Lithium-ion battery recycling through an integrated electro-membrane crystallization technology.

Abstract

Lithium-ion battery (LIB) recycling is crucial for energy security, environmental sustainability, and economic viability, as the finite lifespan of LIBs results in a significant annual accumulation of spent units. However, effectively and precisely recovering valuable metal ions such as Li⁺, Mn²⁺, Ni²⁺ and Co²⁺ from complex LIB leaching solutions remains a major challenge. Here, we present a scalable electro-membrane crystallization-assisted general recycling (e-MCGR) technology for the selective and efficient recovery of those metal ions from LIB leaching solutions. By synergistically integrating electrochemical and electro-membrane technologies, our proposed technology incorporates four key configurations: selective membrane dual-stage distillation, bipolar membrane in-situ crystallization, membrane metal-complexing ex-situ crystallization, and membrane metal-extracting temporal crystallization. We systematically analyze the metal-ion transfer kinetics of electro-membranes (ion selectivity and permeation rates) and the performance of electro-membrane crystallization systems (recovery rates and product purity), alongside evaluating energy consumption, economic viability, and environmental benefits. Our optimized e-MCGR process achieves a recovery of 95.5% for Li⁺, 99.5% for Mn²⁺, 83.1% for Ni²⁺, and 87.3% for Co²⁺, yielding high product purities of 99.9% for Li₂CO₃, 99.9% for Mn₃O₄, 99.5% for Ni(OH)₂ and 92.5% for Co(OH)₂. The e-MCGR technology demonstrates significant potential to reshape LIB recycling paradigms, aligning technological efficiency with energy, environmental and economic sustainability.