Spent Lithium-Ion Batteries Recycling: Comparison
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An urgent demand for recycling spent lithium-ion batteries (LIBs) is expected in the forthcoming years due to the rapid growth of electrical vehicles (EV). To address these issues, various technologies such as the pyrometallurgical and hydrometallurgical method, as well as the newly developed in-situ roasting reduction (in-situ RR) method were proposed in recent studies.

  • Spent lithium-ion batteries
  • Recycling
  • Pyrometallurgical method
  • Hydrometallurgical method
  • Utilization

1. Background for rRecycling sSpent LIBs

    Lithium-ion batteries (LIB) have been commercially used from 1990s. Owing to its excellent properties of high energy density, low self-discharge rate, long storage life, and safe handling, LIBs are found in all aspects of our lives, from small portable electronic devices through electric vehicles to energy storage systems [1]. According to statistics from the White Paper on the Development of China's Lithium-ion Battery Industry (2021), the worldwide LIB production has been increased to 294.5 GWh (over 1.6 million tons) in 2020 with a growth rate of 35.8% [2]. However, the capacity of LIBs substantially decays after 800-1500 charging and discharging cycles due to the destruction of electrode structure, the damage of separator, and the volatilization of electrolyte [3][4], leading to the generation of a huge amount of spent LIBs every year.

2. Necessity of rRecycling sSpent LIBs

    A typical LIB are usually composed of shells, current collectors, active materials, organic electrolyte, separators [5]. The main anode materials of LIB are always graphite while the main components of cathode are diverged, mainly LiCoO2, LiMn2O4, LiFePO4, as well as other lithium metal oxides. In addition, LIBs also contain a certain amount of Polyvinylidene Fluoride (PVDF), LiPF6, C3H4O3, C4H6O3 and other components [6]. Therefore, improper disposal of spent LIBs can cause serious release of toxins such as heavy metals and fluorine-containing organic chemicals, posing potential risks to the environment and human health [7]. On the other hand, valuable metals (e.g. Ni, Co, Li) containing in spent LIBs are at very high levels [3], even higher than those in natural ores. It is reported that China had produced 2.5 billion of spent LIBs with a mass of about 5.0×105 t in 2020 [8]. Therefore, it is of great value to recycle the major components from spent LIBs to prevent environmental pollution and to save natural resources of valuable metals. Recently, many countries have established laws and policies to encourage the development of recycling spent LIBs [9]. In 2019, the U.S. Department of Energy launched the Argonne National Laboratory Battery Recycling Research and Development Center and the Lithium ion Battery Recycling Award program. The German government requires battery manufacturers to register the primary responsibility for recycling the LIBs. For China, Development Plan for Energy Saving and New Energy Automobile Industry (2012-2020) issued by the government clearly mentioned that it is necessary to strengthen the cascade utilization and recycling management of batteries and to guide power battery manufacturers to strengthen the recycling and utilization of spent batteries.

3. Methods for rRecycling sSpent LIBs

    There are three major approaches to recycle the spent LIBs: pyrometallurgy, hydrometallurgy, and direct recycling method [10][11][12]. Pyrometallurgy is an established technology that usually smelting spent LIBs with other types of batteries or ores and industrial wastes at a temperature above 1450 °C to produce mixed metal alloys of Co, Cu, Fe and Ni. Usually, pyrometallurgy does not require pre-sorting of the spent LIBs, but the alloy obtained is needed to be separated for further utilization. Umicore, Inmetco, Accurec, etc are the representative companies using this technology for spent LIB recycling [13]. For hydrometallurgical method, metals in cathode materials are leached by acid. The significant advantage of this method recycling of spent LIB is the high metal recovery rate. The representative companies such as GEM High-Tech, Brunp, Retriev Inc. (previously, Toxco), and Recupyl, are engaged in the hydrometallurgical method [14][15]. As for the direct recycling method, the anode or cathode materials of spent LIBs are refurbished directly, then the products are reused as the electrode materials of the new LIBs. This method is still under development and the representiative company is Ganfeng Lithium (China). In addition to the above methods, there are also novel technologies under investigation such as plasma smelting, bioleaching, in situ roasting, redox targeting based material recycling, etc [16]. In all, different methods for LIB recycling have their own cons. For example, the pyrometallurgical method suffers from high energy consumption and greenhouse gas emission, while the commonly used hydrometallurgical approach produces large amounts of acidic or alkaline wastewater. Therefore, development of the recycling method for spent lithium batteries is a hot topic worthy of investigation.

