friendliness. Additionally, there are numerous additional electrochemical battery performance characteristics that play an equally important role such as longterm cycling performance (cycle life), calendar life, Coulombic efficiency (measure for charge loss due to irreversible side reactions), energy efficiency, and the performance at different charge/discharge rates or at different temperatures. From this perspective, researchers constantly explore new anode and cathode materials for existing battery technologies as well as conceive new electrochemical energy storage concepts. In this context, the last two decades have seen a surge of reports on various low-cost anodes and cathodes for Li-ion and post-Li-ion batteries (Na-, K-, Ca-, Mg-, and Al-ion batteries). Moreover, new electrochemical concepts called graphite dual-ion batteries (GDIBs) have recently attracted significant attention. GDIBs show high potential for the use in grid-scale energy storage applications due to their low cost, relatively high energy densities of up to ≈200 Wh kg −1 and cyclic stability (thousands of cycles and potentially more). In this review, we provide an introduction to the basics of GDIBs. In particular, we discuss their operating mechanisms and cover the topic of energy density calculations. In addition, we highlight the importance of correct reporting of the performance metrics with respect to the energy density of GDIBs. Next, we discuss in detail factors governing the electrochemical performance of graphite cathodes in dual-ion batteries, such as graphite structure, morphology, and particle size. The factors that impact the voltage of electrochemical anion intercalation/deintercalation into graphite will be described as well. With respect to the practical application of the GDIBs, the current collector issues and volume changes of GDIBs will be discussed in the final sections.
Historical AspectsAlthough GDIBs may appear to be newcomers in battery research, they have a long and tangible history. The concept of GDIBs was introduced in the patents of McCullough et al. [1,2] in 1989. The experimental example consisted of two graphite electrodes acting as an anode and a cathode, and a 15 wt% solution of LiClO 4 in propylene carbonate acting as an electrolyte. The oxidation and reduction of cathodic and anodic graphite electrodes occur with concomitant intercalation of Li + cations and ClO 4 − anions, respectively. The latter process is known as the formation of donor-type (cationic) or acceptor-type (anionic) graphite intercalation compounds (GICs). Some years later, in the 1990s, the intercalation of various anions into graphite Rechargeable graphite dual-ion batteries (GDIBs) have attracted the attention of electrochemists and material scientists in recent years due to their low cost and high-performance metrics, such as high power density (≈3-175 kW kg −1 ), energy efficiency (≈80-90%), long cycling life, and high energy density (up to 200 Wh kg −1 ), suited for grid-level stationary storage of electricity.The key feature of GD...