Lithiation-Aided Conversion of End-of-Life Lithium-Ion Battery Anodes to High-Quality Graphene and Graphene Oxide

In the past two decades, lithium-ion (Li-ion) batteries have transformed the appearance of the world. Along with the ever-increasing production and usage are the tremendous number of retired batteries, which have created social and environmental issues, making battery recycling an urgent task. Graphene has exhibited outstanding electronic and mechanical properties but it is still difficult to fabricate high-quality graphene with feasible procedures at low cost. Here, a strategy of smartly converting retired Li-ion battery anodes to graphene and graphene oxide is proposed. The graphite powders collected from end-of-life Li-ion batteries exhibited irregular expansion because of the lithium-ion intercalation and deintercalation in the anodegraphite during battery charge/discharge. Such prefabrication process facilitated both chemical and physical exfoliations of the graphite. Comparing with the graphene oxide derived from pristine, untreated graphite, the graphene oxide from anodegraphite exhibited superlative homogeneity and electrochemical properties. The lithiation aided pre-expansion enabled 4 times enhancement of graphene productivity by shear mixing. Furthermore, the graphene fabrication was seamlessly inserted into the currently used battery recycling streamline in which the acid treatment was found to further swell the graphite lattice, pushing up the graphene productivity to 83.7% (10 times higher than that of pristine graphite powders). The findings create new opportunities for capitalizing on waste batteries to produce high-quality graphene and its derivatives.