RESUMEN
The interfacial instability of high-nickel layered oxides severely plagues practical application of high-energy quasi-solid-state lithium metal batteries (LMBs). Herein, a uniform and highly oxidation-resistant polymer layer within inner Helmholtz plane is engineered by in-situ polymerizing 1-vinyl-3-ethylimidazolium (VEIM) cations preferentially adsorbed on LiNi0.83Co0.11Mn0.06O2 (NCM83) surface, inducing formation of anion-derived cathode-electrolyte interphase with fast interfacial kinetics. Meanwhile, the copolymerization of [VEIM][BF4] and vinyl ethylene carbonate (VEC) endows P(VEC-IL) copolymer with the positively-charged imidazolium moieties, providing positive electric fields to facilitate Li+ transport and desolvation process. Consequently, the Li||NCM83 cells with a cut-off voltage up to 4.5 V exhibit excellent reversible capacity of 130 mAh g-1 after 1000 cycles at 25 °C and considerable discharge capacity of 134 mAh g-1 without capacity decay within 100 cycles at -20 °C. This work provides deep understanding on tailoring electric double layer by cation specific adsorption for high-voltage quasi-solid-state LMBs.
RESUMEN
Solid-state Li-O2 batteries (SSLOBs) have attracted considerable attention because of their high energy density and superior safety. However, their sluggish kinetics have severely impeded their practical application. Despite efforts to design highly efficient catalysts, efficient oxygen reaction evolution at gas-solid interfaces and fast transport pathways in solid-state electrodes remain challenging. Here, we develop a dual electronic-ionic microenvironment to substantially enhance oxygen electrolysis in solid-state batteries. By designing a lithium-decorative catalyst with an engineering crystal structure, the coordinatively unsaturated sites and high concentration of defects alleviate the limitations of electronic-ionic transport in solid interfaces and create a balanced gas-solid microenvironment for solid-state oxygen electrolysis. This strategy facilitates oxygen reduction reaction, mediates the transport of reaction species, and promotes the decomposition of the discharge products, contributing to a high specific capacity with a stable cycling life. Our work provides previously unknown insight into structure-property relationships in solid-state electrolysis for SSLOBs.
RESUMEN
The lithium-sulfur (Li-S) battery with a high theoretical energy density (2560 Wh kg-1) is one of the most promising candidates in next-generation energy storage systems. However, its practical application is impeded by the shuttle effect of lithium polysulfides, huge volume expansion, and overgrowth dendrite of lithium. Herein, we propose an artificial conformal agar polymer coating on a lithium anode (marked as A-Li). The functional layer facilitating the formation of a compact interphase on the lithium anode can effectively accommodate expansive volume and restrain the growth of dendritic lithium. The Li/Li symmetric cell with A-Li delivers stable plating/stripping cycling over 300 h at a high current density of 3.0 mA cm-2 and a high fixed areal capacity of 3.0 mAh cm-2. The cycle life of Li-Cu cells with A-Li is twice longer than that of pristine cells, and the Li-S batteries equipped with A-Li anodes also deliver an enhanced specific capacity and high Coulombic efficiencies. This work provides a pathway to protect metal Li anodes and contributes to the development of high-performance Li-S batteries.
RESUMEN
Owing to the promise of high safety and energy density, all-solid-state batteries are attracting incremental interest as one of the most promising next-generation energy storage systems. However, their widespread applications are inhibited by many technical challenges, including low-conductivity electrolytes, dendrite growth, and poor cycle/rate properties. Particularly, the interfacial dynamics between the solid electrolyte and the electrode is considered as a crucial factor in determining solid-state battery performance. In recent years, intensive research efforts have been devoted to understanding the interfacial behavior and strategies to overcome these challenges for all-solid-state batteries. Here, the interfacial principle and engineering in a variety of solid-state batteries, including solid-state lithium/sodium batteries and emerging batteries (lithium-sulfur, lithium-air, etc.), are discussed. Specific attention is paid to interface physics (contact and wettability) and interface chemistry (passivation layer, ionic transport, dendrite growth), as well as the strategies to address the above concerns. The purpose here is to outline the current interface issues and challenges, allowing for target-oriented research for solid-state electrochemical energy storage. Current trends and future perspectives in interfacial engineering are also presented.
RESUMEN
Black phosphorus modified sulfurized polyacrylonitrile (BP-SPAN) is reported for the first time for Li-S batteries operated in ether electrolyte. The amorphous P2S5+x in BP-SPAN is crucial to suppress the shuttling effect of polysulfides and enhance the reaction kinetics. It delivers an amazing capacity of 1086 mA h g-1 (2C) and capacity retention of 91.1% (0.1C, 100th).
