Work

Rigid Additives Enabling Inorganic‐Rich Interphase via Steric Effects and Van der Waals Force for Stable Lithium Metal Batteries

Year: 2024

Type: article

Abstract: Electrolyte additives (EAs) are cost‐effective for stabilization of lithium metal batteries (LMBs). Nevertheless, most EAs are gradually consumed during the lithium deposition process, rendering them inadequate for long‐term cyclability. Herein, a novel hybrid metal–organic framework (MOF)‐based non‐expendable additive is prepared through polymerization of pentaerythritol tetraacrylate (PETEA) on a zeolitic imidazolate framework (ZIF‐67). Owing to the partial coating by PETEA‐based polymer, the exposed unsaturated metal sites of ZIF‐67 still attenuate the interaction between lithium ions (Li+) and anions, enabling rapid electrochemical kinetics and uniform Li deposition. Concurrently, the polymerized PETEA partially enters the Li+ solvation sheath and expels some organic solvents through Van der Waals interactions, which promotes the derivation of an inorganic‐rich SEI and inhibits dendrite formation. Accordingly, this additive‐contained Li||Li symmetric cell exhibits a stability over 1200 h with a small overpotential of 75 mV. Additionally, the assembled Li||LiFePO4 full cells with negative/positive ratio of 1.76 delivers a stable cyclability over 400 cycles at 0.5 C. Moreover, the Li||LiNi0.8Mn0.1Co0.1O2 high‐voltage full cell displays an impressive capacity retention of 80% over 311 cycles at 0.5 C. This study provides a valuable guidance to design non‐expendable multifunctional EAs for advancing high‐performance LMBs.

Source: Advanced Functional Materials

DOI: 10.1002/adfm.202419656