Recovery of valuable metals from LiNi0.5Co0.2Mn0.3O2 cathode materials of spent Li-ion batteries using mild mixed acid as leachant.

A novel hydrometallurgical process for recycling LiNi0.5Co0.2Mn0.3O2 cathode materials harvested from spent Li-ion batteries (LIBs) is established in this work. The cathode material LiNi0.5Co0.2Mn0.3O2 is dissolved in a mixed acid containing phosphoric acid (leaching agent) and citric acid (leaching agent and reductant). Using 0.2 M phosphoric acid and 0.4 M citric acid with a solid to liquid (S/L) ratio of 20 g/L at 90 °C for 30 min, the proposed method results in a leaching efficiency of ca. 100% for Li, 93.38% for Ni, 91.63% for Co, and 92.00% for Mn, respectively. Kinetics of the leaching process is well described by the Avrami equation. It is found that the leaching process is controlled by surface chemical reactions, and the apparent activation energies (kJ/mol) are 45.83 for Li, 83.01 for Ni, 81.38 for Co and 92.35 for Mn, respectively. With aids of various advanced characterizations methods, including UV-Vis, FT-IR and TOC, we find that there are a great deal of citrates and a small amount of dihydrogen phosphates in the mixed acid leachate. This leaching method enjoys advantages of low acid consumption, short leaching time and no need to add extra reductant.

[1]  John Sullivan,et al.  Impact of recycling on cradle-to-gate energy consumption and greenhouse gas emissions of automotive lithium-ion batteries. , 2012, Environmental science & technology.

[2]  Xiang-pan Chen,et al.  Organic reductants based leaching: A sustainable process for the recovery of valuable metals from spent lithium ion batteries. , 2018, Waste management.

[3]  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 .

[4]  G. P. Nayaka,et al.  Use of mild organic acid reagents to recover the Co and Li from spent Li-ion batteries. , 2016, Waste management.

[5]  N. Bahaloo-Horeh,et al.  Enhanced recovery of valuable metals from spent lithium-ion batteries through optimization of organic acids produced by Aspergillus niger. , 2017, Waste management.

[6]  Li Li,et al.  Preparation of LiCoO2 films from spent lithium-ion batteries by a combined recycling process , 2011 .

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

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

[9]  Yi Zhang,et al.  A novel process for recycling and resynthesizing LiNi1/3Co1/3Mn1/3O2 from the cathode scraps intended for lithium-ion batteries. , 2014, Waste management.

[10]  Tao Zhou,et al.  Hydrometallurgical process for the recovery of metal values from spent lithium-ion batteries in citric acid media , 2014, Waste management & research : the journal of the International Solid Wastes and Public Cleansing Association, ISWA.

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

[12]  Hongbin Cao,et al.  An overview on the processes and technologies for recycling cathodic active materials from spent lithium-ion batteries , 2013 .

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

[14]  Jinhui Li,et al.  Ecodesign in Consumer Electronics: Past, Present, and Future , 2015 .

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

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

[17]  Xiao Lin,et al.  Spent lead-acid battery recycling in China - A review and sustainable analyses on mass flow of lead. , 2017, Waste management.

[18]  Aymeric Girard,et al.  Processes and technologies for the recycling and recovery of spent lithium-ion batteries , 2016 .

[19]  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.

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

[21]  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.

[22]  Jiangrong Kong,et al.  Separation and recovery of metal values from leach liquor of waste lithium nickel cobalt manganese oxide based cathodes , 2015 .

[23]  Haegyeom Kim,et al.  Understanding the Degradation Mechanisms of LiNi0.5Co0.2Mn0.3O2 Cathode Material in Lithium Ion Batteries , 2014 .

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

[25]  Haochen Zhu,et al.  Leaching lithium from the anode electrode materials of spent lithium-ion batteries by hydrochloric acid (HCl). , 2016, Waste Management.

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

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

[28]  Guanghui Li,et al.  Leaching of limonitic laterite ore by acidic thiosulfate solution , 2011 .

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

[30]  Marion Joulié,et al.  Current collectors as reducing agent to dissolve active materials of positive electrodes from Li-ion battery wastes , 2017 .

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

[32]  G. P. Nayaka,et al.  Recovery of valuable metal ions from the spent lithium-ion battery using aqueous mixture of mild organic acids as alternative to mineral acids , 2015 .

[33]  Jian-Guo Yu,et al.  Leaching process for recovering valuable metals from the LiNi1/3Co1/3Mn1/3O2 cathode of lithium-ion batteries. , 2017, Waste management.

[34]  Linda F. Nazar,et al.  Positive Electrode Materials for Li-Ion and Li-Batteries† , 2010 .

[35]  Feng Wu,et al.  Recovery of valuable metals from spent lithium-ion batteries by ultrasonic-assisted leaching process , 2014 .

[36]  G. Santhosh,et al.  Dissolution of cathode active material of spent Li-ion batteries using tartaric acid and ascorbic acid mixture to recover Co , 2016 .

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

[38]  Liping Xu,et al.  Sustainable recovery of valuable metals from spent lithium-ion batteries using DL-malic acid: Leaching and kinetics aspect , 2017, Waste management & research : the journal of the International Solid Wastes and Public Cleansing Association, ISWA.

[39]  Wei Sheng Chen,et al.  Recovery Zinc and Manganese from Spent Battery Powder by Hydrometallurgical Route , 2017 .