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Solid polymer electrolytes (SPEs) have aroused wide interest in lithium batteries because of their sufficient mechanical properties, superior safety performances, and excellent processability. However, ionic conductivity and high‐voltage compatibility of SPEs are still yet to meet the requirement of future energy‐storage systems, representing significant barriers to progress. In this regard, intermolecular interactions in SPEs have attracted attention, and they can significantly impact on the Li+ motion and frontier orbital energy level of SPEs. Recent advances in improving electrochemcial performance of SPEs are reviewed, and the underlying mechanism of these proposed strategies related to intermolecular interaction is discussed, including ion–dipole, hydrogen bonds, π–π stacking, and Lewis acid–base interactions. It is hoped that this review can inspire a deeper consideration on this critical issue, which can pave new pathway to improve ionic conductivity and high‐voltage performance of SPEs.

Developing high‐voltage Mg‐compatible electrolytes (>3.0 V vs Mg) still remains to be the biggest R&D challenge in the area of nonaqueous rechargeable Mg batteries. Here, the key design concepts toward exploring new boron‐based Mg salts in a specific way of highlighting the implications of anions are proposed for the first time. The well‐defined boron‐centered anion‐based magnesium electrolyte (BCM electrolyte) is successfully presented by facile one‐step mixing of tris(2H‐hexafluoroisopropyl) borate and MgF2 in 1,2‐dimethoxyethane, in which the structures of anions have been thoroughly investigated via mass spectrometry accompanied by NMR and Raman spectra. The first all‐round practical BCM electrolyte fulfills all requirements of easy synthesis, high ionic conductivity, wide potential window (3.5 V vs Mg), compatibility with electrophilic sulfur, and simultaneously noncorrosivity to coin cell assemblies. When utilizing the BCM electrolyte, the fast‐kinetics selenium/carbon (Se/C) cathode achieves the best rate capability and the sulfur/carbon (S/C) cathode exhibits an impressive prolonged cycle life than previously published reports. The BCM electrolyte offers the most promising avenue to eliminate the major roadblocks on the way to high‐voltage Mg batteries and the design concepts can shed light on future exploration directions toward high‐voltage Mg‐compatible electrolytes.

Nitrogen-doped MnO/graphene nanosheets (N-MnO/GNS) hybrid material was synthesized by a simple hydrothermal method followed by ammonia annealing. The samples were systematically investigated by X-ray diffraction analysis, Raman spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, and atomic force microscopy. N-doped MnO (N-MnO) nanoparticles were homogenously anchored on the thin layers of N-doped GNS (N-GNS) to form an efficient electronic/ionic mixed conducting network. This nanostructured hybrid exhibited a reversible electrochemical lithium storage capacity as high as 772 mAh g(-1) at 100 mA g(-1) after 90 cycles, and an excellent rate capability of 202 mA h g(-1) at a high current density of 5 A g(-1). It is expected that N-MnO/GNS hybrid could be a promising candidate material as a high capacity anode for lithium ion batteries.

An efficient organic magnesium borate-based electrolyte with non-nucleophilic characteristics for magnesium–sulfur battery.

PPC/LLZTO composite solid electrolyte was developed for a flexible solid lithium battery.