Dielectric elastomer generators (DEGs) based on silicone rubber composites have received considerable attention in recent years. However, the addition of traditional rigid dielectric fillers not only increases the modulus of composites but also leads to interface debonding between the filler and elastomer matrix under high stretching conditions, thereby limiting the energy harvesting performance. Here, gel-like ester group grafted butadiene rubber (GEBR) with a relatively low modulus was synthesized and used as a “soft filler” to enhance energy harvesting performance of PMVS-based DE composites. The GEBR filler with a high concentration of polar groups could lead to an increase in the dielectric constant of GEBR/PMVS composites by the introduction of interfacial polarizability and the improvement of dipole polarizability. Most notably, compared with TiO2 as the rigid filler, the combination of GEBR's deformability under stretching and strong interfacial interaction between the GEBR filler and PMVS matrix could effectively prevent weak interface formation under high strain conditions, and thus hinder the propagation of electrical treeing. As a result, benefiting from the GEBR filler with a low modulus, 5 vol% GEBR/PMVS DEG exhibits an excellent maximal energy density (65.4 mJ g−1) and outstanding power conversion efficiency (38.4%), achieving a high energy density at relatively low input mechanical force. This study presents a pioneering methodology to fabricate high-performance all-organic DE composites for DEGs through designing a soft dielectric filler with exceptional deformability under stretching.
Composite polymer solid electrolytes (CPEs), possessing good rigid flexible, are expected to be used in solid-state lithium-metal batteries. The integration of fillers into polymer matrices emerges as a dominant strategy to improve Li + transport and form a Li + -conducting electrode–electrolyte interface. However, challenges arise as traditional fillers: 1) inorganic fillers, characterized by high interfacial energy, induce agglomeration; 2) organic fillers, with elevated crystallinity, impede intrinsic ionic conductivity, both severely hindering Li + migration. Here, a concept of super-ionic conductor soft filler, utilizing a Li + conductivity nanocellulose (Li-NC) as a model, is introduced which exhibits super-ionic conductivity. Li-NC anchors anions, and enhances Li + transport speed, and assists in the integration of cathode–electrolyte electrodes for room temperature solid-state batteries. The tough dual-channel Li + transport electrolyte (TDCT) with Li-NC and polyvinylidene fluoride (PVDF) demonstrates a high Li + transfer number (0.79) due to the synergistic coordination mechanism in Li + transport. Integrated electrodes’ design enables stable performance in LiNi 0.5 Co 0.2 Mn 0.3 O 2 |Li cells, with 720 cycles at 0.5 C, and 88.8% capacity retention. Furthermore, the lifespan of Li|TDCT|Li cells over 4000 h and Li-rich Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 |Li cells exhibits excellent performance, proving the practical application potential of soft filler for high energy density solid-state lithium-metal batteries at room temperature.
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