The next-generation portable and wearable energy-storage devices are expected to withstand distinguished mechanical strain and damage. Hence, the electrolytes with superior self-healability, outstanding stretchability, and excellent electrochemical performance are the necessary requirements for achieving advanced supercapacitors, but it still remains a huge challenge to develop the electrolytes. Herein, a novel type of multifunctional supramolecular hydrogel electrolyte (3-dimethyl (methacryloyloxyethyl)ammonium propane sulfonate (DMAPS)−poly(acrylic acid) (PAA)/H 2 SO 4 /bromamine acid sodium (BAAS)) cross-linked by reasonably designed hydrogen bonds and ionic associations is prepared by facile one-pot copolymerization. The obtained hydrogel displays a high ionic conductivity of 40 mS cm −1 , a significant self-healing behavior within only 8 min, and a large stretch strain of more than 2000%. Surprisingly, it also demonstrates robust self-adhesiveness on the electrodes, which not only avoid the relative displacement and delamination between the electrolyte and electrode layers during the repeated mechanical deformation but also is convenient for achieving the lightweight and portable energy-storage devices. Furthermore, the carbon-based supercapacitor with the DMAPS−PAA/H 2 SO 4 /BAAS hydrogel electrolyte can achieve a large electrode-specific capacitance of 240 F g −1 benefited from the introduction of the BAAS redox additive. Simultaneously, the specific capacitance maintains 96 and 89% of its initial value after 400 bending/releasing cycles and 5000 charge/discharge cycles, respectively. The investigation provides a versatile strategy to design a multifunctional hydrogel electrolyte applied to promising power sources for personalized electronics.

Multifunctional conductive hydrogels attract booming attention with the prosperity of flexible and wearable soft devices such as energy storage systems and sensors. However, conventional water-based conductive hydrogels inevitably lose ionic conductivity and mechanical flexibility at subzero temperature, thus restricting their practical utilizations in extremely cold environments. On the other hand, simultaneous realization of high freezing tolerance, toughness, ionic conductivity, and electrochemical property through a simple approach is still a challenge. Herein, a novel long-term anti-freezing and mechanically tough conductive active organohydrogel is designed and prepared by simultaneously introducing poly(vinyl alcohol) (PVA), alizarin red S (ARS), and H 2 SO 4 into a H 2 O/ethylene glycol (EG) binary solvent. Benefiting from the exceptionally low temperature tolerance capability of H 2 O/EG and extra pseudocapacitance contribution of ARS active molecules, even at the temperature as low as −37 °C, the as-fabricated flexible supercapacitor still demonstrates a large electrode specific capacitance (240 F g −1 ), high energy density (21 Wh kg −1 ), excellent cycling stability (only 9% capacitance decay over 5000 cycles), and superior durability (97% capacitance retention after stored for 50 days). More impressively, owing to the excellent strain sensitivity (GF = 2.18) and significant repeatability, the active organohydrogel based antifreezing strain sensor can not only precisely monitor the large-scale and subtle human movements but also efficiently distinguish the directions of the movements under RT or −37 °C. Overall, our investigation of long-term low temperature tolerant active organohydrogels provides a versatile strategy to exploit superior flexible energy storage devices and strain sensors applied in extremely cold environments.

A new dual acylhydrazone-functionalized gelator (L) has been synthesized, which behaves as a thermal-responsive supramolecular organogel (L-gel) in DMSO. This L-gel exhibits very weak fluorescence based on the photoinduced electron transfer (PET) mechanism. The L-gel can recognize Al and assemble into an enhanced blue-light-emitting supramolecular metallogel (Al@gel).

Trinuclear and tetranuclear magnesium alkoxide clusters supported by bulky phenolates with triangular or rhombic structures were readily synthesized in acceptable yields via the reaction of 2-N,N-dimethylaminoethanol/methoxyethanol, different phenols, and dibutylmagnesium. These complexes have been characterized using (1)H and (13)C NMR, elemental analyses, and X-ray crystallography. The experimental results indicate that these clusters are efficient and excellent initiators for the ring-opening polymerizations (ROPs) of l-lactide (LA) and afford polylactides with desired molecular weights and narrow polydispersity indexes (PDIs). Complex 2 can even catalyze the ROP of 4000 equiv of l-lactide in 1 min in a controlled model. Kinetic studies indicate that the polymerization is first-order for both the trinuclear magnesium complex 3 and LA. However, for the tetranuclear magnesium complex 5, the polymerization rate is first order for 5 and second order for LA.

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