Advanced Zero-Waste Recycling of Heterogeneous Lithium-Ion Battery Waste Through a Closed-Loop Approach

Abstract

The scalability of current closed-loop battery recycling is fundamentally constrained by a critical industrial bottleneck: the inability to economically process heterogeneous, mixed chemistry waste streams (simultaneous feeds of LFP, high-nickel NMC, and emerging silicon-anode cells) without intensive pre-sorting. This study introduces a disruptive closed-loop architecture that bypasses manual dismantling through an adaptive, selective hydrometallurgical-to-direct regeneration continuum. By deploying localized multi-ion complexation agents coupled with real-time electrochemical phase tuning, our approach simultaneously recovers high-purity transition metals and directly heals degraded crystal lattices across mixed "black mass" inputs without total chemical dissolution. Closed-loop life-cycle and techno-economic analyses reveal a 42% reduction in processing energy and a near-zero secondary wastewater footprint compared to conventional benchmark processes. Crucially, regenerated cathode blends fabricated from random industrial waste feeds exhibit electrochemical performance parity with virgin commercial cells, demonstrating that closed-loop circular manufacturing can transition from idealized single-stream processing to robust, reality-adapted industrial deployment.