Polymer dielectrics, with advanced dielectric properties and heat resistance, are critical for high‐temperature capacitors in various applications. However, the high performance of heat resistance and dielectric properties are quite difficult to achieve all together due to their mutual implication. Here, by intensively investigating the correlation between molecular structure and properties, polyimide dielectrics with i) enhanced dielectric constant by introducing sulfonyl group, ii) low dissipation factor by introducing flexible linkage, and iii) high Tg
(glass transition temperature) by retaining an aromatic structure, are obtained. The sulfonyl‐containing polyimides with different flexible linkages exhibit simultaneously a high dielectric constant (4.50–5.98), low dissipation factor (0.00298–0.00426), and outstanding breakdown strength (most above 500 MV m−1), as well as superior heat resistance (Tg
: 244–304 °C). Specifically, the polyimide (SPI‐1) with sulfonyl group in diamine moiety and para‐para linkage shows stable dielectric properties up to 150 °C, and the discharged energy density and charge–discharge efficiency can be as high as 7.04 J cm−3 and 91.3% at 500 MV m−1, respectively.
Polymer dielectrics with outstanding heat resistance and advanced dielectric properties are of great importance for hightemperature capacitors in the applications of hostile circumstances. In this work, a series of aromatic carbonyl-containing polyimides (CPI) are prepared from the carbonyl dianhydride and different diamines. The correlation between molecular structure (i.e., different linked structure ( O , CH2 , SO2 ) in diamines, the length of repeating unit and the linked position (para-para or meta-meta), and properties is revealed in detail to obtain CPI dielectrics with excellent thermal resistance (glass transition temperature, T g : 241~352 C), reasonably high dielectric constant (3.99~5.23), low dissipation factor (0.00307~0.00395), and admirable breakdown strength (425~552 MV/m) simultaneously. Particularly, CPI-5 with carbonyl structure in dianhydride and sulfonyl group in diamine proves to exhibit discharged energy density and charge-discharge efficiency of 6.34 J/cm 3 and 92.3% at 500 MV/m, respectively. In addition, CPI-5 also displays stable dielectric properties in temperature range of −50-200 C.
Flexible high‐temperature polymeric dielectrics with advanced dielectric properties are urgently demanded in various applications. In this work, series of polymer blend films were prepared from aromatic polythiourea (ArPTU) and polyimide (PI). The experimental results revealed that the blend films were properly engineered to achieve higher breakdown strength, greater dielectric constant, and larger energy density than pure PI film. For instance, the optimum property was obtained from the blend film with 10 wt% ArPTU, exhibiting prominent dielectric properties (K = 4.52, Eb = 443 MV/m), enhanced energy density (4.00 J/cm3) as well as excellent heat resistance (Tg = 419°C). In addition, stable dielectric properties at broad temperature range from −50 to 250°C were also acquired. It is deduced that the good compatibility from ArPTU and PI with similar polarity are responsible for the improved properties. The superior comprehensive properties which combine the advantages of ArPTU and PI suggest the potential applications of ArPTU/PI blend film in high‐temperature dielectric areas.
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