Engineering a Dynamic Solvent-Phobic Liquid Electrolyte Interphase for Long-Life Lithium Metal Batteries.

The heterogeneity, species diversity, and poor mechanical stability of solid electrolyte interphases (SEIs) in conventional carbonate electrolytes result in the irreversible exhaustion of lithium (Li) and electrolytes during cycling, hindering the practical applications of Li metal batteries (LMBs). Herein, this work proposes a solvent-phobic dynamic liquid electrolyte interphase (DLEI) on a Li metal (Li-PFbTHF (perfluoro-butyltetrahydrofuran)) surface that selectively transports salt and induces salt-derived SEI formation. The solvent-phobic DLEI with C-F-rich groups dramatically reduces the side reactions between Li, carbonate solvents, and humid air, forming a LiF/Li3PO4-rich SEI. In situ electrochemical impedance spectroscopy and Ab-initio molecular dynamics demonstrate that DLEI effectively stabilizes the interface between Li metal and the carbonate electrolyte. Specifically, the LiFePO4||Li-PFbTHF cells deliver 80.4% capacity retention after 1000 cycles at 1.0 C, excellent rate capacity (108.2 mAh g-1 at 5.0 C), and 90.2% capacity retention after 550 cycles at 1.0 C in full-cells (negative/positive (N/P) ratio of 8) with high LiFePO4 loadings (15.6 mg cm-2) in carbonate electrolyte. In addition, the 0.55 Ah pouch cell of 252.0 Wh kg-1 delivers stable cycling. Hence, this study provides an effective strategy for controlling salt-derived SEI to improve the cycling performances of carbonate-based LMBs.

Kang Q ，Li Y ，Zhuang Z ，Yang H ，Luo L ，Xu J ，Wang J ，Guan Q ，Zhu H ，Zuo Y ，Wang D ，Pei F ，Ma L ，Zhao J ，Li P ，Lin Y ，Liu Y ，Shi K ，Li H ，Zhu Y ，Chen J ，Liu F ，Wu G ，Yang J ，Jiang P ，Huang X ... -  《-》

Stable Solvent-Derived Inorganic-Rich Solid Electrolyte Interphase (SEI) for High-Voltage Lithium-Metal Batteries.

Chen Z ，Wang B ，Li Y ，Bai F ，Zhou Y ，Li C ，Li T ... -  《-》

In Situ Formed Gel Polymer Electrolytes Enable Stable Solid Electrolyte Interface for High-Performance Lithium Metal Batteries.

Hao Q ，Yan J ，Gao Y ，Chen F ，Chen X ，Qi Y ，Li N ... -  《-》

Promoting a Stable Interface Using Localized High-Concentration Carbonate-Based Electrolyte for Li Metal Batteries.

Le L ，Liao M ，Nguyen A ，Wang D ... -  《-》

An Inorganic-Rich Solid Electrolyte Interphase for Advanced Lithium-Metal Batteries in Carbonate Electrolytes.

In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the Li-metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here, an inorganic-rich SEI is designed on a Li-metal surface to reduce its bonding energy with Li metal by dissolving 4m concentrated LiNO3 in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene-carbonate (FEC)-based electrolyte. Due to the aggregate structure of NO3 - ions and their participation in the primary Li+ solvation sheath, abundant Li2 O, Li3 N, and LiNx Oy grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF6 - ions. The weak bonding of the SEI (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping Coulombic efficiency of 99.55 % (1 mA cm-2 , 1.0 mAh cm-2 ) and the electrolyte also enables a Li||LiNi0.8 Co0.1 Mn0.1 O2 (NMC811) full cell (2.5 mAh cm-2 ) to retain 75 % of its initial capacity after 200 cycles with an outstanding CE of 99.83 %.

Liu S ，Ji X ，Piao N ，Chen J ，Eidson N ，Xu J ，Wang P ，Chen L ，Zhang J ，Deng T ，Hou S ，Jin T ，Wan H ，Li J ，Tu J ，Wang C ... -  《-》