Toward Circular Carbon: Upcycling Coke Oven Waste into Graphite Anodes for Lithium-Ion Batteries

Abstract

This study presents a sustainable upcycling strategy to convert “Pit,” a carbon-rich coke oven by-product from steel manufacturing, into high-purity graphite for use as an anode material in lithium-ion batteries. Despite its high carbon content, raw Pit contains significant impurities and has irregular particle morphology, which limits its direct application in batteries. We employed a multi-step, additive-free refinement process—including jet milling, spheroidization, and high-temperature graphitization—to enhance carbon purity and structural properties. The processed Pit-derived graphite showed a much-improved particle size distribution (D50 reduced from 25.3 μm to 14.8 μm & Span reduced from 1.72 to 1.23), increased tap density (from 0.54 to 0.80 g/cm3), and reduced BET surface area, making it suitable for high-performance lithium-ion batteries anodes. Structural characterization by XRD and TEM confirmed dramatically enhanced crystallinity after graphitization (graphitization degree increasing from ~13 for raw Pit to 95.7% for graphitized Pit at 3000 °C). The fully processed graphite (denoted S_Pit3000) delivered a reversible discharge capacity of 346.7 mAh/g with an initial Coulombic efficiency of 93.5% in half-cell tests—comparable to commercial artificial graphite. Furthermore, when composited with silicon oxide to form a hybrid anode, the material achieved an even higher capacity of 418.0 mAh/g under high mass loading conditions. These results highlight the feasibility of transforming industrial coke waste into value-added electrode materials through environmentally friendly physical processes. The upcycled graphite anode meets industrial performance standards, demonstrating a promising route toward circular economy solutions in both the steel and battery industries.