Lithium-ion battery recycling through an integrated electro-membrane crystallization technology
Yan Zhao, Yangbo Qiu, Lei Xia, Xi Zhang, Shuang Zheng, Gang Lü, Jin Shang, Raf Dewil, Seth B. Darling, Bart Van der Bruggen, Chuyang Y. Tang
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. This study presents a scalable and sustainable electro-membrane crystallization-assisted general recycling technology that efficiently recovers high-purity lithium, manganese, nickel, and cobalt from spent lithium-ion batteries.