Research Progress in Low Dielectric Loss Epoxy Resin Composites

doi:10.19491/j.issn.1001-9278.2021.03.018

Abstract

Abstract:

With the rapid development of the Internet of Things （IoT） and the fifth generation mobile communication technology （5G）， the higher level of requirement has been put forward for the dielectric performance of packaging materials and component substrates. The development of epoxy composites with a low dielectric constant and low dielectric loss has become an important research direction. Some methods for the preparation of low-dielectric epoxy composites were reviewed from the aspects of raw materials， curing conditions， fillers， blends， copolymerization， and multi-layers cast. The mechanisms for low?dielectric composites were also analyzed. Finally， some problems in the preparation of low-dielectric epoxy resins were discussed， and some prospects for future research were provided.

Key words: epoxy, composite, dielectric property, dielectric loss, dissipation factor

CLC Number:

TQ323.5

LUO Xuanang, LIU Shumei, ZHAO Jianqing. Research Progress in Low Dielectric Loss Epoxy Resin Composites[J]. China Plastics, 2021, 35(3): 130-138.

Figures/Tables 6

Fig.1. Two main polarization forms of dielectric loss of materials

Fig.2. Schematic illustration of dipole orientation after structural enhancement of fillers

Fig.3. Schematic of charge separation in Maxwell?Wagner?Sillars effects

Fig.4. Schematic diagram of Coulomb Blockade

Fig.5. Synthetic equation of DCPD?PPO

Fig.6. Schematic illustration of charge distribution in composites

References 40

1	YANG X F， LIU J， CHEN Q， et al. A Low Temperature Vulcanized Transparent Silane Modified Epoxy Resins for LED Filament Bulb Package［J］. Chinese Journal of Polymer Science， 2018， 36（5）：114⁃121.
2	ZHAO H， ZHANG D， TIAN J， et al. Research on Dielectric Properties about Different Curing Degree of Epoxy Glass Fiber［C］//Condition Monitoring and Diagnosis. IEEE， 2018.
3	LIU J， LI X， WEI X. The Dielectric Response Characteristics of Curing Process in Epoxy⁃Mica Composite Insulation ［J］. Electric Machines and Control， 2014， 18（6）：22⁃28.
4	ROGGERO A， CAUSSÉ N， DANTRAS E， et al. Thermal Activation of Impedance Measurements on an Epoxy Coating for the Corrosion Protection： 1. Dielectric Spectroscopy Response in the Dry State［J］. Electrochimica Acta， 2019，doi：10.1016/j.electacta.2019.02.035.
5	尹桂来，李建英，唐壮，等. GIS用环氧浇注材料的介电松弛特性研究［J］. 绝缘材料， 2015（3）：doi：10.3969/j.issn.1009⁃9239.2015.03.011.
	YIN G L， LI J Y， TANG Z， et al. Dielectric Relaxation Characteristic of Epoxy Casting Materials for GIS［J］. Insulating Materials， 2015（3）：doi：10.3969/j.issn.1009⁃9239.2015.03.011.
6	虞锦洪. 高导热聚合物基复合材料的制备与性能研究［D］.上海交通大学，2012.
7	马万里. 环氧树脂/氮化硼微纳米复合材料的导热与电气绝缘性能研究［J］. 绝缘材料， 2019， 52（7）：36⁃42.
	MA W L. Thermal Conductivity and Electrical Insulation Properties of Epoxy/BN Micro and Nano Composites［J］. Insulating Materials， 2019， 52（7）：36⁃42.
8	XU M， CAO X L， YU B L. Study on Properties of Nano⁃SiO₂/Epoxy Resin Composite （Ⅱ） Electrical and Mechanical Properties ［J］. Polymeric Materials Science & Engineering， 2005，21：156⁃159.
