Phenoxy Radical‐Induced Formation of Dual‐Layered Protection Film for High‐Rate and Dendrite‐Free Lithium‐Metal Anodes

Abstract

The uncontrollable dendrite growth of Li metal anode leads to poor cycle stability and safety concerns, hindering its utilization in high energy density batteries. Herein, a phenoxy radical Spiro‐O8 is proposed as an artificial protection film for Li metal anode owing to its excellent film‐forming capability and remarkable ionic conductivity. A spontaneous redox reaction between the Spiro‐O8 and Li metal results in the formation of a uniform and highly ionic conductive organic film in the bottom. Meanwhile, the phenoxy radicals on surface of Spiro‐O8 facilitate the decomposition of Li salt upon exposed to the ether electrolyte and lead the formation of LiF film on the top. Arising from the synergistic effects of inner high ionic conductive film and outer rigid film, stable Li plating/stripping can be realized at a high current density (4000 cycles at 10 mA cm−2) and a high areal capacity of 5 mAh cm−2 for 550 h with an ultrahigh Li utilization rate of 54.6 %. As a proof of concept, this work shows a facile strategy to rationally fabricate dual‐layered interfaces for Li metal anodes.

WITHDRAWN: A voltage-driven dissoluble electrolyte additive enables high-rate and ultralong-life lithium metal batteries

“…The reason of using carbon cloth as matrix is that the three-dimensional (3D) structure of carbon cloth can not only offer a stable host for Li plating/stripping to signi cantly mitigate the volume change of electrode during cycling [34][35][36] , but also provide the possibility for the industrialization of 3D Li-C composite anode due to the convenience of processing 37 . Some previous studies have shown that the cycle stability of Li metal anode in a full cell is worse than that in the symmetrical cell 14,38,39 . Accordingly, we evaluated the electrochemical performance of t-Li 2 ZrF 6 -rich SEI in Li-C||LPF full cells rather than symmetrical cells.…”

Enhanced Li-Ion Diffusion and Cycling Stability of Ni-Free High-Entropy Spinel Oxide Anodes with High-Concentration Oxygen Vacancies

“…3,4 For protecting the environment and achieving the purpose of sustainable development, the development and utilization of new energy are urgently needed. 5,6 Efficient energy storage has been an important bridge for reconciling the immediate quantity of electricity supply and demand, 7,8 so it is necessary to develop an efficient and green secondary energy storage system. 9,10 LIBs are widely used because of their high specific capacity and high security.…”

“…Energy and sustainable development remain the main concerns of all countries in the 21st century. , However, the use of fossil fuels has resulted in many environmental problems, such as increased smog, intensified greenhouse effect, frequent acid rain, and so on. , For protecting the environment and achieving the purpose of sustainable development, the development and utilization of new energy are urgently needed. , Efficient energy storage has been an important bridge for reconciling the immediate quantity of electricity supply and demand, , so it is necessary to develop an efficient and green secondary energy storage system. , LIBs are widely used because of their high specific capacity and high security. , For the current increasing demand, the existing LIBs have been difficult to meet, so it is necessary to develop a new generation of LIB electrode material. , …”

Molecular engineering regulation redox‐dual‐active‐center covalent organic frameworks‐based anode for high‐performance Li storage

“…Nevertheless, with the ever‐increasing demand for LIBs, it is urgently important to construct novel electrode material with high‐performance Li storage and high‐capacity 1–3 . Previous works are mainly concentrated on inorganic compounds (such as transition metal oxide, metal phosphate, sulfide, graphite, P, and Si) as the cathode or anode 4–8 . However, these electrode materials have several defects, including intricate preparation procedure, high toxicity, high‐cost, rapid capacity decay due to their volume expansion during the discharge process 9–11 .…”

“…[1][2][3] Previous works are mainly concentrated on inorganic compounds (such as transition metal oxide, metal phosphate, sulfide, graphite, P, and Si) as the cathode or anode. [4][5][6][7][8] However, these electrode materials have several defects, including intricate preparation procedure, high toxicity, high-cost, rapid capacity decay due to their volume expansion during the discharge process. [9][10][11] This is to the disadvantage of practical application of LIBs.…”