高热稳定性聚芳醚腈电介质薄膜的制备与性能研究
发布时间：2019-02-26 12:48
【摘要】：随着电子信息产业的飞速发展对设备集成化、小型化及可携带化的要求,这就对目前的材料行业提出了新的课题,制备更先进的材料来满足先进设备制造对材料的要求。对于电子产品来说电介质材料是直接影响元器件性能的因素。聚芳醚腈是一种具有杰出性能的特种功能材料,能够应用于社会生活生产的许多方面,高绝缘性、高热稳定性以及优异的介电性能使其在电容器及储能薄膜电容器等电子元器件制造方面有巨大的应用潜力。因此为了拓宽聚芳醚腈的应用,本文通过化学及物理方法对聚芳醚腈基材料的性能进行优化以期能实现在上述方面的实际应用。首先,本文合成了可交联型聚芳醚腈。由于链端邻苯二甲腈在加热或催化条件下会发生成环反应,因此我们通过热交联及加入三官能度邻苯二甲腈作交联剂制备了交联聚芳醚腈薄膜。并通过DSC、TGA、DMA及TMA证明了其具有介电性能-频率、温度、时间以及工作循环稳定性,并证明其能够在宽频范围(100 Hz-200kHz)、宽温度范围(20-350 oC)以及长时间使用并具有优异的可靠性。铁电性测试证明交联聚芳醚腈是典型的线性电介质并且在高温下具有稳定的储能特性。其次,由于聚芳醚腈交联条件苛刻限制了其的制备及应用,因此通过水热法制备了纳米氧化锌晶须(ZnO-nws)并将其作为交联催化剂加入到聚芳醚腈基体中,并研究了其对聚芳醚腈交联反应的催化剂作用以及对交联聚芳醚腈薄膜的交联度、热稳定性、力学性能、介电性能以及储能特性等的影响。通过研究发现纳米氧化锌晶须对交联反应有明显的催化作用可以有效的优化交联工艺并且可以在保证介电性能-温度稳定性的前提下提高介电常数,实现更高的储能密度。最后,为提高交联聚芳醚腈薄膜的介电常数,我们制备了核壳锆酸铅包裹钛酸钡纳米粒子,并作为高介电填料制备了复合高介电聚芳醚腈薄膜。通过对交联度、热稳定性、介电性能及储能特性的研究发现纳米粒子加入不会破坏薄膜的热稳定及介电性能-温度稳定性,并且在提高介电常数的同时保持击穿强度最终实现交联薄膜储能密度的提高,使其在优化的交联工艺条件下得到高介电的交联薄膜。通过本研究表明,交联聚芳醚腈具有极其优异的综合性能,特别是介电性能-温度稳定性以及通过改性使其具有优异的加工性及高介电常数与储能密度使其在薄膜电容器以及储能薄膜电容器方面具有巨大的应用潜力。
[Abstract]:With the rapid development of electronic and information industry, the requirements of equipment integration, miniaturization and portability have been put forward, which puts forward a new subject for the current material industry, and the preparation of more advanced materials to meet the requirements of advanced equipment manufacturing for materials. For electronic products, dielectric materials are the factors that directly affect the performance of components. Poly (aryl ether nitrile) is a special functional material with outstanding properties, which can be used in many aspects of social life, high insulation, High thermal stability and excellent dielectric properties have great potential applications in the manufacture of electronic components such as capacitors and energy storage thin film capacitors. Therefore, in order to broaden the application of poly (aryl ether nitrile), the properties of poly (aryl ether nitrile) based materials were optimized by chemical and physical methods in order to realize the practical application in the above aspects. Firstly, crosslinked poly (aryl ether nitrile) was synthesized. Because the chain-terminated phthalonitrile can be cyclized under heating or catalytic conditions, the crosslinked poly (aryl ether nitrile) thin films were prepared by thermal crosslinking and adding trifunctional phthalonitrile as cross-linking agent. The dielectric properties-frequency, temperature, time and working cycle stability have been proved by DSC,TGA,DMA and TMA, and it has been proved that it can be used in the wide band range (100 Hz-200kHz). Wide temperature range (20? 350 oC) and long-term use with excellent reliability. Ferroelectricity tests show that crosslinked poly (aryl ether nitrile) is a typical linear dielectrics and has stable energy storage characteristics at high temperatures. Secondly, the preparation and application of poly (aryl ether nitrile) crosslinked were restricted by severe conditions, so nano-zinc oxide whiskers (ZnO-nws) were prepared by hydrothermal method and added into poly (aryl ether nitrile) matrix as cross-linking catalyst. The effect of the catalyst on the crosslinking reaction of poly (aryl ether nitrile) and the cross-linking degree, thermal stability, mechanical properties, dielectric properties and energy storage characteristics of the crosslinked poly (aryl ether nitrile) film were also studied. It is found that the nano-ZnO whisker can effectively optimize the crosslinking process and improve the dielectric constant and achieve a higher energy storage density under the premise of ensuring the dielectric property-temperature stability. Finally, in order to improve the dielectric constant of crosslinked poly (aryl ether nitrile) films, core-shell lead zirconate-coated barium titanate nanoparticles were prepared and composite high dielectric polyether nitrile thin films were prepared as high dielectric fillers. It is found that the addition of nano-particles does not destroy the thermal stability and dielectric properties-temperature stability of the thin films by studying the crosslinking degree, thermal stability, dielectric properties and energy storage properties of the films. At the same time, the dielectric constant is increased while the breakdown strength is maintained. Finally, the energy storage density of the cross-linked film is improved, and the high dielectric cross-linking film is obtained under the optimized crosslinking conditions. The results show that the crosslinked poly (aryl ether nitrile) has excellent comprehensive properties. Especially the dielectric properties-temperature stability and its excellent processability and high dielectric constant and energy storage density make it have great potential applications in thin-film capacitors and energy-storage thin-film capacitors.