9	WU R W， ZHANG D H， et al. Effect of Silica Particle Size on Dielectric Properties of SiO₂/Epoxy Composite［J］. The Chinese Journal of Process Engineering， 2015， 15（3）： 530⁃535.
10	KREMER F， SCHÖNHALS A. Broadband Dielectric Spectroscopy［C］// IEEE Conference on Electrical Insulation & Dielectric Phenomena. IEEE， 2010.
11	ZHANG C C， ZHOU H， ZHU J. Preparation and Characterization of Epoxy/SiO₂ Hollow Spheres Composites with Low Dielectric Constant ［J］. Insulating Materials， 2011， 44（3）：1⁃4.
12	何先成，钟翔屿，李晔. QW220/5284RTM复合材料的介电性能研究［J］. 玻璃钢复合材料， 2016（4）： 45⁃50.
	HE X C， ZHONG X Y， LI Y. Study on Dielectric Properties of Quartz Fiber Reinforced 5284rtm Epoxy Resin Composites［J］. Fiber Reinforced Plastics/Composites， 2016（4）： 45⁃50.
13	GAO G P， HU Y， JIA H Y， et al. Acoustic and Dielectric Properties of Epoxy Resin/Hollow Glass Microsphere Composite Acoustic Materials［J］. Journal of Physics and Chemistry of Solids， 2019， 135：109105.
14	HONG X H， HUA Y Q. The Dielectric Properties of Glass Fiber Reinforced Plastics ［J］. New Chemical Materials，2005，33（4）：16⁃19.
15	陈秋婷，梁先文，于淑会，等. 以聚苯胺表面包覆钛酸钡作为填料的环氧复合材料的微观结构与介电性能［J］. 集成技术， 2014（6）：52⁃62.
	CHEN Q T， LIANG X W， YU S H， et al. Microstructure and Dielectric Properties of Epoxy Composites with Polyaniline⁃Deposited BaTiO₃ as Fillers［J］. Journal of Integration Technology， 2014（6）：52⁃62.
16	余燕飞. 钛酸钡/环氧树脂复合材料的制备及其介电性能的研究［D］.北京：北京化工大学， 2007.
17	王歆，夏亚飞，刘继红，等. 钛酸钡⁃环氧树脂复合材料的制备与介电性研究［J］. 中国陶瓷， 2014（3）：20⁃23.
	WANG X， XIA Y F， LIU J H， et al. Study on the Fabrication and Dielectric of Barium Titanate⁃Epoxy Composite［J］. China Ceramics， 2014（3）：20⁃23.
18	陈平，刘胜平，陈辉，等. 温度和水煮时间对玻璃纤维/环氧基复合材料界面层介电性能的影响研究［J］. 复合材料学报， 1997， 14（3）：67⁃71.
	CHEN P， LIU S P， CHEN H， et al. Effect of Temperature and Boiling Time on Dielectric Properties of Glass Fiber/Epoxy Composite Interface Layer［J］. Acta Materiae Compositae Sinica， 1997， 14（3）：67⁃71.
19	陈平，刘胜平，张明艳. 偶联剂对玻璃纤维/环氧树脂基复合材料介电性能的影响［J］. 高分子学报， 1997， 1（4）：492⁃495.
	CHEN P， LIU S P， ZHANG M Y. Effect of Coupling Agent on Dielectric Properties of Glass Fiber/Epoxy Resin Matrix Composites［J］. Acta Polymerica Sinica， 1997， 1（4）：492⁃495.
20	BIAN J P， ZHAO Q L， HOU Z Z， et al. Effect of Alumina Shapes on Dielectric Properties of UV⁃Cured Epoxy Acrylic Composite with Alumina［J］. Royal Society Open Science，2019， 6（1）：181509.
21	CHEN S Y， CHENG Y H， XIE Q， et al. Enhanced Breakdown Strength of Aligned⁃Sodium⁃Titanate⁃Nanowire/Epoxy Nanocomposites and their Anisotropic Dielectric Properties［J］. Composites Part A： Applied Science and Manufacturing， 2019， doi：10.1016/j.compositesa.2019.02.024.
22	白元元，牛玉娟，喻科，等. 一种适用于微波频段的埋入式电容用复合材料的制备及性能研究［C］//第十五届中国覆铜板技术·市场研讨会暨覆铜板产业协同创新国际论坛论，东莞：2014，100⁃104.
23	MEISAK D， MACUTKEVIC J， BYCHANOK D， et al. Broadband Dielectric Properties of Fe₂O₃·H₂O Nanorods/Epoxy Resin Composites［J］. Journal of Nanomaterials， 2019，doi：10.1155/2019/9756920.
24	苏丽. 纳米银/环氧树脂复合材料的制备及其介电性能［J］. 化工进展， 2011， 30（8）：1 800⁃1 804.
	SU L. Preparation and Dielectric Properties of Nano⁃Silver/Epoxy Composites［J］. Chemical Industry and Engineering Progress， 2011， 30（8）：1 800⁃1 804.
25	王童星. 新型功能石墨烯及其高介电常数低介电损耗环氧树脂基复合材料的研究［D］. 苏州：苏州大学.2015.
26	任兆琨，张明艳，孙睿，等. EP/MWNTs/OMMT复合材料的电学性能研究［J］. 绝缘材料， 2013（4）：40⁃42.
