LiF/Li(3)N-Rich Electrode-Electrolyte Interfaces Enabled by Multi-Functional Electrolyte Additive to Achieve High-Performance Li/LiNi(0.8)Co(0.1)Mn(0.1)O(2) Batteries.

LiPF6-based carbonate electrolytes have been extensively employed in commercial Li-ion batteries, but they face numerous interfacial stability challenges while applicating in high-energy-density lithium-metal batteries (LMBs). Herein, this work proposes N-succinimidyl trifluoroacetate (NST) as a multifunctional electrolyte additive to address these challenges. NST additive could optimize Li+ solvation structure and eliminate HF/H2O in the electrolyte, and preferentially be decomposed on the Ni-rich cathode (LiNi0.8Co0.1Mn0.1O2, NCM811) to generate LiF/Li3N-rich cathode-electrolyte interphase (CEI) with high conductivity. The synergistic effect reduces the electrolyte decomposition and inhibits the transition metal (TM) dissolution. Meanwhile, NST promotes the creation of solid electrolyte interphase (SEI) rich in inorganics on the Li metal anode (LMA), which restrains the growth of Li dendrites, minimizes parasitic reactions, and fosters rapid Li+ transport. As a result, compared with the reference, the Li/LiNi0.8Co0.1Mn0.1O2 cell with 1.0 wt.% NST exhibits higher capacity retention after 200 cycles at 1C (86.4% vs. 64.8%) and better rate performance, even at 9C. In the presence of NST, the Li/Li symmetrical cell shows a super-stable cyclic performance beyond 500 h at 0.5 mA cm-2/0.5 mAh cm-2. These unique features of NST are a promising solution for addressing the interfacial deterioration issue of high-capacity Ni-rich cathodes paired with LMA.

Lei Y ，Xu X ，Yin J ，Xi K ，Wei L ，Zheng J ，Wang Y ，Wu H ，Jiang S ，Gao Y ... -  《-》

LiF-Rich Electrode-Electrolyte Interfaces Enabled by Bifunctional Electrolyte Additive to Achieve High-Performance Li/LiNi(0.8)Co(0.1)Mn(0.1)O(2) Batteries.

Lei Y ，Xu X ，Yin J ，Xu J ，Xi K ，Wei L ，Wu H ，Jiang S ，Gao Y ... -  《-》

Multifunctional Electrolyte Additive for Bi-electrode Interphase Regulation and Electrolyte Stabilization in Li/LiNi(0.8)Co(0.1)Mn(0.1)O(2) Batteries.

Jiang S ，Xu X ，Yin J ，Wu H ，Zhu X ，Gao Y ... -  《-》

LiF-Rich Interfaces and HF Elimination Achieved by a Multifunctional Additive Enable High-Performance Li/LiNi(0.8)Co(0.1)Mn(0.1)O(2) Batteries.

Lei Y ，Xu X ，Yin J ，Jiang S ，Xi K ，Wei L ，Gao Y ... -  《-》

Constructing LiF/Li(2)CO(3)-rich heterostructured electrode electrolyte interphases by electrolyte additive for 4.5 V well-cycled lithium metal batteries.

The cycling performance of promising high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) batteries is determined by the interfacial stability between electrodes and electrolyte. However, it is challenging to achieve them under high voltage. Herein, we stabilized 4.5 V Li||NCM811 batteries via electrolyte engineering with pentafluorostyrene (PFBE) as the additive. PFBE contributes to the formation of highly Li+ conductive and mechanically robust LiF/Li2CO3-rich heterostructured interphases on NCM811 cathode and Li metal anode (LMA) surfaces. Such electrode-electrolyte interphases (EEIs) obviously alleviate irreversible phase transition, microcracks induced by stress accumulation and transition metal dissolution in the Ni-rich layered cathode. Meanwhile, the growth of Li dendrites on the LMA surface is effectively controlled. As expected, 4.5 V Li||NCM811 batteries sustain a capacity retention rate of 61.27% after 600 cycles at 0.5 C (100 mA g-1). More importantly, ∼6.69 Ah Li||NCM811 pouch cells with such electrolytes could represent a stable energy density of ∼485 Wh kg-1 based on all cell components.

Hu X ，Li Y ，Liu J ，Wang Z ，Bai Y ，Ma J ... -  《-》