While the thermoelectric (TE) generator has attracted tremendous attention, the development of wearable TE generators with stretchability and self-healability has been a significant challenge. Herein, we report intrinsically self-healable and stretchable ternary ionic TE hybrid materials, composed of a conjugated polymer (polyaniline), a non-conjugated anionic polyelectrolyte (poly(2-acrylamido-2-methyl-1-propanesulfonic acid)), and phytic acid. The proposed materials exhibit an excellent ionic figure-of-merit (ZT_i) as well as remarkable stretchability (up to ∼750%) and autonomous self-healability without any external stimuli. The ionic TE performance was sustainable under severe deformation (50% strain) and multiple self-healing processes (30 cycles), which is the first demonstration of such performance. The ZT_i of the stretchable and self-healable ternary TE hybrids is 1.04. Moreover, a self-healable and stretchable ionic thermoelectric capacitor device is also demonstrated using the ternary TE hybrid.

Silicon (Si) is a promising anode material for lithium‐ion batteries (LIBs) owing to its tremendously high theoretical storage capacity (4200 mAh g⁻¹), which has the potential to elevate the energy of LIBs. However, Si anodes exhibit severe volume change during lithiation/delithiation processes, resulting in anode pulverization and delamination with detrimental growth of solid electrolyte interface layers. As a result, the cycling stability of Si anodes is insufficient for commercialization in LIBs. Polymeric binders can play critical roles in Si anodes by affecting their cycling stability, although they occupy a small portion of the electrodes. This review introduces crucial factors influencing polymeric binders' properties and the electrochemical performance of Si anodes. In particular, we emphasize the structure–property relationships of binders in the context of molecular design strategy, functional groups, types of interactions, and functionalities of binders. Furthermore, binders with additional functionalities, such as electrical conductivity and self‐healability, are extensively discussed, with an emphasis on the binder design principle.

In this study, we develop a stretchable/self-healable polymer, PEDOT:PAAMPSA:PA, with remarkably high ionic thermoelectric (iTE) properties: an ionic figure-of-merit of 12.3 at 70% relative humidity (RH). The iTE properties of PEDOT:PAAMPSA:PA are optimized by controlling the ion carrier concentration, ion diffusion coefficient, and Eastman entropy, and high stretchability and self-healing ability are achieved based on the dynamic interactions between the components. Moreover, the iTE properties are retained under repeated mechanical stress (30 cycles of self-healing and 50 cycles of stretching). An ionic thermoelectric capacitor (ITEC) device using PEDOT:PAAMPSA:PA achieves a maximum power output and energy density of 4.59 μW‧m⁻² and 1.95 mJ‧m⁻², respectively, at a load resistance of 10 KΩ, and a 9-pair ITEC module produces a voltage output of 0.37 V‧K⁻¹ with a maximum power output of 0.21 μW‧m⁻² and energy density of 0.35 mJ‧m⁻² at 80% RH, demonstrating the potential for a self-powering source.