In Situ Topological Interphases Boosting Stable Solid‐State Lithium Metal Batteries

Abstract

Incompatible interphases resulting from the irreconcilable contradiction between impedance and mechanical strength have become one of the major obstacles to the practical application of solid-state lithium metal batteries (SSLMBs). With the employment of a decoupling strategy by rational topological design, herein a topological polymer-reinforced interphase layer is in situ constructed using a synthesized solid polymer electrolyte. As a result, the constructed topological solid electrolyte interphase (SEI) layer harmonizes the enhanced mechanochemical stability and fast diffusion dynamics of Li + , which maintains the integrity and stability of the SEI layer during cycling. In addition, a highly stable and reversible Li nucleation/stripping behaviors exceeding 3000 h and the superior cycling performance of practical LiFePO 4 /Li metal battery beyond 500 cycles can be achieved by virtue of the formation of the topological interphase layer. This design strategy of constructing a topological interphase layer to decouple mechanical strength and the activation energy of Li + transport provides a feasible paradigm for realizing practical SSLMBs.

Locally Saturated Ether-Based Electrolytes With Oxidative Stability For Li Metal Batteries Based on Li-Rich Cathodes

“…These species have been widely observed in sulfonylimide-based electrolytes and are commonly associated with the highly reversible performance they demonstrate. 19,30 Though the carbonate system was also found to produce LiF, its otherwise organic and PO x F ycontaining SEI was evidently insufficient for long-term reversible cycling, as evidenced by the existence of polycarbonate species derived from reductively unstable EC.…”

“…As shown in Figures S5 and S6, the LDME2 system produced abundant LiF, SO x F y , and C–F species derived from FSI – and BTFE decomposition which are maintained after 100 cycles in addition to an increased prevalence of Li–F. These species have been widely observed in sulfonylimide-based electrolytes and are commonly associated with the highly reversible performance they demonstrate. , Though the carbonate system was also found to produce LiF, its otherwise organic and PO x F y -containing SEI was evidently insufficient for long-term reversible cycling, as evidenced by the existence of polycarbonate species derived from reductively unstable EC.…”

Solid-state polymer electrolytes in lithium batteries: latest progress and perspective

“…3e, the CPLAR-SPE LFP/Li battery exhibits a consistent and enduring cycling performance, achieving a capacity of 116.5 mA h g −1 after undergoing 500 cycles at a rate of 0.5 C. Moreover, it consistently maintains an average Coulomb efficiency exceeding 99.78%, further validating the establishment of a steadfast electron-blocking layer that effectively hinders the proliferation of lithium dendrites. 61…”

Practical challenges and future perspectives of solid polymer electrolytes: microscopic structure and interface design

“…Through the high-entropy topological design, Mai et al . 162 achieved a breakthrough in addressing this paradox between mechanical properties and ion conduction, thus improving the mechanical stability and reducing the activation energy of Li + ion transport within SPEs. In detail, a topological interphase layer is in situ constructed with topologically cross-linked poly(1,3-dioxolane) (CPDOL) in the Li/SPE interface.…”