Stable Interface Chemistry and Multiple Ion Transport of Composite Electrolyte Contribute to Ultra‐long Cycling Solid‐State LiNi_0.8Co_0.1Mn_0.1O₂/Lithium Metal Batteries

Abstract

Severe interfacial side reactions of polymer electrolyte with LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode and Li metal anode restrict the cycling performance of solid-state NCM811/ Li batteries.H erein, we propose ac hemically stable ceramicpolymer-anchored solvent composite electrolyte with high ionic conductivity of 6.0 10 À4 Scm À1 ,w hiche nables the solid-state NCM811/Li batteries to cycle 1500 times.T he Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 nanowires (LNs) can tightly anchor the essential N, N-dimethylformamide (DMF) in poly(vinylidene fluoride) (PVDF), greatly enhancing its electrochemical stability and suppressing the side reactions.W ei dentify the ceramic-polymer-liquid multiple ion transport mechanism of the LNs-PVDF-DMF composite electrolyte by tracking the 6 Li and 7 Li substitution behavior via solid-state NMR. The stable interface chemistry and efficient ion transport of LNs-PVDF-DMF contribute to superior performances of the solid-state batteries at wide temperature range of À20-60 8 8C.

A quasi-intercalation reaction for fast sulfur redox kinetics in solid-state lithium–sulfur batteries

“…S2, ESI †), confirming the solid-state property of 1PVHF1FSI. 22,[26][27][28] On the other hand, trace DMF plays the beneficial roles in both the cathode and the anode such as changing the reaction pathway of SPAN and helping form a Li x N-containing SEI component with good ionic conductivity. Commonly, solid polymer electrolytes with good mechanical properties are beneficial for inhibiting lithium dendrite growth.…”

Interfacial Barrier of Ion Transport in Poly(ethylene oxide)–Li7La3Zr2O12 Composite Electrolytes Illustrated by 6Li-Tracer Nuclear Magnetic Resonance Spectroscopy

“…1−3 SSEs can greatly improve the safety and match the lithium metal anode, thus enhancing the energy densities of corresponding solid-state lithium batteries. 4,5 Among various SSEs, polymer electrolytes (such as poly-(ethylene oxide) (PEO), 6 polyvinylidene fluoride (PVDF), 7 poly(methyl methacrylate) (PMMA), 8 and polyacrylonitrile (PAN) 9 based electrolytes) with flexibility and thus good contact with electrodes and easily scalable production have presented promising industrial application prospects and compatibility with commercial lithium-ion batteries. However, lithium ions mainly transmit through the segmental movement of the amorphous domain in polymer electrolytes, resulting in a poor room-temperature ionic conductivity, which has been a decisive issue hindering their further application.…”

“…24 Recently, 6 Li-tracer NMR spectroscopy was applied and presents great superiority to track the Li + transport pathways. Through cycling the 6 5 and PAN-5%LLZO nanowires 26 by utilizing a similar approach. Understanding of the decisive factor for the preferential ion transport pathway is still insufficient and thus crucially necessary for a rational design of the composite polymer electrolytes.…”

“…This may explain the reported various preferential ion transport pathways for different composite electrolytes. 5,25,26 A relatively high interfacial transfer barrier between the polymer phase and the plasticizer, combined with the continuous filler (e.g., nanowires), possibly creates a preferential interfacial transport pathway. Therefore, the compatibility between components in the composite electrolytes and the SCL should be seriously addressed to offer a high-performance electrolyte for an excellent high-rate performance.…”

Critical Current Densities for High-Performance All-Solid-State Li-Metal Batteries: Fundamentals, Mechanisms, Interfaces, Materials, and Applications

“…Several factors have been identified that influence the compatibility of the cathode−electrolyte interface, such as increased active particle size, increased external stress during cycling, and temperature during battery assembly. 131 Swamy et al 132 exploited a b-Li 3 PS 4 /C composite as their electroactive electrode and found that the oxidation of S 2− in sulfide SEs at high voltage produced elemental sulfur. Zhang et al 133 performed in situ EIS and Raman spectroscopy studies to monitor the interface evolutions in the Li-Ni 0.8 Co 0.1 Mn 0.1 O 2 (NCM)/Li 6 PS 5 Cl/Li cell.…”