Multicomponent additive-mediated interfacial engineering enables highly stable lithium-ion pouch cells under harsh working conditions

Well-designed FDP electrolyte will be used in SC-NCM613||graphite pouch full cells operated under harsh working conditions (4.4V or 45 ℃). Remarkably, through building the synergistic effects of CEI/SEI layer between the cathode/anode and electrolyte, the 1700 mAh-level SC-NCM613/graphite pouch cell using FDP containing electrolyte delivers the excellent capacity retention rate of 97.3% after 250 cycles at 4.4 V and 45°C. Benefiting from the improved structural stability, suppressed phase transformation and eliminated parasitic reactions between the electrolyte and electrodes, which paves a new avenue to promote the high-temperature and high voltage performance of commercial Ni-rich single-crystal NCM cathode. [Display omitted] •FDP additives significantly reduce gas evolution.•LiF abundant CEI layers are incorporated by the electrochemical reaction of FDP.•The 1.7 Ah pouch full cell with FDP based electrolyte exhibits 97.3 % capacity retention at 4.4 V over 250 cycles at 45 °C. The interfacial chemistry influenced by electrolyte components, including lithium salts, solvents, and additives, has attracted significant attention for its critical role in advancing high-performance lithium-ion batteries (LIBs). However, the instability of interfacial interactions between traditional electrolytes and electrodes presents a major obstacle to achieving optimal LIB performance, especially in conditions of high temperature and cut-off voltage. This work introduces an interfacial engineering method utilizing a combination of additives − specifically, fluoroethylene carbonate, ethylene sulfate, and propane sultone (referred to as FDP) − to enhance the conventional carbonate electrolyte for applications in high-voltage and high-temperature LIBs. These additives effectively adjust the interactions between lithium ions and solvents, reducing desolvation energy, thereby decreasing gas evolution, mitigating extensive solvent decomposition, and promoting the formation of a thin, uniform, low-impedance elastic interfacial film on both the anode and cathode. Noteworthy results include a 97.3 % capacity retention at 4.4 V over 250 cycles at 45 °C in a 1.7 Ah-level single crystal LiNi0.6Co0.1Mn0.3O2 (SC-NCM613)||graphite pouch full cell incorporating FDP additives. This interfacial engineering approach facilitated by these multicomponent additives presents a highly promising and practical pathway for achieving long-lasting high-voltage and high-temperature LIBs.