Enabling High‐Energy‐Density High‐Efficiency Ferroelectric Polymer Nanocomposites with Rationally Designed Nanofillers

Abstract

Ferroelectric polymers have been regarded as the preferred matrix for high‐energy‐density dielectric polymer nanocomposites because of their highest dielectric constants among the known polymers. Despite a library of ferroelectric polymer‐based composites having been demonstrated as highly efficient in enhancing the energy density, the charge–discharge efficiency remains moderate because of the high intrinsic loss of ferroelectric polymers. Herein, a systematic study of the oxide nanofillers is presented with varied dielectric constants and the vital role of the dielectric match between the filler and the polymer matrix on the capacitive performance of the ferroelectric polymer composites is revealed. A combined experimental and simulation study is further performed to specifically investigate the effect of the nanofiller morphology on the electrica properties of the polymer nanocomposites. The solution‐processed ferroelectric polymer nanocomposite embedded with Al2O3 nanoplates exhibits markedly improved breakdown strength and discharged energy density along with an exceptional charge–discharge efficiency of 83.4% at 700 MV m−1, which outperforms the ferroelectric polymers and nanocomposites reported to date. This work establishes a facile approach to high‐performance ferroelectric polymer composites through capitalizing on the synergistic effect of the dielectric properties and morphology of the oxide fillers.

High‐Temperature High‐Energy‐Density Dielectric Polymer Nanocomposites Utilizing Inorganic Core–Shell Nanostructured Nanofillers

“…It is evident that the J values of the PEI nanocomposites are significantly reduced upon the addition of inorganic nanoparticles and minimized at 11 vol%, i.e., 1.65 × 10 −8 A cm −2 of PEI/ZrO 2 and 2.51 × 10 −9 A cm −2 of PEI/Al 2 O 3 @ZrO 2 nanocomposites at 150 °C and 150 MV m −1 . The further increase of the filler content leads to the increment in J, which could be attributed to the overlap of the interfacial regions of adjacent nanoparticles that is conducive to charge transport [29,[48][49][50] and responsible for the decreased E b and η values of the polymer composites at relatively high filler loadings. The nearly one order of magnitude lower J of PEI/Al 2 O 3 @ZrO 2 with respect to that of PEI/ ZrO 2 can be further understood from the finite element simulations as shown in Figure S19, Supporting Information.…”

Prediction of Energy Storage Performance in Polymer Composites Using High‐Throughput Stochastic Breakdown Simulation and Machine Learning

“…In addition, additional literature results were used to verify the machine learning results (used as the colored symbols), and the polymer‐based composites parameters used in the additional machine learning are listed in Table S5 (Supporting Information). [ 21 , 39 ] The majority of the data points are located around the black straight line, which indicates that our machine learning can be treated as a predictive model. It should be noted that some of these data points were used for high‐throughput stochastic breakdown simulation and machine learning, while others were outside the database.…”

“…The experimental breakdown strengths of polymer‐based composites are cited from the references. [ 21 , 39 ]…”

“…[ 15 , 16 , 17 , 18 ] A number of possible dielectric breakdown mechanisms and factors of polymer‐based composites have been proposed, including filler ε r , filler size ( d ), and filler content ( v ), but these proposals tend to be limited to single variable, while few of them take into account multiple variables. [ 19 , 20 , 21 , 22 ] Hence, building sensible multiple variables links to gain fundamental insights on dielectric breakdown behaviors is instructive to innovative design of high U polymer‐based composites.…”

Effect of organic Na+‐montmorillonite on the dielectric and energy storage properties of polypropylene nanocomposites with polypropylene‐graft‐maleic anhydride as compatibilizer

“…23,24 According to previous studies, 2D nanofillers commonly behaved much better enhancing effect for the energy storage ability. [25][26][27] Furthermore, among all the 2D nanomaterials, organic montmorillonite (org-MMT) belongs to the cost-effective and efficient modifier for the preparation of dielectric nanocomposites. For example, Tomer prepared org-MMT modified low-density polyethylene (LDPE) and linear LDPE (LLDPE) grafted maleic anhydride (MAH) nanocomposites.…”