Beneficial impact of lithium bis(oxalato)borate as electrolyte additive for high-voltage nickel-rich lithium-battery cathodes

High-voltage nickel-rich layered cathodes possess the requisite, such as excellent discharge capacity and high energy density, to realize lithium batteries with higher energy density. However, such materials suffer from structural and interfacial instability at high voltages (>4.3 V). To reinforce the stability of these cathode materials at elevated voltages, lithium borate salts are investigated as electrolyte additives to generate a superior cathode-electrolyte interphase. Specifically, the use of lithium bis(oxalato)borate (LiBOB) leads to an enhanced cycling stability with a capacity retention of 81.7%. Importantly, almost no voltage hysteresis is detected after 200 cycles at 1C. This outstanding electrochemical performance is attributed to an enhanced structural and interfacial stability, which is attained by suppressing the generation of micro-cracks and the superficial structural degradation upon cycling. The improved stability stems from the formation of a fortified borate-containing interphase which protects the highly reactive cathode from parasitic reactions with the electrolyte. Finally, the decomposition process of LiBOB and the possible adsorption routes to the cathode surface are deduced and elucidated.

Automated summary

High-voltage nickel-rich layered cathodes have excellent discharge capacity and high energy density but are structurally and interfacially unstable at high voltages (>4.3 V). By using lithium borate salts as electrolyte additives, an enhanced cathode-electrolyte interphase is generated to improve the stability. Specifically, the use of lithium bis(oxalato)borate (LiBOB) leads to enhanced cycling stability and almost no voltage hysteresis after 200 cycles at 1C.