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The inherent low dielectric constant of polyimide (PI) dielectrics restricts their applications to become a component of high energy density film capacitors. In this work, double core–shell structured barium titanate@magnesium oxide@polydopamine (BaTiO3@MgO@PDA) nanoparticles were synthesized successfully and utilized as high dielectric constant functional fillers for PIs, in which the insulating MgO layer meliorated dielectric constant difference between BaTiO3 and PI matrix, and the organic PDA layer improved the compatibility between the inorganic fillers and PI matrices. Then, a series of sandwich‐structured PI‐based hybrid films was prepared through a layer‐by‐layer solution casting method. The middle layer of pure PI with excellent insulating properties effectively suppressed charge injection. With the combination of sandwich structure and the BaTiO3@MgO@PDA nanoparticles, the PI hybrid film containing 15 wt% fillers in the outer layers achieved the maximum breakdown strength of 425.68 kV/mm and the maximum energy density of 5.132 J/cm3, which was 68.3% and 413% higher than those of pure PI film, respectively, meanwhile maintained a low dielectric loss value of 0.0083 at 1 kHz. The introduction of BaTiO3@MgO@PDA enhanced the interfacial polarization due to the high barrier energy between adjacent layers preventing the transfer of electrons and weakening the leakage current in the sandwich‐structured composite film. This work demonstrates that an appropriate combination of high dielectric hybrid fillers and multilayer structure can effectively increase the energy storage density of PI substrate for high‐temperature energy storage applications. Highlights: The double core–shell structured BaTiO3@MgO@PDA was synthesized successfully.The sandwich‐structured hybrid films were prepared by layer‐by‐layer method.The energy density of hybrid films reached a high value of 5.132 J/cm3. [ABSTRACT FROM AUTHOR]

Under extreme conditions, the polymer dielectric materials are expected to have good dielectric properties and heat resistance. Polyimide (PI) has high service temperature (>250°C) and low dielectric loss, but its low dielectric constant limits its further application. The addition of MXene can significantly improve the dielectric constant of PI, but the poor compatibility between MXene and weak polar matrix leads to Bénard‐Marangoni (BM) instability in the process of thermal imidization. This issue can be solved by the surface modification of MXene. Therefore, in this work, a new cetyltrimethylammonium bromide (CTAB) decorated MXene/PI nanocomposite film was prepared by in‐situ polymerization. With the addition of 7 wt% MXene@CTAB, the PI nanocomposite shows improved dielectric constant (k = 7.8 at 100 Hz), which is 2.4 times that of pure PI due to the formation of micro‐capacitors structure and Maxwell‐Wagner‐Sillars (MWS) interfacial polarization. Its dielectric loss keeps at an ultra‐low level (0.027 at 100 Hz) while that of 7 wt% MXene/PI nanocomposite is 3.027. It is owing that CTAB inhibits the agglomeration of MXene. In addition, MXene@CTAB/PI composites have excellent thermal stability, good hydrophobicity, and low water absorption. The above properties ensure MXene@CTAB/PI composites wide application in various extreme situations. [ABSTRACT FROM AUTHOR]

Novel fluorine-containing polyimides were synthesized through copolymerization by using 2,3,3′,4′-biphenyltetracarboxylic dianhydride (α-BPDA) and 4,4′-(4,4′-isopropydenediphenox-y) bis-(phthalic anhydride) (BPADA) as dianhydrides and 4,4′-oxydianiline (ODA) and 2,2 - Bis [4-(4-aminophenoxy)phenyl]-hexafluoropropanane (HFBAPP) as diamines. Noncoplanar structure, flexible ether bond, and trifluoromethyl give the polyimide good thermoplastic, solubility, and heat resistance. The glass transition temperatures of polyimide films are 232.5°C∼262.2°C, the 5% weight loss temperatures are 521.5°C∼531.0°C, and the residual mass is more than 50% as heating to 800°C. With the increase of HFBAPP content in diamine, the dielectric constant of the material decreases from 3.21 to 2.78, and the dielectric loss decreases from 0.00962 to 0.00687 at 1 MHz, which greatly improves the dielectric properties of the material. [ABSTRACT FROM AUTHOR]

The advancement of the microelectronics industry necessitates the use of interlayer insulation materials with low dielectric constants and high mechanical properties. In this paper, a new type of copolymerized fluorinated polyimide (PI) is synthesized, and mixed with polyhedral oligomeric silsesquioxane (POSS) functionalized mesoporous silica (MCM‐41@POSS). The PI/MCM‐41@POSS composites exhibit good hydrophobicity. With the addition of 3 wt% MCM‐41@POSS, the PI composite attained an ultralow dielectric constant (k = 1.88) and low dielectric loss (0.01) at 1 MHz, which is attributed to the mesoporous structure of MCM‐41 and the restriction of polarization in the bonded region. The decorated POSS effectively prevents the penetration of PI molecular chains into the mesopores of MCM‐41. In addition, the PI composites containing 3 wt% of MCM‐41@POSS obtain the highest maximum stress of 104.03 MPa with an elongation at break of 13.73%. The hydrophobic PI composites with ultralow‐k are expected to be good candidates as interlayer materials in microelectronics devices. [ABSTRACT FROM AUTHOR]

