Grafting a Polymer Coating Layer onto Li1.2 Ni0.13 Co0.13 Mn0.54 O2 Cathode by Benzene Diazonium Salts to Facilitate the Cycling Performance and High-Voltage Stability.

Li-rich Mn-based cathodes have been regarded as promising cathodes for lithium-ion batteries because of their low cost of raw materials (compared with Ni-rich layer structure and LiCoO2 cathodes) and high energy density. However, for practical application, it needs to solve the great drawbacks of Li-rich Mn-based cathodes like capacity degradation and operating voltage decline. Herein, an effective method of surface modification by benzene diazonium salts to build a stable interface between the cathode materials and the electrolyte is proposed. The cathodes after modification exhibit excellent cycling performance (the retention of specific capacity is 84.2% after 350 cycles at the current density of 1 C), which is mainly attributed to the better stability of the structure and interface. This work provides a novel way to design the coating layer with benzene diazonium salts for enhancing the structural stability under high voltage condition during cycling.

Hydrogen-Bonded Organic Framework as Superior Separator with High Lithium Affinity C═N Bond for Low N/P Ratio Lithium Metal Batteries.

Lithium dendrite and side reactions are two major challenges for lithium metal anode. Here, the highly lithophilic triazine ring in the hydrogen-bonded organic framework is recommended to accelerate the desolvation process of lithium ions. Among them, the formation of Li-N bonds between lithium ions and the triazine ring in CAM reduces the diffusion energy barrier of Li+ crossing the SEI interface and the desolvation energy barrier of Li+ exiting from the solvent sheath so that the rapid and homogeneous deposition of lithium-ion can be achieved. Meanwhile, the lithium-ion migration coefficient can be as high as 0.70. CAM separator is used to assemble lithium metal batteries with nickel-rich cathodes (NCM 622). When N/P = 8 and 5, the capacity retention rates of Li-NCM 622 full cell are 78.2% and 80.5% after 200 and 110 cycles, respectively, and the Coulomb efficiency can be maintained at 99.5%, showing excellent cycle stability.

Interface Engineering of All-Solid-State Batteries Based on Inorganic Solid Electrolytes.

All-solid-state batteries (ASSBs) based on inorganic solid electrolytes (SEs) are one of the most promising strategies for next-generation energy storage systems and electronic devices due to the higher energy density and intrinsic safety. However, the poor solid-solid contact and restricted chemical/electrochemical stability of inorganic SEs both in cathode and anode SE interfaces cause contact failure and the degeneration of SEs during prolonged charge-discharge processes. As a result, the increasing interface resistance significantly affects the coulombic efficiency and cycling performance of ASSBs. Herein, we present a fundamental understanding of physical contact and chemical/electrochemical features of ASSB interfaces based on mainstream inorganic SEs and summarize the recent work on interface modification. SE doping, optimizing morphology, introducing interlayer/coating layer, and utilizing compatible electrode materials are the key methods to prevent side reactions, which are discussed separately in cathode/anode-SE interface. We also highlight the constant extra stack pressure applied during ASSB cycling, which is important to the electrochemical performance. Finally, our perspectives on interface modification for practical high-performance ASSBs are put forward.