Formulating the Electrolyte Towards High‐Energy and Safe Rechargeable Lithium–Metal Batteries

Abstract

Rechargeable lithium-metal batteries with ac elllevel specific energy of > 400 Wh kg À1 are highly desired for next-generation storage applications,yet the researchhas been retarded by poor electrolyte-electrode compatibility and rigorous safety concerns.W ed emonstrate that by simply formulating the composition of conventional electrolytes, ah ybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-richl ayered oxide cathodes.B ye mploying the new electrolyte,L ik LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells showf avorable cycling and rate performance,a nd a1 0AhL i k Li-Ni 0.8 Co 0.1 Mn 0.1 O 2 pouchc ell demonstrates ap ractical specific energy of > 450 Wh kg À1 .Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces towardpractical realization of high-energy rechargeable batteries.

Constructing Highly Conductive and Thermomechanical Stable Quasi‐Solid Electrolytes by Self‐Polymerization of Liquid Electrolytes within Porous Polyimide Nanofiber Films

“…In the mixed solution, LiPF 6 would quickly decompose and release gaseous phosphorus pentafluoride (PF 5 ) and the PF 5 could trigger the cationic ringopening reactions of DOL. [41][42][43][44][45] Then, the PF 5 combined with a trace of water to form H + (PF 5 OH) − , which acted as the initiator that induced the insertion of oxygen ions into the ring-opening DOL monomer to trigger the growth of polymer chains. At the same time, LiTFSI worked as a catalyst that promoted the self-polymerization of DOL.…”

Achieving a Stable Solid Electrolyte Interphase and Enhanced Thermal Stability by a Dual-Functional Electrolyte Additive toward a High-Loading LiNi0.8Mn0.1Co0.1O2 /Lithium Pouch Battery

“…Therefore, developing novel electrolyte additives to simultaneously reduce intrinsic electrode reactivity and provide heat cut-off functionality is of great challenge. 38 Moreover, most research in this field only focused on the chemistry and electrochemical process of the electrolyte. It should be pointed out that a cell is the complex system with multiple spatial and temporal scales.…”

“…In terms of the separator, our group proposed heatproof–fireproof bifunctional separators for delaying heat generation and preventing the internal short circuit of high energy density LIBs. , In addition, designing nonflammable electrolytes by adding a fire retardant is an effective method to prevent the battery from burning. − However, most fire retardants are traditional passive protection and can only reduce the heat release when the batteries are on the verge of fire. Therefore, developing novel electrolyte additives to simultaneously reduce intrinsic electrode reactivity and provide heat cut-off functionality is of great challenge . Moreover, most research in this field only focused on the chemistry and electrochemical process of the electrolyte.…”

In Situ Formed Poly(ester-alt-acetal) Electrolytes with High Oxidation Potential and Electrode–Electrolyte Interface Stability

“…Given the escalating need for safe energy storage devices with high energy density, nonvolatile polymer electrolytes (PEs) for lithium metal batteries (LMBs) have emerged as a focal point of current research. , The development of PEs with improved ionic conductivity, thermal stability, electrode–electrolyte interface stability, and compatibility is overwhelming and on the road. − Thereof, the preparation of PEs by in situ polymerization is an emerging method for the preparation of LMBs with enhanced interfacial compatibility and battery performance. , The typical PEs produced by in situ polymerization have been widely investigated, such as poly­(dioxolane) from cationic polymerization of dioxolane, − poly­(vinylene carbonate) from free radical polymerization of vinyl carbonate, , and poly­(ethylene glycol) diglycidyl ether from anionic polymerization of ethylene oxide . During the in situ polymerization process for LMBs, the surface of the electrodes can be fully wetted first by the monomers, leading to the filling of gaps and defects, and the performance of such PE-based batteries can be significantly enhanced in comparison to traditional PEs. , …”