Green and Scalable Production of High‐Quality Graphene by Solid Lithiation and Exfoliation

ABSTRACT High‐quality graphene prepared by eco‐friendly green methods is critical for maximizing the performance of its applications. Here, we use solid lithiation and exfoliation to achieve the green and scalable production of high‐quality graphene, avoiding the use of strong oxidants. This intercalation‐exfoliation process yields high‐quality few‐layered graphene nanosheets with an average thickness of 1.1 nm and high crystallinity. The produced graphene nanosheets have a low defect density ( I D / I G ≈0.11) and a high C/O ratio (∼24.6), enabling large‐scale dispersion and production with a yield of 26.7%. Furthermore, our graphene nanosheets show good thermal stability, remaining stable without significant weight loss up to 550°C and almost completely decomposing around 700°C in thermogravimetric analysis. In addition, the as‐exfoliated graphene nanosheets were used as a conductive substrate for an oxygen evolution reaction catalyst. Cobalt‐loaded graphene exhibits excellent catalytic activity and long‐term stability, with an overpotential of 0.34 V at 10 mA cm −2 and a Tafel slope of 99 mV dec −1 . Our work thus provides an efficient, green route to high‐quality graphene, unlocking its potential for next‐generation applications in electronics, energy storage, and composite materials.