Efficient and economical recovery of lithium, cobalt, nickel, manganese from cathode scrap of spent lithium-ion batteries

Abstract A combined process was presented to recover valuable metals from lithium nickel cobalt manganese (NCM) cathodes of spent lithium-ion batteries. In this process, the cathode scrap was first roasted with carbonaceous reductant, and then carbonation water leaching was employed to selectively extract Li from the roasted cathodes. Finally, the obtained residue was leached in sulfuric acid solution to recover Co, Ni and Mn. A systematic investigation combining thermodynamic analysis, leaching experiments and characterization was conducted to explore the effect of operating conditions and leaching mechanism. The results indicate that the leaching of Li is significantly improved by injecting of CO2 into the leaching system, and more than 80% of Li can be leached within 10 min at a low liquid-solid ratio. High-quality Li2CO3 can be prepared from the leachate by direct evaporation. More than 96% of Ni, Co and Mn are extracted without adding reductant under the conditions of a H2SO4 dosage of 1.15 times the theoretical value, a time of 2.5 h, a temperature of 55 °C and a liquid-solid ratio of 3.5 mL g−1. The acid leaching process is more efficient and economical, which is ascribed to the transformation of the low-valence states of metals with high activity after reduction roasting.

[1]  Guoyong Huang,et al.  Recovery of lithium from the effluent obtained in the process of spent lithium-ion batteries recycling. , 2017, Journal of environmental management.

[2]  P. Lens,et al.  Leaching and selective zinc recovery from acidic leachates of zinc metallurgical leach residues. , 2017, Journal of hazardous materials.

[3]  S. Nishihama,et al.  Selective Recovery of Lithium from Cathode Materials of Spent Lithium Ion Battery , 2016 .

[4]  B. D. Pandey,et al.  Hydrometallurgical processing of spent lithium ion batteries (LIBs) in the presence of a reducing agent with emphasis on kinetics of leaching , 2015 .

[5]  Chein-Chi Chang,et al.  A combined recovery process of metals in spent lithium-ion batteries. , 2009, Chemosphere.

[6]  Liping Xu,et al.  An atom-economic process for the recovery of high value-added metals from spent lithium-ion batteries , 2016 .

[7]  P. Dvořák,et al.  RECOVERY OF LITHIUM FROM WASTE MATERIALS , 2012 .

[8]  B. Swain Recovery and recycling of lithium: A review , 2017 .

[9]  Li Li,et al.  Sustainable Recovery of Cathode Materials from Spent Lithium-Ion Batteries Using Lactic Acid Leaching System , 2017 .

[10]  Xianlai Zeng,et al.  Novel approach to recover cobalt and lithium from spent lithium-ion battery using oxalic acid. , 2015, Journal of hazardous materials.

[11]  M. Kocakerim,et al.  Dissolution of Colemanite in Aqueous Solutions Saturated with Both Sulfur Dioxide (SO2) Gas and Boric Acid , 2006 .

[12]  Hongbin Cao,et al.  Selective recovery of valuable metals from spent lithium-ion batteries – Process development and kinetics evaluation , 2018 .

[13]  Hongrui Ma,et al.  Recovery of valuable metals from waste cathode materials of spent lithium-ion batteries using mild phosphoric acid. , 2017, Journal of hazardous materials.

[14]  Callie W. Babbitt,et al.  Targeting high value metals in lithium-ion battery recycling via shredding and size-based separation. , 2016, Waste management.

[15]  Zhenyu Liu,et al.  Kinetics of Vanadium Leaching from a Spent Industrial V2O5/TiO2 Catalyst by Sulfuric Acid , 2014 .

[16]  Diran Apelian,et al.  A novel method to recycle mixed cathode materials for lithium ion batteries , 2013 .

[17]  O. Quiroga,et al.  Dissolution kinetics of hydroboracite in water saturated with carbon dioxide , 2000 .

[18]  Zhenming Xu,et al.  Environmentally-friendly oxygen-free roasting/wet magnetic separation technology for in situ recycling cobalt, lithium carbonate and graphite from spent LiCoO2/graphite lithium batteries. , 2016, Journal of hazardous materials.

[19]  B. D. Pandey,et al.  Extraction of lithium from primary and secondary sources by pre-treatment, leaching and separation: A comprehensive review , 2014 .

[20]  Hongxu Li,et al.  A promising approach for the recovery of high value-added metals from spent lithium-ion batteries , 2017 .

[21]  Jiefeng Xiao,et al.  Recycling metals from lithium ion battery by mechanical separation and vacuum metallurgy. , 2017, Journal of hazardous materials.

[22]  Keqiang Qiu,et al.  Organic oxalate as leachant and precipitant for the recovery of valuable metals from spent lithium-ion batteries. , 2012, Waste management.

[23]  Faqiang Li,et al.  Refining of crude Li2CO3 via slurry phase dissolution using CO2 , 2007 .

[24]  Dawei Song,et al.  LiCoO2: recycling from spent batteries and regeneration with solid state synthesis , 2015 .

[25]  Guoyong Huang,et al.  Synthesis and performance of spherical LiNixCoyMn1-x-yO2 regenerated from nickel and cobalt scraps , 2016 .

[26]  Oladele A Ogunseitan,et al.  Potential environmental and human health impacts of rechargeable lithium batteries in electronic waste. , 2013, Environmental science & technology.

[27]  Xingfu Song,et al.  Recovery of Lithium, Nickel, Cobalt, and Manganese from Spent Lithium-Ion Batteries Using l-Tartaric Acid as a Leachant , 2017 .

[28]  J. Jandova,et al.  Processing of spent Li/MnO2 batteries to obtain Li2CO3 , 2006 .

[29]  Hongbin Cao,et al.  Lithium Carbonate Recovery from Cathode Scrap of Spent Lithium-Ion Battery: A Closed-Loop Process. , 2017, Environmental science & technology.

[30]  G Prabaharan,et al.  An innovative approach to recover the metal values from spent lithium-ion batteries. , 2016, Waste management.

[31]  Yi Zhang,et al.  Spent lithium-ion battery recycling - Reductive ammonia leaching of metals from cathode scrap by sodium sulphite. , 2017, Waste management.

[32]  T. Çalban,et al.  Leaching kinetics of colemanite in potassium hydrogen sulphate solutions , 2012 .

[33]  M. Ojeda,et al.  Cathodes of spent Li-ion batteries: Dissolution with phosphoric acid and recovery of lithium and cobalt from leach liquors , 2017 .

[34]  N. Haque,et al.  Indirect Carbonation of Victorian Brown Coal Fly Ash for CO2 Sequestration: Multiple-Cycle Leaching-Carbonation and Magnesium Leaching Kinetic Modeling , 2014 .

[35]  M. Avrami Kinetics of Phase Change. I General Theory , 1939 .