LiNi0.8Mn0.1Co0.1O2||SiOx@graphite (NCM811||SiOx@G)-based lithium-ion batteries
(LIBs)
exhibit high energy density and have found wide applications in various
fields, including electric vehicles. Nonetheless, its low-temperature
performance remains a challenge. One of the most efficacious strategies
to enhance the low-temperature functionality of battery is the development
of appropriate electrolytes with low-temperature suitability. Herein, p-tolyl isocyanate (PTI) and 4-fluorophenyl isocyanate (4-FI)
are used as additive substances to integrate into the electrolytes
to improve the low-temperature performance of the battery. Theoretical
calculations and experimental results indicate that PTI and 4-FI can
both preferentially generate a stable SEI on the electrode surface,
which is beneficial to reduce the interfacial impedance. As a result,
the additive, i.e. 4-FI, is superior to PTI in improving the low-temperature
performance of the battery due to the optimization of F in the SEI
membrane components. At room temperature, the cyclic stability of
the NCM811/SiOx@G pouch cell increases from 92.5% (without additive)
to 94.2% (with 1% 4-FI) after 200 cycles at 0.5 C. Under the operating
temperature of −20 °C, the cyclic stability of the NCM811/SiOx@G
pouch cell increases from 83.2% (without additive) to 88.6% (with
1% 4-FI) after 100 cycles at 0.33 C. Therefore, a rational interphase
design involving the modification of the additive structure is a cost-effective
way to improve the performance of LIBs.