A silane molecule with an unsaturated functionality effectively scavenges harmful hydrogen fluoride from the electrolyte and forms a complex, which experiences preferential oxidation and eventually delivers the fluorine species to the interphase that protects cathodes of high energy density batteries.

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

O3-Type layered oxides are widely studied as cathodes for sodium-ion batteries (SIBs) due to their high theoretical capacities. However, their rate capability and durability are limited by tortuous Na+ diffusion channels and complicated phase evolution during Na+ extraction/insertion. Here we report our findings in unravelling the mechanism for dramatically enhancing the stability and rate capability of O3-NaNi0.5Mn0.5–x Sb x O2 (NaNMS) by substitutional Sb doping, which can alter the coordination environment and chemical bonds of the transition metal (TM) ions in the structure, resulting in a more stable structure with wider Na+ transport channels. Furthermore, NaNMS nanoparticles are obtained by surface energy regulation during grain growth. The synergistic effect of Sb doping and nanostructuring greatly reduces the ionic migration energy barrier while increasing the reversibility of the structural evolution during repeated Na+ extraction/insertion. An optimized NaNMS-1 electrode delivers a reversible capacity of 212.3 mAh g–1 at 0.2 C and 74.5 mAh g–1 at 50 C with minimal capacity loss after 100 cycles at a low temperature of −20 °C. Such electrochemical performance is superior to most of the reported layered oxide cathodes used in rechargeable SIBs.

Enhancing the electrode/electrolyte interface stability of high-capacity LiNiCoAlO (LNCA) cathode material is urgently required for its application in next-generation lithium-ion battery. Herein, we demonstrate that enhanced interfacial stability of LNCA can be achieved by simply introducing 2 wt % N-allyl- N, N-bis(trimethylsilyl)amine (NNB) electrolyte additive. Electrolyte oxidation reactions and electrode structural destruction are greatly suppressed in the electrolyte with NNB additive, leading to improved cyclic stability of LNCA from 72.8 to 86.2% after 300 cycles. The mechanism of NNB on improving the cyclic stability of LNCA has been verified to its excellent solid electrolyte interface (SEI) film-forming capability. Moreover, the X-ray diffraction and X-ray photoelectron spectroscopy results indicate that the NNB-derived Si-containing SEI film restrains the Li/Ni disorder of LNCA during cycling, which further improves the cyclic stability of Ni-rich LNCA. Importantly, the charging/discharging test reveals that the NNB additive effectively improves the cyclic stability of the LNCA/graphite full cell.

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