【学位授予单位】：电子科技大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB383.2
本文编号：2430784
[Abstract]:With the rapid development of electronic and information industry, the requirements of equipment integration, miniaturization and portability have been put forward, which puts forward a new subject for the current material industry, and the preparation of more advanced materials to meet the requirements of advanced equipment manufacturing for materials. For electronic products, dielectric materials are the factors that directly affect the performance of components. Poly (aryl ether nitrile) is a special functional material with outstanding properties, which can be used in many aspects of social life, high insulation, High thermal stability and excellent dielectric properties have great potential applications in the manufacture of electronic components such as capacitors and energy storage thin film capacitors. Therefore, in order to broaden the application of poly (aryl ether nitrile), the properties of poly (aryl ether nitrile) based materials were optimized by chemical and physical methods in order to realize the practical application in the above aspects. Firstly, crosslinked poly (aryl ether nitrile) was synthesized. Because the chain-terminated phthalonitrile can be cyclized under heating or catalytic conditions, the crosslinked poly (aryl ether nitrile) thin films were prepared by thermal crosslinking and adding trifunctional phthalonitrile as cross-linking agent. The dielectric properties-frequency, temperature, time and working cycle stability have been proved by DSC,TGA,DMA and TMA, and it has been proved that it can be used in the wide band range (100 Hz-200kHz). Wide temperature range (20? 350 oC) and long-term use with excellent reliability. Ferroelectricity tests show that crosslinked poly (aryl ether nitrile) is a typical linear dielectrics and has stable energy storage characteristics at high temperatures. Secondly, the preparation and application of poly (aryl ether nitrile) crosslinked were restricted by severe conditions, so nano-zinc oxide whiskers (ZnO-nws) were prepared by hydrothermal method and added into poly (aryl ether nitrile) matrix as cross-linking catalyst. The effect of the catalyst on the crosslinking reaction of poly (aryl ether nitrile) and the cross-linking degree, thermal stability, mechanical properties, dielectric properties and energy storage characteristics of the crosslinked poly (aryl ether nitrile) film were also studied. It is found that the nano-ZnO whisker can effectively optimize the crosslinking process and improve the dielectric constant and achieve a higher energy storage density under the premise of ensuring the dielectric property-temperature stability. Finally, in order to improve the dielectric constant of crosslinked poly (aryl ether nitrile) films, core-shell lead zirconate-coated barium titanate nanoparticles were prepared and composite high dielectric polyether nitrile thin films were prepared as high dielectric fillers. It is found that the addition of nano-particles does not destroy the thermal stability and dielectric properties-temperature stability of the thin films by studying the crosslinking degree, thermal stability, dielectric properties and energy storage properties of the films. At the same time, the dielectric constant is increased while the breakdown strength is maintained. Finally, the energy storage density of the cross-linked film is improved, and the high dielectric cross-linking film is obtained under the optimized crosslinking conditions. The results show that the crosslinked poly (aryl ether nitrile) has excellent comprehensive properties. Especially the dielectric properties-temperature stability and its excellent processability and high dielectric constant and energy storage density make it have great potential applications in thin-film capacitors and energy-storage thin-film capacitors.
【学位授予单位】：电子科技大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TB383.2
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