Regulating electrode-electrolyte interphases and eliminating hydrogen fluoride to boost electrochemical performances of Li/NCM811 batteries

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Li metal batteries (LMBs) coupled with Ni-rich materials are promising candidates for next-generation high-energy-density lithium batteries. However, due to the inferior stability of cathode/solid-electrolyte interphases (CEI/SEI) and aggressive chemistry of Ni-rich cathode materials, Li metal anode (LMA) and LiPF6-based carbonate electrolytes pose a threat to the achievement of high-energy-density LMBs. Herein, 1-(trimethylsilyloxy)cyclohexene (TMSCH) with functional groups (C=C, Si-O) as a novel multi-functional electrolyte additive is employed to regular the CEI/SEI films on the both Ni-rich cathode materials (LiNi0.8Co0.1Mn0.1O2, NCM811) and LMA surface, and scavenge detrimental hydrogen fluoride (HF) to enhance electrochemical performances of the Li/NCM811 batteries. Furthermore, the theoretical calculation, electrochemical measurements and physical characterizations demonstrate the feasibility and effectiveness of the strategy. Specially, the TMSCH-derived SEI film exhibits a hierarchical structure consisting of an organic-rich outer layer and a LiF-rich inner layer. Accordingly, the microcracks generation of NCM811 secondary particles, transition metal ions dissolution, lithium dendrite growth, parasitic reactions and HF generation of electrolyte are effectively addressed. As a result, with existence of the TMSCH additive, the capacity retention of Li/NCM811 batteries at 1C are remarkably enhanced from 68.2% to 84.9% at 30 °C and 64.2% to 85.8% at 45 °C. Furthermore, the Li/Li symmetric cells with TMSCH can stably cycle over 1000 h at 0.2 mA cm−2 and exhibit super-low overpotential of 75 mV at 1 mA cm−2.