Recovery of valuable metal ions from the spent lithium-ion battery using aqueous mixture of mild organic acids as alternative to mineral acids

Abstract A well characterized cathode material (LiCoO2) recovered from spent lithium-ion battery is dissolved in aqueous mixture of citric acid (chelating agent) and ascorbic acid (reductant) at 80 °C. The dissolution proceeds with a reductive-complexing mechanism, and complete dissolution occurs in about 6 h when stoichiometric amount of C/A is used. The dissolution rate constants (k) are 3.1 × 10− 3 min− 1 for Li and 0.8 × 10− 3 min− 1 for Co ions as determined by ‘cubic rate law’ plots. The formation of Co(III)– to Co(II)–citrate during the dissolution is confirmed from the UV–Vis spectra. The dissolved solution was subjected for selective precipitation of cobalt as Co-oxalate and lithium as LiF using oxalic acid and NH4F, respectively. The present study has a merit when compared to literature reports as we make use of mild organic acids as alternatives to mineral acids.

[1]  V. G. Celante,et al.  Electrochemical recovery of cobalt and copper from spent Li-ion batteries as multilayer deposits , 2010 .

[2]  Jinki Jeong,et al.  Hydrometallurgical process for recovery of cobalt from waste cathodic active material generated during manufacturing of lithium ion batteries , 2007 .

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

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

[5]  Y. Nishi.  Lithium ion secondary batteries; past 10 years and the future , 2001 .

[6]  Li Li,et al.  Bioleaching mechanism of Co and Li from spent lithium-ion battery by the mixed culture of acidophilic sulfur-oxidizing and iron-oxidizing bacteria. , 2009, Bioresource technology.

[7]  M. Cassir,et al.  Electrochemical behavior of sebaconitrile as a cosolvent in the formulation of electrolytes at high potentials for lithium-ion batteries , 2014 .

[8]  Florence Ansart,et al.  Advances in the recovering of spent lithium battery compounds , 2002 .

[9]  Denise Crocce Romano Espinosa,et al.  Recycling of batteries: a review of current processes and technologies , 2004 .

[10]  J. Manjanna,et al.  Dissolution studies of chromium substituted iron oxides in reductive-complexing agent mixtures , 2001 .

[11]  Junmin Nan,et al.  Recovery of metal values from spent lithium-ion batteries with chemical deposition and solvent extraction , 2005 .

[12]  Arthur E. Martell,et al.  Critical Stability Constants , 2011 .

[13]  Bruno Scrosati,et al.  A laboratory-scale lithium-ion battery recycling process , 2001 .

[14]  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.

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

[16]  Young Han Kim,et al.  Development of a metal recovery process from Li-ion battery wastes , 2005 .

[17]  Marcelo Borges Mansur,et al.  Analysis of a hydrometallurgical route to recover base metals from spent rechargeable batteries by liquid–liquid extraction with Cyanex 272 , 2006 .

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

[19]  Kang-In Rhee,et al.  Reductive leaching of cathodic active materials from lithium ion battery wastes , 2003 .

[20]  Marcelo Borges Mansur,et al.  Hydrometallurgical separation of aluminium, cobalt, copper and lithium from spent Li-ion batteries , 2009 .

[21]  A. Manthiram,et al.  Chemical Extraction of Lithium from Layered LiCoO2 , 1996 .

[22]  Eric M. Garcia,et al.  Electrochemical recycling of cobalt from cathodes of spent lithium-ion batteries , 2007 .

[23]  Denise Crocce Romano Espinosa,et al.  An overview on the current processes for the recycling of batteries , 2004 .

[24]  John B. Goodenough,et al.  LixCoO2 (0, 1980 .

[25]  Linda Gaines,et al.  Recovery of metals from spent lithium-ion batteries with organic acids as leaching reagents and environmental assessment , 2013 .

[26]  M. G. Segal,et al.  Kinetics of metal oxide dissolution. Reductive dissolution of nickel ferrite by tris(picolinato)vanadium(II) , 1982 .

[27]  Bruno Scrosati,et al.  A laboratory-scale lithium battery recycling process1This work has been presented as an invited talk at the 4th International Battery Recycling Congress, Hamburg, Germany, 1–3 July, 1998.1 , 1999 .

[28]  A. L. Salgado,et al.  Recovery of zinc and manganese from spent alkaline batteries by liquid–liquid extraction with Cyanex 272 , 2003 .

[29]  Peter G. Bruce,et al.  Synthesis of layered LiMnO2 as an electrode for rechargeable lithium batteries , 1996, Nature.

[30]  J. Manjanna,et al.  Preparation and Kinetic Considerations for the Dissolution of Cr‐substituted Iron Oxides in Reductive‐complexing Formulations , 2008 .

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

[32]  Jung-Ho Wee,et al.  A feasibility study on direct methanol fuel cells for laptop computers based on a cost comparison with lithium-ion batteries , 2007 .

[33]  B. D. Pandey,et al.  Recovery of lithium and cobalt from waste lithium ion batteries of mobile phone. , 2013, Waste management.

[34]  Kang-In Rhee,et al.  Preparation of LiCoO2 from spent lithium-ion batteries , 2002 .

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

[36]  J. Dewulf,et al.  Recycling rechargeable lithium ion batteries: Critical analysis of natural resource savings , 2010 .

[37]  Yu-Chuan Lin,et al.  A novel recovery process of metal values from the cathode active materials of the lithium-ion secondary batteries , 2009 .

[38]  Y. J. Lee,et al.  The role of citrate and phthalate during Co(II) coprecipitation with calcite , 2006 .

[39]  Keqiang Qiu,et al.  Vacuum pyrolysis and hydrometallurgical process for the recovery of valuable metals from spent lithium-ion batteries. , 2011, Journal of hazardous materials.

[40]  B. D. Pandey,et al.  Selective separation and recovery of cobalt from leach liquor of discarded Li-ion batteries using thiophosphinic extractant , 2013 .

[41]  D. Ra,et al.  Used lithium ion rechargeable battery recycling using Etoile-Rebatt technology , 2006 .

[42]  Hiroki Nagasawa,et al.  Separation of lithium and cobalt from waste lithium-ion batteries via bipolar membrane electrodialysis coupled with chelation , 2013 .

[43]  Atsushi Iizuka,et al.  Adaptation of minerals processing operations for lithium-ion (LiBs) and nickel metal hydride (NiMH) batteries recycling: Critical review , 2013 .

[44]  B. Friedrich,et al.  Development of a recycling process for Li-ion batteries , 2012 .