Interphasial Engineering via Individual Moiety Functionalized Organosilane Single-Molecule for Extreme Quick Rechargeable SiO/NCM811 Lithium-Ion Batteries

Abstract

The individual moiety-functionalized organosilane single molecule, that is, 1,1,1,5,5,5-hexamethyl-3-[(trimethylsilyl)­oxy]-3-vinyltrisiloxane (TMSV), is investigated as an electrolyte additive for a less charge-consuming and viscoelastic solid electrolyte interphase (SEI) forming agent, finally accomplishing extremely quick (6 min) rechargeable SiO/NCM811 lithium-ion batteries. The moiety of the vinyl group serves with a poly­(ethylene oxide)-like viscoelastic SEI film on the SiO electrode, which provides a physicochemically stable interphase during long-term cycling. The increase of DC-iR due to electrolyte decomposition on the continuously exposed SiO surface with cycling is inhibited by the alternated SEI composition. Degradation of bulk electrolyte solution caused by thermal decomposition of the LiPF6 salt is also suppressed by the trimethylsilyl moiety in the TMSV additive, which scavenges HF. Owing to the multifunctionality of TMSV, the cycle performance of laminated pouch full cells comprising high-nickel-contented NCM811 positive electrode and SiO-enriched negative electrode is significantly improved at both room and elevated temperatures. Furthermore, the 6 min quick recharging cycle performance is also enhanced by the TMSV additive.

Interface Engineering with Nonsacrificial Perfluorinated-Anion Additives for Boosting the Kinetics of Lithium-Ion Batteries

“…A SEI is known to be a complex mixture of compounds, and the physicochemical properties of the SEI are mostly determined by the type of solvents, electrolyte salts, and additives. Of these, the SEI properties including chemical composition, thickness, uniformity, and morphology can be controlled by various SEI-forming additives, and the related numerous studies have been reported. − The most well-known and widely used SEI-forming additive for a graphite negative electrode is vinylene carbonate (VC). ,− By adding small amounts of VC into an electrolyte solution, the reinforcement of the SEI on graphite is achieved through formation of representative poly­(VC)-based polymeric compounds. , However, an overquantified or unoptimized SEI layer from the additive increases the impedance of LIBs, which leads to degradation of the battery performance, especially at high-rate or low-temperature conditions. − Therefore, the advanced interface engineering by efficient control of additive decomposition without compromising other SEI functions is another important strategy to minimize the interphasial impedance, improving LIB performance.…”

Robust and Fast‐Ion Conducting Interphase Empowering SiOx Anode Toward High Energy Lithium–Ion Batteries

“…Varied strategies, such as materials modification, [18][19][20][21][22][23][24][25][26][27][28][29][30][31] electrolytes formulation, [32][33][34][35][36][37][38][39] and binders development, [40,41] have been taken to tackle the obstacles of SiO x -based anodes. As for materials modification, surface coating, [19][20][21][22][23][24] element doping [25][26][27] and prelithiation [28][29][30][31] strategies have been always adopted.…”

Beneficial Role of Inherently Formed Residual Lithium Compounds on the Surface of Ni-Rich Cathode Materials for All-Solid-State Batteries

“…Ni-rich cathode materials (LiNi x Co y Mn z O 2 , NCMs) are widely used as cathode active materials for LIBs because of their high specific capacity, − and hence, NCMs are also the most promising cathode materials for sulfide-based all-solid-state batteries (ASSBs) because of their sophisticated characteristics. Meanwhile, the surface engineering of NCMs is highly important to fully utilize the characteristics of NCMs. ,− Owing to the high vapor pressure of Li at high calcination temperatures of NCMs, which leads to the formation of a Li-deficient phase, NCMs are synthesized using excess Li sources .…”