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The performance of lithium–sulfur (Li–S) batteries is greatly hindered by the notorious shuttle effect of lithium polysulfides (LiPSs). To address this issue, in situ topochemical oxidation derivative TiC@carbon‐included TiO2 (TiC@C‐TiO2) core–shell composite is designed and proposed as a multifunctional sulfur host, which integrates the merits of conductive TiC core to facilitate the redox reaction kinetics of sulfur species, and porous C‐TiO2 shell to suppress the dissolution and shuttling of LiPSs through chemisorption. A unique dual chemical mediation mechanism is demonstrated for the proposed TiC@C‐TiO2 composite that synergistically entraps LiPSs through thiosulfate/polythionate conversion coupled with strong polar–polar interaction. The morphological characterization reveals that the TiC@C‐TiO2‐based cathode can well regulate the distribution of electrode materials to retard their accumulation inside the electrode, ensuring effective contact between the active materials and electrolyte. Based on its unique function and structure, the cathode delivers an improved capacity of 1256 mAh g−1 at 0.2C, a remarkable rate capability of 643 mAh g−1, and an ultralow capacity decay rate of 0.065% per cycle at 2C over 900 cycles. This work not only demonstrates a dual chemical mediation mechanism to immobilize LiPSs, but also provides a universal strategy to construct multifunctional sulfur hosts for advanced Li–S batteries.

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Utilizing ionic liquids (ILs) with low flammability as the precursor component for a gel polymer electrolyte is a smart strategy out of safety concerns. Solvate ionic liquids (SILs) consist of equimolar lithium bis­(trifluoromethylsulfonyl)­imide and tetraglyme, alleviating the main problems of high viscosity and low Li+ conductivity of conventional ILs. In this study, within a very short time of 30 s, a SIL turns immobile using efficient and controllable UV-curing with an ethoxylated trimethylolpropane triacrylate (ETPTA) network, forming a homogeneous SIL-based gel polymer electrolyte (SGPE) with enhanced thermal stability (216 °C), robust mechanical strength (compression modulus: 1.701 MPa), and high ionic conductivity (0.63 mS cm–1 at room temperature). A Li|SGPE|LiFePO4 cell demonstrates high charge/discharge reversibility and cycling stability with a capacity retention rate of 99.7% after 750 cycles and an average Coulombic efficiency of 99.7%, owing to its excellent electrochemical compatibility with Li-metal. A close-contact electrode/electrolyte interface is formed by in situ curing of the electrolyte on the electrode surface, which enables the pouch full cell to work stably under the conditions of cutting/bending. In view of the excellent mechanical, thermal, and electrochemical performances of SGPE, it is believed to be a promising gel polymer electrolyte for constructing high-safety lithium-ion batteries (LIBs).

Miniaturized and flexible power resources such as supercapacitors with resistance of high voltage play a critical role as potential energy storage devices for implantable and portable electronics because of their convenience, high power density, and long-term stability. Herein, we propose a novel strategy for the fabrication of high voltage microsupercapacitors (HVMSCs) employing porous laser-induced graphene (from polyimide films with alkalization treatment) followed by laser carving of the polyvinyl alcohol/H 3 PO 4 gel electrolyte to realize a series assembly of supercapacitors and significantly increase the voltage resistance. The results elucidated that HVMSCs (3 mm × 21.15 mm) exhibited excellent capacitive performance including exceptional potential window (10 V), high areal capacitance (244 μF/cm 2 ), acceptable power density (274 μW/cm 2 ) and energy density (3.22 μW h/cm 2 ), good electrochemical stability and flexibility at different bending status (0, 45, 90, 135, and 180°), as well as impressive voltage durability more than 5 V in smaller scale (0.5 mm × 5.5 mm). As such, the HVMSCs have great potential to be integrated with microcircuit modules for the next-generation self-powered systems and storage electronic devices in high voltage applications.