Surpassing Metal‐Centric E‐Waste Recycling: Unveiling Graphite in Spent Lithium‐Ion Batteries Towards Electrocatalytic Upcycling

ABSTRACT With tonnes of battery shredded globally, tracing down pathways in upcycling black mass (BM) as catalysts would be a game changer. Existing unwavering synergic combination of inherent metals and graphite in BM drives this novel objective. Herein, we report the critical role of spent graphite for electrocatalytic water splitting applications by systematic evaluation of diverse NMC, LFP, and LCO BM. The study revealed an interesting pattern, wherein the graphite in BM complemented their impurity flaws by delivering an excellent oxygen evolution reaction (OER) activity. Defects, surface activation, structural variation, and metal‐graphite synergism arising from prolonged cycle life served as a serendipitous finding of upcycling BM for OER, despite being loaded with impurities and/or degradation byproducts. Further, among these BM sets, direct upcycling of select graphite‐containing BM via mechanochemical functionalisation aided downsized derivatives delivering an overpotential of 260 mV at 10 mA cm −2 , while functionalized graphite via bioleaching BM recorded an overpotential of 249 mV, an epoch‐making record in graphite upcycling. By correlating the overall insights using advanced material, electrochemical characterisation studies, and life cycle analysis, the current study unlocks spent graphite benefits for achieving sustainable energy solutions and beyond.