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Sustainable Upcycling of Battery Graphite Scrap via Synergistic Air Oxidation and Ammonia Etching
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DOI：10.1039/D6GC02178F.png)
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Abstract
En 中文
The exponential growth of the lithium-ion battery industry has generated substantial manufacturing scrap; presenting an urgent imperative for sustainable resource recovery.Traditional graphite anode recycling relies heavily on volatile organic solvents and corrosive inorganic acids; posing severe environmental and occupational risks. This study introduces a zero-waste; closed-loop upcycling framework for battery manufacturing scraps utilizing solely pure deionized water; static air; and recoverable aqueous ammonia. By exploiting intrinsic thermodynamic wettability contrasts; complete binder-free aqueous delamination of the active graphite coating from the copper foil is achieved under ultrasonic assistance. Subsequent low-temperature ( 440°C)air pyrolysis simultaneously decomposes the polyvinylidene fluoride binder and oxidizes trace copper impurities. Final purification via room-temperature ammonia leaching selectively extracts copper as [Cu(NH 3 ) 4 ] 2+ ; reducing residual copper concentrations to an ultralow 4.65 ppm without generating acidic effluents. Crucially; the synergistic application of thermal air oxidation and mild alkaline etching induces controlled microstructural remodeling. This dual-etching mechanism generates a hierarchical pore structure that nearly doubles the specific surface area (from 4.4 to 8.3 m 2 g -1 ) while introducing topological edge defects. This rationally engineered porosity facilitates a kinetic shift from bulk diffusion to pseudocapacitive charge storage; significantly accelerating solid-state lithium-ion transport. Consequently; the regenerated graphite delivers an initial discharge capacity of 372.71 mAh g -1 ; an initial Coulombic efficiency of 93.6%; and robust long-term cycling stability in full-cell configurations; maintaining 80.35% capacity over 800 cycles at a rigorous 2 C rate.This inherently benign methodology transforms hazardous manufacturing waste into high-performance; fast-charging energy storage materials.
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