Polyimide (PI) is considered one of the most promising candidate materials for the microelectronics and wireless communication industries. Nevertheless, the relatively high dielectric constant of PI has become a significant obstacle, constraining its utilization in the realm of microelectronics. Herein, novel PI nanocomposite films were fabricated by incorporating covalent organic frameworks (COFs) and their functionalized counterparts (COF@POSS and COF@DTF) through post-synthetic modification. Among all PI nanocomposites films, PI/COF@POSS nanocomposite film including 2 wt% COF@POSS achieved the lowest dielectric constant (2.41) and dielectric loss (0.0076). These values represented a reduction of 22.5 % and 24 % compared to pure PI, respectively. The decrease in dielectric constant is ascribed to the combined influence of the porous structure of COF and the augmentation in free volume fraction caused by the steric hindrance of POSS. Additionally, the tensile strength of the PI/COF@POSS and PI/COF@DTF nanocomposite films increased up to 121.1 MPa and 112.0 MPa, representing a 95 % and 80 % improvement over pure PI, respectively. Furthermore, the introduction of COFs functionalized with POSS and DTF significantly enhanced the hydrophobicity of PI nanocomposite films. The combination of porous organic nanofillers with surface functionalization offers a feasible route to create low-k PI nanocomposite films with improved mechanical properties and hydrophobicity. The PI nanocomposite films with functional covalent organic frameworks exhibited the decreased dielectric constant and dielectric loss with improved mechanical performance. [Display omitted] • The novel low dielectric PI films were obtained by adding functional COFs. • PI/COF@POSS films achieved the lowest dielectric constant of 2.41. • The maximum tensile strength of PI/COF@POSS films reaches 121.1 MPa. • The hydrophobicity of PI/COF@DTF films is greatly improved. [ABSTRACT FROM AUTHOR]

Nowadays, polyimide (PI) with low dielectric constant is expected to be widely applied in microelectronics. For this reason, hollow glass microspheres (HGM) modified by silane coupling agent KH‐550 (K‐HGM), a series of HGM/PI and K‐HGM/PI composite films with excellent thermal performance, hydrophobic and low dielectric constant were fabricated by in situ polymerization. The effect of HGM/K‐HGM content on the properties of composite films was studied. The superior heat resistance of HGM can improve the thermal performance of composite films. Due to silane coupling agent KH‐550, K‐HGM exhibits a good interfacial compatibility with PI matrix and forms an interfacial adhesion region. With the HGM loading of 6%, comparing with pure PI films, the glass transition temperatures (Tg) of composite films were dramatically increased by 32.3°C. Especially, the low dielectric constant of 2.21 and dielectric loss of 0.0059 at 1 MHz were obtained for the PI/K‐HGM composite film with addition of 8 wt%. Thus, PI/K‐HGM composite films show more excellent performance. The current work provides a promising solution for fabrication of PI with low dielectric constant and superior thermal performance that may be applied in microelectronics industry. [ABSTRACT FROM AUTHOR]

The all organic PI composites with size adjustable hollow polydopamine microspheres (H-PDA) exhibited decreased the dielectric constant and dielectric loss with enhanced mechanical performance. [Display omitted] • The ultra-low dielectric polyimide composites with hollow polydopamine microspheres were successfully synthesized. • The PI/H-PDA composite achieved the ultra-low dielectric constant of 1.96 with a dielectric loss of 0.0123 at 1 MHz. • The PI/H-PDA composites possessed excellent thermal stability and mechanical properties. Polydopamine (PDA) has been extensively investigated due to its excellent adhesion ability and versatile chemical potential for secondary reactions. However, the potential application of hollow polydopamine microspheres (H-PDA) in the field of low-dielectric electronic packaging remains an unexplored area. Here, H-PDA microspheres with adjustable size were synthesized by a template-assisted approach, and the influence of size and content of H-PDA on the comprehensive performance of PI/H-PDA composites was explored in detail. The morphology observation revealed that the presence of H-PDA could be homogeneously dispersed in the PI matrix, and the PI/H-PDA composite containing 2 wt% H-PDA-800 achieved the lowest dielectric constant of 1.96 with a dielectric loss of 0.0123 at 1 MHz. It was attributed to the synergistic effects of nano-sized air bubbles from H-PDA and the dielectric confinement effect. Meanwhile, PI/H-PDA composites maintained high thermal stability (T 5 > 517 °C). In addition, the incorporation of H-PDA had a strengthening and toughening effect on PI composites, which can be explained by the sliding theory of macromolecular chains. This work offers a feasible strategy to obtain ultra-low dielectric constant of porous PI composites while maintaining good mechanical properties and thermal stability. [ABSTRACT FROM AUTHOR]