	REN Z K， ZHANG M Y， SUN R， et al. Dielectric Properties Study of Epoxy/Multi⁃walled Carbon Nanotubes/Organic Montmorillonite Composites［J］. Insulating Materials， 2013（4）：40⁃42.
27	LUO H C， QIU J， et al. Carbon Nanotubes/Epoxy Resin Metacomposites with Adjustable Radio⁃Frequency Negative Permittivity and Low Dielectric Loss［J］. Ceramics International， 2018，45（1）：doi： 10.1016/j.ceramint.2018.09.253.
28	汪水平，中村茂夫. 活性酯固化环氧树脂物性的研究［J］.高分子学报，1999，1（6）：741⁃747.
	WANG S P， NAKAMURA S. Study on Physical Properties of Modified Products by Modification of Active Esters And Epoxy Resin［J］. Acta Polymerica Sinica，1999，1（6）：741⁃747.
29	CAO Y M， SUN J. Dielectric Properties of the Modified Epoxy Resins by Polyester ［J］. Journal of Xi’an Jiaotong University， 2000，34（8）：75⁃78.
30	吴唯，陈诗英，宗孟静子. 纳米Al₂O₃/聚醚砜⁃环氧树脂复合材料的介电性能及热稳定性能［J］. 材料导报， 2017（20）：24⁃27，32.
	WU W， CHEN S， ZONG M. Dielectric Properties and Thermal Stability of Nano⁃Al₂O₃/Polyether Sulfone⁃Epoxy Resin Composites［J］. Materials Review， 2017（20）：24⁃27，32.
31	HWANG H J， HSU S W， CHUNG C L， et al. Low Dielectric Epoxy Resins from Dicyclopentadiene⁃Containing Poly（Phenylene Oxide） Novolac Cured with Dicyclopentadiene Containing Epoxy［J］. Reactive & Functional Polymers， 2008， 68（8）： 1 185⁃1 193.
32	商宇飞. 低介电笼型倍半硅氧烷改性氰酸酯—环氧树脂复合材料的制备与表征［D］.北京：北京化工大学，2008.
33	任强，韩玉，李锦春，等. 低介电高耐热环氧树脂/聚苯醚/POSS纳米复合材料研究［J］. 功能材料， 2013， 44（9）：1 320⁃1 323.
	REN Q， HAN Y， LI J C， et al. Studies on the Epoxy/Poly（Phenylene Ether）/POSS Nanocomposites with Low Dielectric and High Heat Resistant Properties［J］. Journal of Functional Materials， 2013， 44（9）：1 320⁃1 323.
34	钱军民，李旭祥.环氧树脂改性研究进展［J］.工程塑料应用， 2001，29（10）：50⁃53.
	QIAN J M， LI X X. Advance in the Modification Research of Epoxy Resin ［J］. Engineering Plastics Application， 2001，29（10）：50⁃53.
35	ZHANG Y R， ZHAO C J， LIU J. Preparation and Characterization of Ultralow Dielectric and Fibrous Epoxy Thermoset Cured with Poly（Arylene Ether Ketone） Containing Phenolic Hydroxyl Groups［J］. European Polymer Journal， 2018，doi：10.1016/j.eurpolymj.2018.08.059.
36	LIANG L， YU R B， ZHANG Z Y， et al. Study on the Dielectric Properties of Dimethylbenzene⁃Cyanate Esters/Epoxy Resin Curing System ［J］. Thermosetting Resin， 2012（5）：19⁃21.
37	ZHANG S， LI X D， FAN H J， et al. Epoxy Nanocomposites： Improved Thermal and Dielectric Properties by Benzoxazinyl Modified Polyhedral Oligomeric Silsesquioxane［J］. Materials Chemistry and Physics， 2018，doi：10.1016/j.matchemphys.2018.10.048.
38	叶伦学，唐文东，黄杰. 一种新型低羟基含磷环氧的合成及性能研究［J］. 覆铜板资讯， 2019， 118（1）：34⁃38.
	YE L X， TANG W D， HUANG J. Synthesis and Properties of a New Low Hydroxy Phosphorous Epoxy［J］. Copper Clad Laminate Information， 2019， 118（1）：34⁃38.
39	ZHAO D， YUAN L， LIANG G Z， et al. Orientating Carbon Nanotube Bundles and Barium Titanate Nanofibers in Tri⁃Layer Structure to Develop High Energy Density Epoxy Resin Composites with Greatly Improved Dielectric Constant and Breakdown Strength［J］. Composites， 2019， 173：107030.
40	WANG B， LIU L， HUANG L， et al. Fabrication and Origin of High⁃k Carbon Nanotube/Epoxy Composites with Low Dielectric Loss Through Layer⁃by⁃Layer Casting Technique［J］. Carbon， 2015， 85：28⁃37.

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