References

  1. Zhang, T.; He, Y.; Ge, L.; Fu, R.; Zhang, X.; Huang, Y; Characteristics of wet and dry crushing methods in the recycling process of spent lithium-ion batteries. J. Power Sources 2013, 240, 766–771.
  2. White Paper on the Development of China's Lithium-ion Battery Industry (2021) . Https://baijiahao.baidu.com/s?id=1690837068997058666&wfr=spider&for=pc. Retrieved 2021-10-28
  3. Fabian Diaz; Yufengnan Wang; Reiner Weyhe; Bernd Friedrich; Gas generation measurement and evaluation during mechanical processing and thermal treatment of spent Li-ion batteries. Waste Management 2018, 84, 102-111, 10.1016/j.wasman.2018.11.029.
  4. Jun Li; Yiming Lai; Xianqing Zhu; Qiang Liao; Ao Xia; Yun Huang; Xun Zhu; Pyrolysis kinetics and reaction mechanism of the electrode materials during the spent LiCoO2 batteries recovery process. Journal of Hazardous Materials 2020, 398, 122955, 10.1016/j.jhazmat.2020.122955.
  5. Jiefeng Xiao; Jia Li; Zhengming Xu; Recycling metals from lithium ion battery by mechanical separation and vacuum metallurgy. Journal of Hazardous Materials 2017, 338, 124-131, 10.1016/j.jhazmat.2017.05.024.
  6. Diaz, F.; Wang, Y.; Moorthy, T.; Friedrich, B; Degradation mechanism of nickel-cobalt-aluminum (NCA) cathode material from spent lithium-ion batteries in microwave-assisted pyrolysis. Metals. Metals (Basel) 2018, 8, 565, doi:10.3390/met8080565.
  7. Guangwen Zhang; Yaqun He; Yi Feng; Haifeng Wang; Xiangnan Zhu; Pyrolysis-Ultrasonic-Assisted Flotation Technology for Recovering Graphite and LiCoO2 from Spent Lithium-Ion Batteries. ACS Sustainable Chemistry & Engineering 2018, 6, 10896-10904, 10.1021/acssuschemeng.8b02186.
  8. Chunwei Liu; Jiao Lin; HongBin Cao; Yi Zhang; Zhi Sun; Recycling of spent lithium-ion batteries in view of lithium recovery: A critical review. Journal of Cleaner Production 2019, 228, 801-813, 10.1016/j.jclepro.2019.04.304.
  9. Weiguang Lv; Zhonghang Wang; HongBin Cao; Yong Sun; Yi Zhang; Zhi H.I. Sun; A Critical Review and Analysis on the Recycling of Spent Lithium-Ion Batteries. ACS Sustainable Chemistry & Engineering 2018, 6, 1504-1521, 10.1021/acssuschemeng.7b03811.
  10. Dahui Wang; Hao Wen; Huaijing Chen; Yujiao Yang; Hongyan Liang; Chemical evolution of LiCoO2 and NaHSO4·H2O mixtures with different mixing ratios during roasting process. Chemical Research in Chinese Universities 2016, 32, 674-677, 10.1007/s40242-016-5490-2.
  11. Jiakai Mao; Jia Li; Zhengming Xu; Coupling reactions and collapsing model in the roasting process of recycling metals from LiCoO2 batteries. Journal of Cleaner Production 2018, 205, 923-929, 10.1016/j.jclepro.2018.09.098.
  12. Pratima Meshram; B.D. Pandey; T.R. Mankhand; Hydrometallurgical processing of spent lithium ion batteries (LIBs) in the presence of a reducing agent with emphasis on kinetics of leaching. Chemical Engineering Journal 2015, 281, 418-427, 10.1016/j.cej.2015.06.071.
  13. Brian Makuza; Qinghua Tian; Xueyi Guo; Kinnor Chattopadhyay; Dawei Yu; Pyrometallurgical options for recycling spent lithium-ion batteries: A comprehensive review. Journal of Power Sources 2021, 491, 229622, 10.1016/j.jpowsour.2021.229622.
  14. Jung, J.C.Y.; Sui, P.C.; Zhang, J; A review of recycling spent lithium-ion battery cathode materials using hydrometallurgical treatments. J. Energy Storage 2021, 35, 102217, 10.1016/j.est.2020.102217..
  15. Yanyan Zhao; Oliver Pohl; Anand Bhatt; Gavin Collis; Peter Mahon; Thomas Rüther; Anthony Hollenkamp; A Review on Battery Market Trends, Second-Life Reuse, and Recycling. Sustainable Chemistry 2021, 2, 167-205, 10.3390/suschem2010011.
  16. Fangfang Wang; Tao Zhang; Yaqun He; Yuemin Zhao; Shuai Wang; Guangwen Zhang; Yu Zhang; Yi Feng; Recovery of valuable materials from spent lithium-ion batteries by mechanical separation and thermal treatment. Journal of Cleaner Production 2018, 185, 646-652, 10.1016/j.jclepro.2018.03.069.
  17. Fangfang Wang; Tao Zhang; Yaqun He; Yuemin Zhao; Shuai Wang; Guangwen Zhang; Yu Zhang; Yi Feng; Recovery of valuable materials from spent lithium-ion batteries by mechanical separation and thermal treatment. Journal of Cleaner Production 2018, 185, 646-652, 10.1016/j.jclepro.2018.03.069.
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