Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging

Rapid charging of Li-ion batteries is limited by lithium plating on graphite anodes, whereby Li+ ions are reduced to Li metal on the graphite particle surface instead of inserting between graphitic layers, which directly contributes to cell capacity loss because of the low reversibility of the Li plating/stripping process. Precisely identifying the onset and amount of Li plating is therefore vital in order to remedy these issues. We demonstrate a titration technique with a detection limit of 20 nmol (5 × 10–4 mAh) of Li that can be used to quantify inactive Li that remains on the graphite electrode after fast charging. The titration is extended to quantify the total amount of solid carbonate species and lithium acetylide (Li2C2) within the solid–electrolyte interphase (SEI), and electrochemical modeling is used to determine the Li plating exchange current density (10 A/m2) and stripping efficiency (65%) of plated Li metal on graphite. These techniques provide a highly accurate measure of the onset of Li plating and quantitative insight into graphite SEI evolution during fast charging.