Issue 45, 2024

Three-dimensional covalent organic framework-based artificial interphase layer endows lithium metal anodes with high stability

Abstract

To gain a deeper understanding and address the scientific challenges of lithium dendrite growth, a robust solid-state electrolyte interface (SEI) with good mechanical properties and rapid ion conduction is crucial for the advancement of lithium metal batteries. Artificial SEI layers based on organic polymers, such as covalent organic frameworks (COF), have garnered widespread attention due to their flexible structural design and tunable functionality. In this work, a COF with 3D spatial geometric symmetry and a fully covalent dia topology was synthesized and used as artificial SEI layers. A combination of comprehensive DFT calculations and ex situ/in situ characterizations have unraveled the impact of interpenetrated chain segments and anchoring lithiophilic groups on the microscopic dynamics related to Li ion desolvation, charge transfer, migration pathways, and deposition morphology. The ultralow polarization voltage of 46 mV for 9400 hours with a symmetric Li|Li cell at a harsh current density of 10 mA cm−2, as well as the high Li+ utilization, low polarization voltage, and prolonged lifespan for 3D-COF-modified Li|S and Li|LFP full cells, unambiguously corroborate the interphase reliability. This work also aims to shed new light on the use of multi-dimensional porous polymer SEI layers to revive highly stable Li metal batteries.

Graphical abstract: Three-dimensional covalent organic framework-based artificial interphase layer endows lithium metal anodes with high stability

Supplementary files

Article information

Article type
Edge Article
Submitted
07 Aug 2024
Accepted
14 Oct 2024
First published
17 Oct 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 19160-19167

Three-dimensional covalent organic framework-based artificial interphase layer endows lithium metal anodes with high stability

K. Zheng, Z. Gou, C. Zhang, Y. Zhang, Y. Dou, S. Liu, Y. Zhang and Y. Zhang, Chem. Sci., 2024, 15, 19160 DOI: 10.1039/D4SC05297H

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