Reactivity of Carbonaceous Anodes Used in Lithium-ion Batteries, Part I: Correlation of Structural Parameters and Reactivity

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Abstract
Carbonaceous anodes are the most practical elecrode for application in lithium-ion battery, mainly due to their low cost, flexibility for modification to achieve high energy capacity and high rate capability, abundance and environmentally uniquencess. Despite superior advantages of carbonaceous anodes vs other alternative anode and metallic lithium, there is considerable reactivity of lithiated graphite with organic electrolytes, which is a major safety concern. In this work, we report the nature of gaceous species generated on various carbonaceous anodes during initial charge-discharge cycling. The correlation between structural parameters of carbonaceous materials and their irreversible capacity loss have been investigated. Structural parameters have been studied using x-ray diffraction, Raman spectroscopy, and scanning and transmission electron microscopy. We have found a direct correlation between crystal morphology, degree of disorder, degree of graphitisation and the irreversible capacity loss. There is also a direct correlation between the irrversible capacity loss and the volume of gas generated during initial charge- disharge cycling. Results also show the importance of removing adsorbed and trapped gases in addition to removal of bonded impurities, such as functional groups from carbonaceous electrode before fabrication of batteries.Particular attention is given on thermal analysis for different graphite compounds and the influence of different parameters and conditions: nature of graphite in term of specific surface area, degree of graphitization and the length of microcristallites, degree of intercalation, nature of electrolytes on irreversible capacity loss and volume of gases generated during the initial charge-discharge cycles.