Thermal treatment and ammoniacal leaching for the recovery of valuable metals from spent lithium-ion batteries

被引:168
作者
Chen, Yongming [1 ]
Liu, Nannan [1 ]
Hu, Fang [2 ]
Ye, Longgang [3 ]
Xi, Yan [1 ]
Yang, Shenghai [1 ]
机构
[1] Cent S Univ, Sch Met & Environm, Changsha 410083, Hunan, Peoples R China
[2] Cent S Univ, Coll Chem & Chem Engn, Changsha 410083, Hunan, Peoples R China
[3] Hunan Univ Technol, Sch Met & Mat Engn, Zhuzhou 412007, Peoples R China
关键词
Spent Li-ion batteries; Cathode active powder; Thermal treatment; Ammoniacal leaching; Double salts; CATHODIC ACTIVE MATERIALS; COBALT; ACID; TECHNOLOGIES; PRETREATMENT; EXTRACTION; SEPARATION; SULFITE; NICKEL; WASTES;
D O I
10.1016/j.wasman.2018.02.024
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The recycling of spent commercial lithium-ion batteries (LIBs) generates numerous environmental and economic benefits. In this research, a thermal treatment-ammoniacal leaching process is proposed to recover valuable metals from cathode active powder. Based on the thermal behavior by TG-DSC analysis, the cathode active powder is calcined at 300 degrees C and 550 degrees C in air atmosphere, and the crystalline phase characterization indicates that a new phase of Co3O4 appears in the cathode active powder calcined at 550 degrees C, which signifies that the layer structure of LiCoO2 collapses. The valence of manganese increases to form Li4Mn3O12 in spinel structure of LiMn2O4. Using calcined cathode powder as feed material, ammoniacal leaching is carried out in (NH4)(2)SO4-(NH4)(2)SO3 solution. Under the optimum conditions, Ni, Co, Mn and Li can be completely leached out with efficiencies of 98%, 81%, 92% and 98%, respectively. However, with the increase of ammonia concentration, the leaching efficiency of Mn decreases dramatically to 4% due to the formation of double salts. It is found that Co and Mn can be precipitated into residues in the form of (NH4)(2)Co(SO4)2 center dot H2O, (NH4)(2)Mn(SO3)(2)center dot H2O and (NH4)(2)Mn(SO4)(2)center dot 6H(2)O under different leaching parameters. Based on the corresponding relationship between the leaching efficiency and phase evolution of object element, selective leaching can be achieved by controlling the formation of double salts. (C) 2018 Elsevier Ltd. All rights reserved.
引用
收藏
页码:469 / 476
页数:8
相关论文
共 30 条
[1]   Leaching and separation of Co and Mn from electrode materials of spent lithium-ion batteries using hydrochloric acid: Laboratory and pilot scale study [J].
Barik, S. P. ;
Prabaharan, G. ;
Kumar, L. .
JOURNAL OF CLEANER PRODUCTION, 2017, 147 :37-43
[2]   A brief review on hydrometallurgical technologies for recycling spent lithium-ion batteries [J].
Chagnes, Alexandre ;
Pospiech, Beata .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2013, 88 (07) :1191-1199
[3]   Enhanced recycling network for spent e-bicycle batteries: A case study in Xuzhou, China [J].
Chen, Fu ;
Yang, Baodan ;
Zhang, Wangyuan ;
Ma, Jing ;
Lv, Jie ;
Yang, Yongjun .
WASTE MANAGEMENT, 2017, 60 :660-665
[4]   Effect of synthesis condition on the structural and electrochemical properties of Li[Ni1/3Mn1/3Co1/3]O2 prepared by carbonate co-precipitation method [J].
Cho, TH ;
Park, SM ;
Yoshio, M ;
Hirai, T ;
Hideshima, Y .
JOURNAL OF POWER SOURCES, 2005, 142 (1-2) :306-312
[5]   A laboratory-scale lithium-ion battery recycling process [J].
Contestabile, M ;
Panero, S ;
Scrosati, B .
JOURNAL OF POWER SOURCES, 2001, 92 (1-2) :65-69
[6]   Electrochemical recycling of cobalt from cathodes of spent lithium-ion batteries [J].
Freitas, M. B. J. G. ;
Garcia, E. M. .
JOURNAL OF POWER SOURCES, 2007, 171 (02) :953-959
[7]   Electrodeposition of cobalt from spent Li-ion battery cathodes by the electrochemistry quartz crystal microbalance technique [J].
Garcia, E. M. ;
Santos, J. S. ;
Pereira, E. C. ;
Freitas, M. B. J. G. .
JOURNAL OF POWER SOURCES, 2008, 185 (01) :549-553
[8]   Recovery of lithium and cobalt from spent lithium-ion batteries using organic acids: Process optimization and kinetic aspects [J].
Golmohammadzadeh, Rabeeh ;
Rashchi, Fereshteh ;
Vahidi, Ehsan .
WASTE MANAGEMENT, 2017, 64 :244-254
[9]   Simultaneous recycling of nickel metal hydride, lithium ion and primary lithium batteries: Accomplishment of European Guidelines by optimizing mechanical pre-treatment and solvent extraction operations [J].
Granata, G. ;
Pagnanelli, F. ;
Moscardini, E. ;
Takacova, Z. ;
Havlik, T. ;
Toro, L. .
JOURNAL OF POWER SOURCES, 2012, 212 :205-211
[10]   Recycling of lithium-ion batteries: a novel method to separate coating and foil of electrodes [J].
Hanisch, Christian ;
Loellhoeffel, Thomas ;
Diekmann, Jan ;
Markley, Kely Jo ;
Haselrieder, Wolfgang ;
Kwade, Arno .
JOURNAL OF CLEANER PRODUCTION, 2015, 108 :301-311