Easy processing and flexibility of polymer electrolytes make them very promising in developing all-solid-state lithium batteries. However, their low room-temperature conductivity and poor mechanical and thermal properties still hinder their applications. Here, we use LiLaZrTaO (LLZTO) ceramics to trigger structural modification of poly(vinylidene fluoride) (PVDF) polymer electrolyte. By combining experiments and first-principle calculations, we find that La atom of LLZTO could complex with the N atom and C═O group of solvent molecules such as N,N-dimethylformamide along with electrons enriching at the N atom, which behaves like a Lewis base and induces the chemical dehydrofluorination of the PVDF skeleton. Partially modified PVDF chains activate the interactions between the PVDF matrix, lithium salt, and LLZTO fillers, hence leading to significantly improved performance of the flexible electrolyte membrane (e.g., a high ionic conductivity of about 5 × 10 S cm at 25 °C, high mechanical strength, and good thermal stability). For further illustration, a solid-state lithium battery of LiCoO|PVDF-based membrane|Li is fabricated and delivers satisfactory rate capability and cycling stability at room temperature. Our study indicates that the LLZTO modifying PVDF membrane is a promising electrolyte used for all-solid-state lithium batteries.

Tetrakis(aryloxy)phthalocyanine (4c) and its Zn congeners (4a and 4b) and Ni congener (4d) were synthesized, and their self-assembling properties in coordinating and non-coordinating solvents were investigated by absorption and fluorescence spectroscopy, matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF MS), and transmission electron microscopy (TEM). Compounds 4a and 4b in non-coordinating solvents exhibit red-shifted and split Q-bands in absorption spectra even at very low concentrations, suggesting J-aggregate formation. The MALDI-TOF MS for the samples of 4a and 4b prepared from chloroform solutions gives the monomer and aggregate signals. The TEM images of such samples display an indefinite two-dimensional network structure. The aggregates break up into monomers when a coordinating solvent is added to the solution. The driving force for the aggregate formation is proposed to be the complementary coordination of the ether oxygen in the aryloxy groups of one molecule to the core Zn of another molecule of phthalocyanine.

In situ synthesized Ag nanodots enhances electrostatic energy storage by tuning dipoles.

α-Aryl/alkoxy-substituted phthalocyanines (Pcs) were synthesized and the formation of J-type self-aggregation for zinc phthalocyanines has been observed in organic non-coordinating solvents. The mechanism of the formation of this self-assembly was studied by UV–vis spectroscopy, fluorescence spectroscopy and MALDI-TOF MS, which revealed that it was stabilized by Zn–O self-coordination.