Sustainable Recycling and Regeneration of Cathode Scraps from Industrial Production of Lithium-Ion Batteries

The burst demand of lithium-ion batteries (LIBs) for energy storage leads to an increasing production of LIBs. The huge amount of electrode scraps produced during the industrial production cannot be overlooked. A sustainable and simple method was developed to regenerate Li(Ni1/3Co1/3Mn1/3)O2 electrode scraps as new cathodes for LIBs. Three different separation processes, including direct calcination, solvent dissolution, and basic solution dissolution, were applied to obtain the active materials. Then, a heat treatment was used to regenerate the scraps. The effects of separation methods and heat treatment temperatures were systematically investigated. The results show that the scraps regenerated with solvent dissolution and heat treatment at 800 °C deliver the highest reversible discharge capacities of 150.2 mA h g–1 at 0.2C after 100 cycles with capacity retention of 95.1%, which is comparable with commercial Li(Ni1/3Co1/3Mn1/3)O2 cathodes. When cycled at 1C, a highly reversible discharge capacity of 128...

[1]  J. Dahn,et al.  Influence of LiF Additions on Li [ Ni x Co1 − 2x Mn x ] O 2 Materials Sintering, Structure, and Lithium Insertion Properties , 2004 .

[2]  Tao Zhou,et al.  Sustainable Recovery of Metals from Spent Lithium-Ion Batteries: A Green Process , 2015 .

[3]  Dawei Song,et al.  Recovery and heat treatment of the Li(Ni1/3Co1/3Mn1/3)O2 cathode scrap material for lithium ion battery , 2013 .

[4]  L. Monconduit,et al.  The Solid Electrolyte Interphase a key parameter of the high performance of Sb in sodium-ion batteries: Comparative X-ray Photoelectron Spectroscopy study of Sb/Na-ion and Sb/Li-ion batteries , 2015 .

[5]  Hang Hu,et al.  Hydrometallurgical recovery of metal values from sulfuric acid leaching liquor of spent lithium-ion batteries. , 2015, Waste management.

[6]  M. R. Palacín,et al.  Why do batteries fail? , 2016, Science.

[7]  Zhiwen Zeng,et al.  Process for the recovery of cobalt oxalate from spent lithium-ion batteries , 2011 .

[8]  Hannah M. Dahn,et al.  Impact of Binder Choice on the Performance of α-Fe2O3 as a Negative Electrode , 2008 .

[9]  Feng Wu,et al.  Recovery of cobalt and lithium from spent lithium ion batteries using organic citric acid as leachant. , 2010, Journal of hazardous materials.

[10]  S. Oswald.  Binding energy referencing for XPS in alkali metal-based battery materials research (I): Basic model investigations , 2015 .

[11]  Wolfgang Haselrieder,et al.  Recycling of lithium-ion batteries: a novel method to separate coating and foil of electrodes , 2015 .

[12]  Xiaofeng Wang,et al.  Application for Simply Recovered LiCoO2 Material as a High-Performance Candidate for Supercapacitor in Aqueous System , 2015 .

[13]  Feng Wu,et al.  Environmental friendly leaching reagent for cobalt and lithium recovery from spent lithium-ion batteries. , 2010, Waste management.

[14]  Guoyong Huang,et al.  Synthesis and performance of Li[(Ni1/3Co1/3Mn1/3)(1-x)Mgx]O2 prepared from spent lithium ion batteries. , 2013, Journal of hazardous materials.

[15]  P. Biensan,et al.  Surface film formation on electrodes in a LiCoO2/graphite cell: A step by step XPS study , 2007 .

[16]  T. Rojo,et al.  Composition and evolution of the solid-electrolyte interphase in Na2Ti3O7 electrodes for Na-ion batteries: XPS and Auger parameter analysis. , 2015, ACS applied materials & interfaces.

[17]  J. Dahn,et al.  Combinatorially Prepared [LiF]1−xFex Nanocomposites for Positive Electrode Materials in Li-Ion Batteries , 2008 .

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

[19]  D. Deng,et al.  Trash to Treasure: Transforming Waste Polystyrene Cups into Negative Electrode Materials for Sodium Ion Batteries , 2015 .

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

[21]  Chen Jiangping,et al.  Environmentally friendly recycling and effective repairing of cathode powders from spent LiFePO4 batteries , 2016 .

[22]  J. Badyal,et al.  Surface modification of poly(vinylidene difluoride)(PVDF) by LiOH , 1991 .

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

[24]  Dongge Wang,et al.  Heat treatment of LiCoO2 recovered from cathode scraps with solvent method , 2014 .

[25]  De-cheng Li,et al.  Preparation, morphology and electrochemical characteristics of LiNi1/3Mn1/3Co1/3O2 with LiF addition , 2006 .

[26]  M. Armand,et al.  Issues and challenges facing rechargeable lithium batteries , 2001, Nature.

[27]  Feng Wu,et al.  Succinic acid-based leaching system: A sustainable process for recovery of valuable metals from spent Li-ion batteries , 2015 .

[28]  H. Thomas,et al.  A review of processes and technologies for the recycling of lithium-ion secondary batteries , 2008 .

[29]  Jun Lu,et al.  Design of surface protective layer of LiF/FeF3 nanoparticles in Li-rich cathode for high-capacity Li-ion batteries , 2015 .

[30]  Kevin G. Gallagher,et al.  The significance of Li-ion batteries in electric vehicle life-cycle energy and emissions and recycling's role in its reduction , 2015 .

[31]  J. Dahn,et al.  Effect of Heat Treatment on Si Electrodes Using Polyvinylidene Fluoride Binder , 2008 .

[32]  A. Chagnes,et al.  A brief review on hydrometallurgical technologies for recycling spent lithium‐ion batteries , 2013 .

[33]  Xiaojuan Duan,et al.  Facile Preparation of MnO2/Graphene Nanocomposites with Spent Battery Powder for Electrochemical Energy Storage , 2015 .

[34]  Li Li,et al.  Ascorbic-acid-assisted recovery of cobalt and lithium from spent Li-ion batteries , 2012 .

[35]  Jinhui Li,et al.  Recycling of Spent Lithium-Ion Battery: A Critical Review , 2014 .

[36]  Linda Gaines,et al.  To recycle, or not to recycle, that is the question: Insights from life-cycle analysis , 2012 .

[37]  M. Watanabe,et al.  XPS study of lithium surface after contact with lithium-salt doped polymer electrolytes , 2001 .