High energy batteries urgently required to power electric vehicles are restricted by a number of challenges, one of which is the sluggish kinetics of cell reactions under low temperatures. A novel approach is reported to improve the low temperature performance of high energy batteries through rational construction of low impedance anode and cathode interface films. Such films are simultaneously formed on both electrodes via the reduction and oxidation of a salt, lithium difluorobis(oxalato) phosphate. The formation mechanisms of these interface films and their contributions to the improved low temperature performances of high energy batteries are demonstrated using various physical and electrochemical techniques on a graphite/LiNi0.5Co0.2Mn0.3O2 battery using 1 m LiPF6‐ethylene carbonate/ethyl methyl carbonate (1/2, in weight) baseline electrolyte. It is found that the interface impedances, especially the one on the anode, constitute the main obstacle to capacity delivery of high energy batteries at low temperatures, while the salt containing fluorine and oxalate substructures used as additives can effectively suppress them.

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Phenyl vinyl sulfone (PVS) as a novel electrolyte additive is used to construct a protective interface film on layered lithium-rich cathode. Charge-discharge cycling demonstrates that the capacity retention of Li(LiMnNiCo)O after 240 cycles at 0.5 C between 2.0 and 4.8 V (vs Li/Li) reaches about 80% by adding 1 wt % PVS into a standard (STD) electrolyte, 1.0 M LiPF in EC/EMC/DEC (3/5/2 in weight). This excellent performance is attributed to the special molecular structure of PVS, compared to the additives that have been reported in the literature. The double bond in the molecule endows PVS with preferential oxidizability, the aromatic ring ensures the chemical stability of the interface film, and the sulfur provides the interface film with ionic conductivity. These contributions have been confirmed by further electrochemical measurements, theoretical calculations, and detailed physical characterizations.

DTYP exhibits multiple functionalities that dramatically improve the performance of a high voltage Li-ion cell using LiNi0.5Mn1.5O4 at elevated temperature.

HF-induced performance degradation and DEPP-based strategy for NCA.

Compared with other commercial cathode materials, the LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode (NCM811) has high specific capacity and a relatively low cost. Nevertheless, the higher nickel content in NCM811 leads to an extremely unstable interface between the electrode and the electrolyte, resulting in inferior cyclic stability of the corresponding cell. Use of film-forming additives is regarded as the most feasible and economic approach to construct a stable interface on the NCM811 cathode. However, less effective electrolyte additives have been reported to date. Herein, we propose a valid film-forming electrolyte additive, 2,4,6triphenyl boroxine (TPBX), for application in a high-voltage NCM811 cathode. Experimental and computational results reveal that the TPBX additive can be preferentially oxidized to generate a highly stable and conductive cathode electrolyte interface (CEI) layer on the NCM811 cathode, which efficiently suppresses the detrimental side reaction and improves the electrochemical performance eventually. In detail, the cyclic stability of the Li/NCM811 half-cell is enhanced from 57% (without additive) to 78% (with 5% TPBX) after 200 cycles at 1C between 3.0 and 4.35 V. At a high current rate of 15C, the TPBX-containing electrode delivers a capacity of about 135 mAh g −1 , which is much higher than that of the electrode without the additive (80 mAh g −1 ). Interestingly, the TPBX is also reduced earlier than the ethylene carbonate (EC) solvent to form an ionically conductive solid electrolyte interface (SEI) film on the graphite anode. Due to the CEI layer on the cathode and the SEI film on the anode simultaneously formed by the TPBX additive, the cyclic performance of the graphite/ LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cell is enhanced. Therefore, the incorporation of the TPBX additive into the electrolyte provides a convenient method for the commercial application of the high-energy-density NCM811 cathode in high-voltage lithium-ion batteries. KEYWORDS: LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), electrolyte additive, 2,4,6-triphenyl boroxine, cathode electrolyte interface, high-energy-density lithium-ion battery