polymers, 2023, 15(8): 1928.
[15] Yang Yongming, Xian Guijun, Li Hui, et al.Thermal aging of an anhydride-cured epoxy resin[J]. Polymer Degradation and Stability, 2015, 118: 111-119.
[16] Zhang Xiaoxing, Wu Yunjian, Wen Hao, et al.The influence of oxygen on thermal decomposition characteristics of epoxy resins cured by anhydride[J]. Polymer Degradation and Stability, 2018, 156: 125-131.
[17] Zhu Mingxiao, Li Jiacai, Song Henggao, et al.Determination of trap energy in polyethylene with different aging status by molecular dynamics and density function theory[J]. IEEE Transactions on Dielectrics and Electrical Insulation, 2019, 26(6): 1823-1830.
[18] Liu Hechen, Sun Zhanglin, Wei Liwei, et al.Double-dynamic crosslinked epoxy vitrimer resin prepared using transesterification and dynamic disulfide bonds: High-performance, degradable, self-healing, environment-friendly[J]. Polymer Testing, 2023, 126: 108145.
[19] Luo Chumeng, Yang Wei, Qi Wen, et al.Cost-efficient and recyclable epoxy vitrimer composite with low initial viscosity based on exchangeable disulfide crosslinks[J]. Polymer Testing, 2022, 113: 107670.
[20] Chen Mao, Zhou Lin, Wu Yeping, et al.Rapid stress relaxation and moderate temperature of malleability enabled by the synergy of disulfide metathesis and carboxylate transesterification in epoxy vitrimers[J]. ACS Macro Letters, 2019, 8(3): 255-260.
[21] 刘贺晨, 孙章林, 刘云鹏, 等. 基于酯交换的可回收类玻璃化环氧树脂制备与性能研究[J]. 电工技术学报, 2023, 38(15): 4019-4029.
Liu Hechen, Sun Zhanglin, Liu Yunpeng, et al.Preparation and properties of recyclable vitrified epoxy resin based on transesterification[J]. Transactions of China Electrotechnical Society, 2023, 38(15): 4019-4029.
[22] Xu Mingxin, Di Jinyi, Wu Yachang, et al.Insights into the pyrolysis mechanisms of epoxy resin polymers based on the combination of experiments and ReaxFF-MD simulation[J]. Chemical Engineering Journal, 2023, 473: 145404.
[23] Khajeh A, Mustapha F, Sultan M T H, et al. The effect of thermooxidative aging on the durability of glass fiber-reinforced epoxy[J]. Advances in Materials Science and Engineering, 2015, 2015: 372354.
[24] Ponnamma D, Ramachandran R, Hussain S, et al.Free-volume correlation with mechanical and dielectric properties of natural rubber/multi walled carbon nanotubes composites[J]. Composites Part A: Applied Science and Manufacturing, 2015, 77: 164-171.
[25] Pei Yanmin, Wang Kai, Zhan Maosheng, et al.Thermal-oxidative aging of DGEBA/EPN/LMPA epoxy system: chemical structure and thermal-mechanical properties[J]. Polymer Degradation and Stability, 2011, 96(7): 1179-1186.
[26] Li Ke, Wang Kai, Zhan Maosheng, et al.The change of thermal-mechanical properties and chemical structure of ambient cured DGEBA/TEPA under accelerated thermo-oxidative aging[J]. Polymer Degradation and Stability, 2013, 98(11): 2340-2346.
[27] Zhou Yao, Li Li, Han Zhubing, et al.Self-healing polymers for electronics and energy devices[J]. Chemical Reviews, 2023, 123(2): 558-612.
[28] 王镜然, 王英杰, 庄宏伟, 等. 低压电缆绝缘热氧老化过程中介电响应的Davidson-Cole分析[J]. 电工技术学报, 2023, 38(15): 4030-4039.
Wang Jingran, Wang Yingjie, Zhuang Hongwei, et al.Dielectric response during thermal-oxidative aging of low-voltage cable insulation analyzed by Davidson-Cole[J]. Transactions of China Electrotechnical Society, 2023, 38(15): 4030-4039.
[29] 王有元, 王施又, 黄炎光, 等. 干式变压器环氧树脂热老化特性研究[J]. 高电压技术, 2018, 44(1): 187-194.
Wang Youyuan, Wang Shiyou, Huang Yanguang, et al.Study on thermal aging characteristics of epoxy resin of dry-type transformer[J]. High Voltage Engineering, 2018, 44(1): 187-194.
[30] 段玉兵, 韩明明, 王兆琛, 等. 不同热老化温度下高压电缆绝缘特性及失效机理[J]. 电工技术学报, 2024, 39(1): 45-54.
Duan Yubing, Han Mingming, Wang Zhaochen, et al.Insulation characteristics and failure mechanism of high-voltage cables under different thermal aging temperatures[J]. Transactions of China Electrotechnical Society, 2024, 39(1): 45-54.
[31] Zhang Yucheng, Li Wendong, Zhao Xin, et al.Epoxy-based high-k composite vitrimer: With low dielectric loss, high breakdown strength and surface electrical damage repairability[J]. Chemical Engineering Journal, 2023, 473: 145199.
[32] Lu Jiwei, Schmidt S, Boesch D S, et al.Low-loss tunable capacitors fabricated directly on gold bottom electrodes[J]. 2006, 88(11): 112905.
[33] 刘贺晨, 魏利伟, 孙章林, 等. 催化剂对基于动态酯交换Vitrimers材料性能的影响[J]. 电工技术学报, 2024, 39(16): 5134-5148.
Liu Hechen, Wei Liwei, Sun Zhanglin, et al.Effect of catalysts on the performance of vitrimers based on dynamic ester exchange[J]. Transactions of China Electrotechnical Society, 2024, 39(16): 5134-5148.