“…With the continuously growing market for electric vehicles and portable electronics, it is urgent to develop lithium-ion batteries (LIBs) with higher energy density, which can be realized by increasing the cell voltage and/or the cell capacity according to the energy density calculation. − In recent years, tremendous efforts have been dedicated to exploring high-voltage/capacity cathode materials, such as LiCoPO 4 , , LiNi 0.5 Mn 1.5 O 4 , , and LiNi x Mn y Co z O 2 (NMC, x + y + z = 1) layered oxides. − For instance, LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NMC111) has a theoretical capacity of 287 mAh g –1 , with its capacity proportional to the charging voltage. , Therefore, elevating the upper cutoff voltage is a straightforward approach to increase the cell capacity and energy. Nevertheless, the NMC cathodes generally suffer from structural and thermal instabilities under high cutoff voltage (≥4.4 V) which thus significantly degrades the cell life. , On the other hand, the electrolyte is of vital importance for promoting the reversible redox reaction of the electrodes; , it is composed of 1 M lithium hexafluorophosphate (LiPF 6 ) dissolved in the mixed solvent of ethylene carbonate (EC) and a linear carbonate such as dimethyl carbonate (DMC) or diethyl carbonate (DEC).…”