Organic Nitrate Additive for High‐Rate and Large‐Capacity Lithium Metal Anode in Carbonate Electrolyte

Abstract

Lithium nitrate has been widely used to improve the interfacial stability of Li metal anode in ether electrolyte. However, the low solubility limits its application in carbonate electrolytes for high‐voltage Li metal batteries. Herein, nitrated polycaprolactone (PCL‐ONO2), which is prepared via the acylation of polycaprolactone diol (PCL‐diol) followed by the grafting of nitrate group, has been proposed as an electrolyte additive to introduce high‐concentration NO3− into carbonate electrolytes for the first time. The theoretical calculations and X‐ray photoelectron spectroscopy depth profiling demonstrate that the PCL‐ONO2 additive preferentially reacts with Li metal and in situ constructs a stable dual‐layered solid electrolyte interphase film, presenting an inner nitride‐rich layer and an outer flexible PCL‐based layer on the surface of Li metal anode. As a result, the Li metal anode delivers an impressive long‐term cycling performance over 1400 h at an elevated area capacity of 10.0 mAh cm−2 and an ultrahigh current density of 10.0 mA cm−2 in the Li symmetrical cells. Moreover, the PCL‐ONO2 additive enables the full cells constructed by coupling high‐loading LiFePO4 (20.0 mg cm−2) or LiNi0.5Co0.2Mn0.3 (16.5 mg cm−2) cathode and thin Li metal anode (≈50 µm) to demonstrate greatly improved cycling stability and rate capability.

Advanced Micro/Nanostructure Silicon-Based Anode Materials for High-Energy Lithium-Ion Batteries: From Liquid- to Solid-State Batteries

“…Moreover, Si’s high Young’s modulus endows it with dimensional robustness under pressure and reliable performance at ambient temperatures . Notably, the inherent air stability of Si obviates the need for the stringent conditions of a glovebox during anode fabrication, allowing for a more straightforward process in a dry environment. , Importantly, the integration of Si anodes into existing LIBs production lines presents a streamlined avenue toward manufacturing. Hence, Si is poised with promising industrial prospects within the solid-state battery domain, holding the potential to take the lead over lithium metalan accomplishment that could propel the commercialization of advanced cathodes when paired with high-voltage, high-capacity counterparts in the field of SSBs.…”

A Review on Covalent Organic Frameworks as Artificial Interface Layers for Li and Zn Metal Anodes in Rechargeable Batteries

“…used polyhexylactone (PCL‐ONO 2 ) prepared by acylated diol (PCL‐diol) as a new electrolyte additive to realize the introduction of high concentration NO 3 − into carbonate electrolyte. [ 122 ] PCL‐ONO 2 will preferentially react with Li metal to form a bilayer SEI with an internal nitrogen‐rich layer and an external flexible‐rich organic layer. The internal rigid nitrogen‐rich layer can inhibit Li dendrite growth, inhibit solvent penetration, and promote the rapid transfer of Li + .…”

Fluorinated Thiophene-Based Electrolyte Additives Enable a Robust Cathode Electrolyte Interphase with Conformal Homogeneity for a High-Voltage LiNi0.8Co0.15Al0.05O2 Cathode

“…As the requirement of high-performance batteries becomes more and more outstanding in the energy storage devices, such as electronic mobile and electrical vehicles, lithium–ion batteries (LIBs) have attracted more and more attention due to its environment friendliness, high safety, and satisfactory durability. − However, the current development of LIBs cannot meet the increasing energy density demand of large-scale energy storage systems due to the sluggish exploration of high voltage cathodes and/or high specific capacity electrode material, as well as the insufficiently stable interphase on high-capacity electrodes. − Compared to the high specific capacity of the Si/graphite anode, the output capacity and the operation voltage of the cathode play a determinative role in affecting the overall full-battery performance, i.e., energy density. Therefore, developing a high-voltage cathode with decent cycle durability is of great significance to improve the energy density and the cycle life of LIBs.…”