期刊
ACS ENERGY LETTERS
卷 8, 期 5, 页码 2463-2474出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.3c00600
关键词
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This study presents a class of electrostatic covalent organic frameworks (COFs) as molecular traps for high-energy-density Li metal batteries. These COF traps effectively chelate transition metal ions, enhance Li+ desolvation, suppress solvent decomposition, and immobilize anions. The resulting battery with COF traps achieves high energy densities under a constrained cell configuration.
Regulating electrostatic interactions between charged molecules is crucial for enabling advanced batteries with electrochemical reliability. To address this issue, herein, we present a class of electrostatic covalent organic frameworks (COFs) as on-demand molecular traps for high-energy-density Li metal batteries (LMBs). A bipyridine-based COF and its quaternized derivative are synthesized and incorporated into LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes and Li metal protective layers, respectively. These COF molecular traps are effective in chelating transition metal ions dissolved from the cathodes, enhancing Li+ desolvation, suppressing solvent decomposition, and immobilizing anions of electrolytes. The resulting LMB with the COF molecular traps fully utilizes the theoretical specific capacity of NCM811 at cathodes and allows stable Li plating/ stripping at anodes. A pouch-type LMB full cell with the COF molecular traps provides high gravimetric/volumetric energy densities (466.7 Wh k(gcell)( -1)/1370.1 Wh L-cell(-1)) under a constrained cell configuration, exceeding those of previously reported Li metal batteries based on porous crystalline frameworks.
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