The recovery of NCM (LiNi x Co y Mn 1-x-y O 2 , abbreviated as NCM) cathode materials from retired lithium-ion batteries is a research hotspot in resource recycling field. Nevertheless, due to aluminum impurities mixed in raw materials, Li(I) and Al(III) ions are easy to combine to form water-insoluble LiAlO 2 during reduction, affecting Li(I) ions’ water-leaching efficiency. In this study, the LiAlO 2 formation environment is analyzed. Thermodynamic analysis reveals that there is generally less spontaneity in the reaction of Li (I) ions with aluminum monomers compared to Al 2 O 3 , and the introduction of CO 2 can inhibit Li-Al-O substance production. Li-Al binding experiments show that there is almost no direct reaction between Li 2 CO 3 and aluminum monomers, but under Ar atmosphere, Li 2 CO 3 and Al 2 O 3 can easily lead to Li-Al binding, a kinetic analysis considers that binding is controlled by chemical reaction, with an activation energy of 57.78 kJ/mol, and the activation energy increases to 88.028 kJ/mol with CO 2 atmosphere. Under reduced optimization conditions (reduction temperature: 500 °C, time: 6 h, and m NCM : m Al = 1: 0.25), the carbonation water-leaching efficiency can reach 95.1% for Li(I) ions and less than 1% for Ni(II), Co(II), Mn(II), and Al(III) ions. Thus, this work offers a theoretical basis for the industrial Li(I) ions’ recovery from aluminum-containing NCM materials.
Guange Wang,Tong Wu,Borui Liu,Shanshan Gong,Qing Huang,Yuefeng Su,Feng Wu,Ryan M. Kelly
Considering that lithium-ion battery (LIB) is still an indispensable and important component of energy storage materials, the sustainable post-processing of spent LIBs in labs or enterprises becomes a tricky problem. Herein, a novel scheme is proposed to dissert the recycling of the spent LIBs. The LIB is recycled into Li(Ni0.9Co0.05Mn0.05)O2 (NCM90) cathode material with high specific capacity by introducing an innovative hydrometallurgy-coprecipitation treatment method. The spent LiCoO2 (LCO) cathode material is firstly leached by sulfuric acid, and the leachate is gradient used as the raw materials to resynthesize high-nickel NCM material by adjusting the leachate dosage to about 50%. Interestingly, when the dosage exceeds 50%, the crystal structure aggravates, and Li+/Ni2+ mixing improves. The specific capacity of regenerated battery is 181.4 mAh g−1 at 0.5 C (1 C = 200 mAh g−1) and the capacity retention achieves 93.2% after 100 cycles. The reasons can be attributed to the cation mixing and crystal strucure and the small amount of Al doping. In conclusion, this combined method recycling of LIBs has huge potential value for environment protection and production.
危险品化学品经营许可证（带存储）