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High performance polymer dielectrics are a key component for printed electronics. In this work, organo-soluble polymers of intrinsic microporosity (PIMs) are reported for the first time to demonstrate desirable dielectric properties with a high permittivity (or κ ), heat resistance, and low dielectric loss simultaneously. Due to the highly dipolar sulfonyl side groups (4.5 D) and rigid contorted polymer backbone, a sulfonylated PIM (SO 2 -PIM) enabled friction-free rotation of sulfonyl dipoles in the nanopores. As such, an optimal balance between relatively high κ and low dielectric loss is achieved in a broad temperature window (−50–200 °C). For example, the discharged energy density reached 17 J cm −3 with κ = 6.0. The discharge efficiency was 94% at 150 °C/300 MV m −1 and 88% at 200 °C/200 MV m −1 . Furthermore, its application as a high- κ gate dielectric in field effect transistors (FETs) is demonstrated. With the bilayer SO 2 -PIM/SiO 2 gate dielectric, InSe FETs exhibited a high electron mobility in the range of 200–400 cm 2 V −1 s −1 , as compared to 40 cm 2 V −1 s −1 for the bare SiO 2 -gated InSe FET. This study indicates that highly dipolar PIMs with a rigid polymer backbone and large free volume are promising as next generation gate dielectric materials for printed electronics. 

A new class of high‐temperature dipolar polymers based on sulfonylated poly(2,6‐dimethyl‐1,4‐phenylene oxide) (SO₂‐PPO) was synthesized by post‐polymer functionalization. Owing to the efficient rotation of highly polar methylsulfonyl side groups below the glass transition temperature (T_g≈220 °C), the dipolar polarization of these SO₂‐PPOs was enhanced, and thus the dielectric constant was high. Consequently, the discharge energy density reached up to 22 J cm⁻³. Owing to its highT_g , the SO₂‐PPO₂₅sample also exhibited a low dielectric loss. For example, the dissipation factor (tan δ) was 0.003, and the discharge efficiency at 800 MV m⁻¹was 92 %. Therefore, these dipolar glass polymers are promising for high‐temperature, high‐energy‐density, and low‐loss electrical energy storage applications.

 

A new class of high‐temperature dipolar polymers based on sulfonylated poly(2,6‐dimethyl‐1,4‐phenylene oxide) (SO₂‐PPO) was synthesized by post‐polymer functionalization. Owing to the efficient rotation of highly polar methylsulfonyl side groups below the glass transition temperature (T_g≈220 °C), the dipolar polarization of these SO₂‐PPOs was enhanced, and thus the dielectric constant was high. Consequently, the discharge energy density reached up to 22 J cm⁻³. Owing to its highT_g , the SO₂‐PPO₂₅sample also exhibited a low dielectric loss. For example, the dissipation factor (tan δ) was 0.003, and the discharge efficiency at 800 MV m⁻¹was 92 %. Therefore, these dipolar glass polymers are promising for high‐temperature, high‐energy‐density, and low‐loss electrical energy storage applications.