金属有机框架包覆铁电二维纳米片增强聚醚酰亚胺复合介质高温储能性能研究

doi:10.19595/j.cnki.1000-6753.tces.240437

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摘要

聚合物基电介质中有机相与无机相间的界面层的理化性质显著影响其储能特性,然而现有研究中多利用有机或无机组分的界面层来提高有机相与无机相间的相容性。该文在高介电常数铌酸钙（CNO）纳米片表面成功地包覆了一层多孔结晶的金属有机框架层（MOF）,聚合物基体中的分子链可在MOF的多孔结构中三维穿插与化学键合,形成的界面层可缓和填料和基体间电性能的不匹配,抑制无机填料和有机基体直接接触导致的载流子聚集,有效地降低了在复合电介质薄膜高温下工作时的电导损耗,提高了150℃工作时的击穿场强和能量存储能力。尤其是填充质量分数为0.2%的PEI/CNO@MOF复合电介质在150℃工作时的放电能量密度可达3.5 J/cm³,同时充电-放电效率大于90%,具有潜在的实际应用价值。该文不仅提供了一种简便有效的高温界面设计策略,同时也为设计高储能特性聚合物电介质提供了技术范本。

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关键词 ：聚合物电介质, 复合材料, 金属有机框架, 电容储能

Abstract：

Polymer film capacitors find wide use in vehicle inverters and wind power due to their fast charge and discharge rates. However, evolving needs, like high-temperature oil and gas exploration, demand advancements. Current Biaxially-oriented Polypropylene (BOPP) capacitors face limitations due to low polarity and temperature constraints. Developing polymer composite film capacitors with high energy density under heat is urgently needed. Directly filling nanosheets into polymers shows promise for its simplicity, enhanced polarization, and scalability, thus extensively researched.
Due to the size effect, there exists a significant number of inorganic-organic interfaces between existing inorganic fillers and polymers, this widespread interface in polymer-based composite dielectrics is considered to be a decisive factor affecting energy storage characteristics. However, the substantial disparity in surface compatibility and physical-chemical properties between inorganic fillers and organic polymer impedes the achievement of high application electric fields and discharge energy densities in directly filled polymer composite dielectrics. In this study, to prevent direct contact between inorganic filler calcium niobate nanosheets (CNO) and the molecular chains of organic polymer polyetherimide (PEI), a porous crystalline metal-organic framework (MOF) was employed to encapsulate the CNO. The resulting CNO@MOF complex was then incorporated into PEI to establish an inorganic-organic interface, with MOF serving as the transitional medium. The three-dimensional interpenetration and chemical bonding between MOF and PEI effectively enhance filler-polymer compatibility. For example, under transmission electron microscopy (TEM), no nanoscale defects or pores were observed between CNO and PEI. To further confirm the chemical interaction between MOF and PEI, synchrotron radiation X-ray absorption fine structure spectroscopy revealed the Zn—C coordination environment between MOF and PEI, validating the chemical interaction between the two materials. Based on the characterization results, the physicochemical properties of MOF as a transitional interface between inorganic and organic phases were comprehensively ascertained.
Moreover, the incorporation of inorganic fillers significantly boosts the dielectric constant of the composite films while suppressing the loss tangent under periodic electric fields. The optimized composite film featuring this interface achieves a breakdown field (E_b) of 484 MV/m at 150℃, representing a 21% increase over pure PEI. Leakage current density tests and hysteresis loop tests confirm that polymer composite dielectrics exhibit lower current density and energy loss under applied electric fields. Ultimately, the best-performing composite film achieves a discharge energy density of 3.5 J/cm³, with a charge-discharge efficiency of 90%. By combining the characterization of interface structure with experimental results, this paper proposes a transition interface design methodology that effectively enhances the capacitive capabilities of polymer matrix composite dielectric films under high-temperature, high-electric field conditions, offering a reliable strategy and direction for the development of high-performance polymer capacitors.

Key words： Polymer dielectrics composite metal-organic framework capacitive energy storage

收稿日期: 2024-03-19

PACS:

TM211

通讯作者: 刘晓旭男,1982年生,教授,博士生导师,研究方向为聚合物电介质储能。E-mail：xiaoxuliu@sust.edu.cn

作者简介: 陈东洋男,2000年生,硕士研究生,研究方向为聚合物电介质储能。E-mail：chendongyang@sust.edu.cn

引用本文:

陈东洋, 刘晓旭, 孙家明, 陈皓男, 尤晓光. 金属有机框架包覆铁电二维纳米片增强聚醚酰亚胺复合介质高温储能性能研究[J]. 电工技术学报, 0, (): 2492928-2492928. Chen Dongyang, Liu Xiaoxu, Sun Jiaming, Chen Haonan, You Xiaoguang. High Temperature Energy Storage Performance Enhanced by Metal-Organic Frame Coated Ferroelectric Two-Dimensional Nanosheets Filled with Polyetherimide Composite Dielectric. Transactions of China Electrotechnical Society, 0, (): 2492928-2492928.

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