This article first describes fundamental aspects of the electrochemical intercalation of anions into graphite. Then, the electrochemical preparation of covalent-type graphite intercalation comopouds, especially, graphite oxide and application of graphite as the cathode of dual-ion battery are discussed.

Abstract

In this review, fundamental aspects of the electrochemical intercalation of anions into graphite have been first summarized, and then described the electrochemical preparation of covalent-type GICs and application of graphite as the cathode of dual-ion battery. Electrochemical overoxidation of anion GICs provides graphite oxide and covalent-fluorine GICs, which are key functional materials for various applications including energy storage devices. The reaction conditions to obtain fully oxidized graphite has been mentioned. Concerning the application of graphite for the cathode of dual-ion battery, it stably delivers about 110 mA h g⁻¹ of reversible capacity in usual organic electrolyte solutions. The combination of anion and solvent as well as the concentration of the anions in the electrolyte solutions greatly affect the performance of graphite cathode such as oxidation potential, rate capability, cycling properties, etc. The interfacial phenomenon is also important, and fundamental studies of charge transfer resistance, anion diffusion coefficient, and surface film formation behavior have also been summarized. The use of smaller anions, such as AlCl₄ ⁻, Br⁻ can increase the capacity of graphite cathode. Several efforts on the structural modification of graphite and development of electrolyte solutions in which graphite cathode delivers higher capacity were also described.