Zincophilic Anionic Hydrogel Electrolyte with Interfacial Specific Adsorption of Solvation Structures for Durable Zinc Ion Hybrid Supercapacitors

Abstract

The rechargeable zinc ion hybrid supercapacitors (ZHSCs) are critically hindered by the low Coulombic efficiency and poor lifespan due to the continuous water‐induced side reactions and uncontrolled dendrite growth of the Zn anode. Herein, a zincophilic anionic hydrogel electrolyte (PSCA/Zn(OTf)2) is constructed by incorporating the dodecyl sulfate anions ((OSO3R)−) micelles to manipulate the solvation structures of Zn2+ cations via the moderate ion–ion coordination interactions for manipulating the Zn deposition behavior and interfacial chemistry on Zn electrode. Joint experimental and theoretical results show that the constructed solvated Zn2+ cations with the ionized (OSO3R)− electron donor significantly restrict the occurrence of adverse reactions (hydrogen evolution reactions). Concomitantly, the newly involved (OSO3R)− anions influence the adsorption configurations of solvated Zn2+ ions, which alter the electrocrystallization patterns for dendrite‐free growth and induce the oriented deposition for rapid reaction kinetics of Zn electrodes. As a proof of concept, the Zn||Zn symmetric cells with PSCA/Zn(OTf)2 exhibit high reversibility for deposition/stripping behavior with an extended long cycle span. Significantly, benefiting from the synergy of the modulatory electrolyte environment and the regulated adsorption configurations, a quasi‐solid‐state Zn||PSCA/Zn(OTf)2||N‐doped porous carbon material (NPC) ZHSC exhibits exceptional cycling stability for over 40 000 cycles with a low capacity decay (0.00027% per cycle).

Wood-based electrolyte with reversible phase transition for smart thermal-shutdown self-protection

“…Natural balsa wood was chosen as substrate because of its lightweight, well-aligned channels and gradient-porosity. 26,27 After delignification, DW had higher charge density, better electrochemical stability, as well as higher hydrophilicity and specific surface area (Fig. S1, S2 and Table S2†), which improved the bonding force and electrochemical performance of the electrolyte.…”

Multiresponsive Bilayer Hydrogel Actuator with Switchable Shape Morphing Capability and Visible Color/Fluorescence Change

“…Therefore, some of the SMA can be assembled into OP-10 through hydrophobic interactions and become encapsulated within the micelles. Consequently, after the free radical polymerization, the PSMA segments formed and penetrated through the OP-10 micelle. , Then, the thermal- and pH- responsive monomer DMAEMA (for volume change), hydrophilic monomer AM, and pH-responsive monomer VPES (for visible color variation) were added to the DPM solution along with the initiator and cross-linking agent (PEGDA) followed by thermal polymerization under room temperature for 1 h to prepare the PADS@DPM hydrogel as the first layer. Subsequently, a reactant solution containing NIPAM, DMAEMA, the initiator, and the cross-linking agent was injected into the mold to form the second PND layer.…”

Gel polymer electrolytes for rechargeable batteries toward wide-temperature applications

“…To address this, regulating the solvation structure and thereby the ion transport behavior by structuring/functionalizing the polymer matrix is attracting soaring interest in the GPE research community. 205,206 Chen's group suggested that the interaction between DMF-dehydrofluorinated PVDF and the [DMF–Li + ] complex promotes the charge carrier along PVDF segmental chains (Fig. 9(a1)).…”

“…11(b 1 )). 84,206,229,241 For example, Luo and co-workers developed a GPE composed of 0.5 M NaPF 6 /diglyme in polymerized 1,3-dioxolane (poly-DOL). They indicated that the poly-DOL segments in the GPE help to weaken the interaction between Na + ions and diglyme solvents and confine the PF 6 − anions.…”