Search

Lithium‐ion batteries (LIBs) suffer from energy loss and safety hazards under high‐rate conditions, because of the sluggish electrochemical kinetics and unstable interfacial passivation. Herein, a PC‐based electrolyte using weakly solvated solvent ethyl trifluoroacetate is developed to improve interfacial kinetics and stability in LIBs. A microsolvating competition is revealed in the bulk electrolyte, forming a loose Li+ coordination configuration with benign Li+ affinity and high ionic conductivity. Furthermore, an inorganic‐rich interphase is constructed on a graphite anode, affording smooth Li+ desolvation and reliable passivation. Consequently, the NCM622/graphite cell in PC‐based electrolyte shows improved cycling stability (82.2% after 200 cycles) and rate capability (83% at 4C compared to 0.1C) at a high‐voltage of 4.5 V, much better than those of EC‐based electrolyte (76.2% after 200 cycles and 74% at 4C). Additionally, the PC‐based electrolyte affords reversible operation at –40 °C while the EC‐based electrolyte fails at –40 °C. This work highlights the potential of solvation structure engineering for low‐energy‐barrier electrolyte. [ABSTRACT FROM AUTHOR]

Ni−rich cathodes are hopeful materials for advanced lithium−ion batteries (LIBs) due to high capacity. Nonetheless, the chemical crosstalk triggered by reactive oxygen (O*) represents a critical factor in thermal runaway (TR). Currently, there are few effective means to prevent this parasitic reaction. Here, inspired by the O* scavenging effect of β−carotene in living organisms, it is innovatively identified that β−carotene can impede TR by restraining the escape of O* during the thermal decomposition of nickel−rich cathodes. Using LiNi0.6Co0.2Mn0.2O2 as model and extending to higher nickel content cathodes (LiNi0.8Co0.1Mn0.1O2, LiNi0.9Co0.05Mn0.05O2), it is demonstrated that β−carotene can undergo an in situ oxygen copolymerization reaction to trapping O*, thereby attenuating chemical crosstalk. Additionally, the generated oxygen copolymer can also adjust band center of the O 2p orbitals of delithiated cathode, alleviating the charge compensation behavior of oxygen anions, and thus delaying the phase transition of charged LiNi0.8Co0.1Mn0.1O2. As a result, the TR trigger temperature of NCM811∣Graphite pouch cell is increased from 131.0 to 195.0 °C and maximum temperature is reduced from 657.8 to 412.4 °C. This work introduces a new and simple strategy for designing functional additives to block TR, offering a promising avenue for advancing the safety of LIBs. [ABSTRACT FROM AUTHOR]

The sufficient and reversible active lithium is the cornerstone for the operation of high‐energy lithium‐ion batteries. However, active lithium is inevitably depleted due to the formation of a solid electrolyte and the presence of irreversible side reactions. The shortage of lithium in optimally designed batteries not only leads to a depreciation of energy density but also deteriorates the electrode structure resulting in degradation of cycle life. Inspiringly, prelithiation technology that additionally compensates for lithium has been proposed and is playing an increasingly significant role in enhancing battery energy density and prolonging cycle life. Herein, guided by the factors that initiate lithium loss, the action mechanism and the effectiveness of prelithiation are scrutinized. Moreover, the emerging advanced prelithiation technologies based on anode/cathode materials, the key barriers, and the applicability at scale are systematically summarized and compared. Integrating the challenges and development trends aspires to provide a comprehensive prelithiated hybrid lithium replenishment and storage technology as a reference in the scale‐up of prelithiation technologies. [ABSTRACT FROM AUTHOR]