A Novel and Sustainable Approach to Enhance the Li-Ion Storage Capability of Recycled Graphite Anode from Spent Lithium-Ion Batteries

Bhar, Madhushri; Bhattacharjee, Udita; Sarma, Dhritismita; Krishnamurthy, Satheesh; Yalamanchili, Kaliprasad; Mahata, Arup and Martha, Surendra K. (2023). A Novel and Sustainable Approach to Enhance the Li-Ion Storage Capability of Recycled Graphite Anode from Spent Lithium-Ion Batteries. ACS Applied Materials & Interfaces, 15(22) pp. 26606–26618.

DOI: https://doi.org/10.1021/acsami.3c02272

Abstract

The ubiquitous manufacturing of lithium-ion batteries (LIBs) due to high consumer demand produces inevitable e-waste that imposes severe environmental and resource sustainability challenges. In this work, the charge storage capability and Li-ion kinetics of the recovered water-leached graphite (WG) anode from spent LIBs are enhanced by using an optimized amount of recycled graphene nanoflakes (GNFs) as an additive. The WG@GNF anode exhibits an initial discharge capacity of 400 mAh g^–1 at 0.5C with 88.5% capacity retention over 300 cycles. Besides, it delivers an average discharge capacity of 320 mAh g^–1 at 500 mA g^–1 over 1000 cycles, which is 1.5–2 times higher than that of WG. The sharp increase in electrochemical performance is due to the synergistic effects of Li-ion intercalation into the graphite layers and Li-ion adsorption into the surface functionalities of GNF. Density functional theory calculations reveal the role of functionalization behind the superior voltage profile of WG@GNF. Besides, the unique morphology of spherical graphite particles trapping into graphene nanoflakes provides mechanical stability over long-term cycling. This work explains an efficient strategy to upgrade the electrochemical compatibility of recovered graphite anode from spent LIBs toward next-generation high-energy-density LIBs.

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