This work addresses the preparation of new polymer dielectrics working under the dipolar glass polymer (DGP) concept. Herein, we report the synthesis and characterization of four hetero-functionalized polyitaconates bearing sulfones as high dipole moment entities and norbornane or adamantane structures responsible for increasing the glass transition temperature (Tg) and thus the range of temperatures where they can work without degrading or showing high energy dissipation. As a result, all obtained polymers exhibited dielectric constants (εr’) between 5.1 and 6.2 while presenting low loss factors (Tan(δ) < 0.01), reaching the status of high-dielectric polymers with a low dissipative behavior. In addition, it was demonstrated that including bulky structures into their polymer backbone allows for an increase of up to 80 °C in their working temperature ranges, expanding the temperature range where they behave as DGPs in an outstanding manner. A complete structural, thermal and dielectric characterization was carried out in terms of infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), thermogravimetry (TGA), differential scanning calorimetry (DSC) and broad dielectric spectroscopy (BDS). Overall, these materials seem to fulfill the basic requirements to be considered good candidates for dielectric applications such as energy storage, confirming the versatility of polyitaconate-based materials.

The Polymers & Soft Matter team acknowledges the funding provided by Grant No. PID2021-123438NB-I00 from MCIN/AEI/10.13039/501100011033, as well as the support from “ERDF A way of making Europe,” Grant No. TED2021-130107 A-I00, also funded by MCIN/AEI/10.13039/501100011033, and Unión Europea “NextGenerationEU/PRTR.” Additionally, we acknowledge the financial support from Eusko Jaurlaritza under code: IT1566-22 and Gipuzkoako Foru Aldundia, Programa de Red Guipuzcoana de Ciencia,Tecnología e Innovación, code: 2023-CIEN-000069-01. G. K. thanks to Ministerio de Ciencia, Innovacion y Universidades, grant number PID2021-126417NB-I00 and by the Gobierno Vasco/Eusko Jaurlaritza, grant number IT1690-22. D. D. D. thanks the Spanish Ministry of Science, Innovation and Universities for the grants TED2021-132847B-I00 and PID2019-105391GB-C21 funded by MCIN/AEI/10.13039/501100011033 and NANOtec, INTech, Cabildo de Tenerife and ULL for laboratory facilities.

Peer reviewed