Hydrogen Bond Networks Stabilized High-Capacity Organic Cathode for Lithium-Ion Batteries.

Angewandte Chemie (International ed. in English)(2023)

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Abstract
High-capacity small organic materials are plagued by their high solubility. Here we proposed constructing hydrogen bond networks (HBN) via intermolecular hydrogen bonds to suppress the solubility of active material. The illustrated 2, 7- diamino-4, 5, 9, 10-tetraone (PTO-NH ) molecule with intermolecular hydrogen (H) bond between O in -C=O and H in -NH , which make PTO-NH presents transverse two-dimensional extension and longitudinal π-π stacking structure. In situ Fourier transform infrared spectroscopy (FTIR) has tracked the reversible evolution of H-bonds, further confirming the existence of HBN structure can stabilize the intermediate 2-electron reaction state. Therefore, PTO-NH with HBN structure has higher active site utilization (95 %), better cycle stability and rate performance. This study uncovers the H-bond effect and evolution during the electrochemical process and provides a strategy for materials design.
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Key words
High Capacity,Hydrogen Bond Networks,Intermolecular Hydrogen Bonds,Lithium Batteries,PTO-NH2
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