Hydrogen-Type Binding Sites in Carbonaceous Electrodes for Rapid Lithium Insertion

ACS Appl Mater Interfaces. 2023 Aug 23;15(33):39211-39217. doi: 10.1021/acsami.3c05047. Epub 2023 Aug 11.

Abstract

Direct pyrolysis of coronene at 800 °C produces low-surface-area, nanocrystalline graphitic carbon containing a uniquely high content of a class of lithium binding sites referred to herein as "hydrogen-type" sites. Correspondingly, this material exhibits a distinct redox couple under electrochemical lithiation that is characterized as intermediate-strength, capacitive lithium binding, centered at ∼0.5 V vs Li/Li+. Lithiation of hydrogen-type sites is reversible and electrochemically distinct from capacitive lithium adsorption and from intercalation-type binding between graphitic layers. Hydrogen-type site lithiation can be fully retained even up to ultrafast current rates (e.g., 15 A g-1, ∼40 C) where intercalation is severely hampered by ion desolvation kinetics; at the same time, the bulk nature of these sites does not require a large surface area, and only minimal electrolyte decomposition occurs during the first charge/discharge cycle, making coronene-derived carbon an exceptional candidate for high-energy-density battery applications.

Keywords: anode; carbon; energy storage; graphitic; insertion mechanism; lithium-ion; pseudocapacitive; rapid charging.