The Defect Chemistry of Carbon Frameworks for Regulating the Lithium Nucleation and Growth Behaviors in Lithium Metal Anodes

Carbon materials have been widely considered as the frameworks in lithium (Li) metal anodes due to their lightweight, high electrical conductivity, and large specific surface area. Various heteroatom-doping strategies have been developed to enhance the lithiophilicity of carbon frameworks, thus rendering a uniform Li nucleation in working Li metal batteries. The corresponding lithiophilicity chemistry of doping sites has been comprehensively probed. However, various defects are inevitably introduced into carbon materials during synthesis and their critical role in regulating Li nucleation and growth behaviors is less understood. In this contribution, the defect chemistry of carbon materials in Li metal anodes is investigated through first-principles calculations. The binding energy towards a Li atom and the critical current density are two key descriptors to reveal the defect chemistry of carbon materials. Consequently, a diagram of designing carbon frameworks with both high lithiophilicity and a large critical current density is built, from which the Stone-Wales defect is predicted to possess the best performance for delivering a uniform Li deposition. This work uncovers the defect chemistry of carbon frameworks and affords fruitful insights into defect engineering for achieving dendrite-free Li metal anodes.