Among so-called “next generation” battery technologies, lithium metal batteries (LMBs) enabled by solid-state electrolytes are considered key to achieve rechargeable batteries with higher energy density and safety than current lithium ion batteries (LIBs). This article briefly evaluates various aspects of polymer electrolytes from history, macromolecular architecture, material classification, and electrode optimization, with special emphasis on solid polymer electrolytes (SPEs) and single ion conducting polymeric electrolytes. Representative interfaces and interphases as well as corresponding engineering strategies adopted for the anticipated goals are briefly summarized, including various approaches adopted to mitigate the shortcomings at the interfaces. Significant weight should be given for research and development of SPEs, as they could be an enabler for solid-state LMBs with attractive performance and made by comparatively easy electrode and cell processing techniques.

Application of different electrolyte components as blends in nonaqueous electrolyte formulations represents a viable approach towards improving the overall performance and reliability of a lithium ion battery cell. By combining the advantages of different electrolyte constituents, cell chemistry can be optimized and tailored for a specific purpose. In this paper, the current progress on possibilities, advantages, as well as limitations of blended nonaqueous electrolyte formulations, including solvent, salt and additive blends is reviewed and discussed. Emphasis is set on the physicochemical, electrochemical, and safety aspects. In addition, the aim of this review is to provide perspective and possible strategy for further and future development of blended nonaqueous electrolytes with long life, high energy density, high power, and adequate safety at competitive manufacturing costs. The provided overview and perspective on blended nonaqueous electrolyte formulations should encourage researchers to proceed with further and deeper investigations in this promising field of advanced batteries.

Allyl ether-functional polycarbonates, synthesized by organocatalytic ring-opening polymerization of the six-membered cyclic carbonate monomer 2-allyloxymethyl-2-ethyltrimethylene carbonate, were used to prepare non-polyether polymer electrolytes. UV-crosslinking of the allyl side groups provided mechanically stable electrolytes with improved molecular flexibility-T g below 220 8C-and higher ionic conductivity-up to 4.3 3 10 27 S/ cm at 25 8C and 5.2 3 10 26 S/cm at 60 8C-due to the plasticizing properties of the allyl ether side groups. The electrolyte function was additionally demonstrated in thin-film Li battery cells.

Li + -conducting solid polymer electrolytes (SPEs) obtained from supramolecular self-assembly of trimethylated cyclodextrin (TMCD), poly(ethylene oxide) (PEO), and lithium salt are investigated for application in lithium-metal batteries (LMBs) and lithium-ion batteries (LIBs). The considered electrolytes comprise nanochannels for fast lithium-ion transport formed by CD threaded on PEO chains. It is demonstrated that tailored modification of CD beneficially influences the structure and transport properties of solid polymer electrolytes, thereby enabling their application in LMBs. Molecular dynamics (MD) simulation and experimental data reveal that modification of CDs shifts the steady state between lithium ions inside and outside the channels, in this way improving the achievable ionic conductivity. Notably, the designed SPEs facilitated galvanostatic cycling in LMBs at fast charging and discharging rates for more than 200 cycles and high Coulombic efficiency.Letter pubs.acs.org/macroletters

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