No abstract

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.

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.

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.