Biotreatment for the spent lithium-ion battery in a three-module integrated microbial-fuel-cell recycling system
Graphical abstract
Introduction
In recent decades, LIBs have been widely used in many fields, such as mobile electronics, aerospace, and medical care, etc., due to its some instinct advantages including high energy density, large working voltage, long cycle life, and minor memory effect(Chen et al., 2019, Huang et al., 2019a, Sattar et al., 2019, Zhang et al., 2019). The vigorous development of the new-energy vehicles has expanded the demanding production of LIBs and further irritated the increases in the price of raw materials (Guo et al., 2018, Yang et al., 2018). Commonly, LIBs would suffer the inactivation process after about 3 to 5 years. LIBs scrapped from the commercial vehicles and passenger cars will reach 84 GWh and 17.5 GWh, respectively, with around 1.16 million tons in total in 2023(Ku et al., 2016, Zeng et al., 2015, Zhang et al., 2014). Co and Li coming from the mineral resources of raw materials have been rapidly consumed in many countries, especially in China. The relative shortage in the resources and the imbalance between the supply and demand have restricted the healthy development of the power industry (Huang et al., 2019c, Zhang et al., 2018a). In this perspective, recycling Co and Li from the spent LIBs not only solves the potential environmental problems also eases the constraining status caused by the shortage of regeneration resources (Boxall et al., 2018, Dutta et al., 2018, Nascimento et al., 2018, Omelchuk and Chagnes, 2018).
The pretreatment and the chemical recycling for the spent LIBs have been systemically developed until now (Meng et al., 2017, Meng et al., 2018a, Meng et al., 2018b, Meng et al., 2018c). Some traditional pyrometallurgy and hydrometallurgy techniques, such as (bio)leaching, adsorption, ion exchange, chemical precipitation, and solvent extraction, etc. have been applied to the recycling of LIBs(Chagnes and Pospiech, 2013, Gratz et al., 2014, Horeh et al., 2016, Jha et al., 2013, Joulie et al., 2014, Pospiech, 2014, Swain, 2017, Zhang et al., 2018b). However, some drawbacks including high energy consumption, strong reliance on the chemical reagents, and cumbersome route have explicitly hindered the application of these methods (Golmohammadzadeh et al., 2018, Swain, 2017, Yao et al., 2018). Microbial electrolysis cells (MECs) have been proposed as a promising and innovative technology for the recovery of Co and Li from the spent LIBs in overcoming the conventional bottlenecks (Jadhav et al., 2017, Yu et al., 2018). MEC can reduce Co from cathodes, separate Co and Li, and simplify the recovery of Li in the downstream process. However, the consumption of precious metal catalysts and the additional voltage needed to compensate the thermodynamic cap potentially limit the application of MECs in the scale and scope (Hasany et al., 2016, Kadier et al., 2016, Kadier et al., 2014). Correspondingly, the biocathode and self-driven MFCs have been proposed as some improved steps to reduce the cost of some noble catalysts, to lower the overpotentials of MEC systems, and to increase the collateral electricity output without external voltage(Huang et al., 2014a, Huang et al., 2014b, Shen et al., 2015, Wu et al., 2015). However, these researches were dwarfed by the obvious decreases in the removal and recovery rates of Co and Li (Huang et al., 2019c).
In this study, a complete bio-electrochemical (BE) recycling platform was constructed to achieve the recovery of Li and Co from the cathodic material of the spent LIBs. The BE platform consisted of three indispensable and sequential subsystems, MFC-A, MFC-B, and MFC-C. To achieve the maximum recoveries of Li and Co from the cathodic materials, the running performance of each subsystem was consorted and improved based on the adjustment of parameters. The effects of the initial pH in the catholyte and the loading ratios of LiCoO2 attached to the carbon brush in the MFC-A system were fully studied. The combination of parameters in the MFC-B system was quantitatively optimized to maximize the removal and recovery of Co-based on the analysis results of the individual and synergetic influences of four variables towards the responses in the central composite design (CCD). The effects of the dosing concentrations of Li+ and the concentrations of (NH4)2CO3 on the recovery of Li and power generation were comprehensively investigated in the MFC-C system. To better integrate the three subsystems and expand the application scale of the BE platform, the reaction mechanisms of each subsystem were discussed in depth by overviewing the experimental results of indicators and analyzing the morphological and spectra results. The research not only provides a novel method in guiding the step recovery of Co and Li from the cathodic material of spent LIBs in a compacted BE platform and supplies the feasibility of green recycling for the solid waste based on ensuring high recovery rates.
Section snippets
Preparation of LiCoO2 and modified granular activated carbons
The spent LIB was collected from some recycling boxes installed in the college. The cylindrical spent LIBs were discharged by connecting the wires and electrolytes before a dismantling and separating procedure (Huang et al., 2019a, Huang et al., 2019c). The active materials of cathode foils were separated, ground, and immersed in N-methyl-2-pyrrolidone, sequentially. LiCoO2 was further shredded from the aluminum foils by ultrasonic washing at 40 kHz and 160 W over 15 min. LiCoO2 powders were
Electroactive acclimation in the three MFC subsystems
The running performance of the BE recycling system during the acclimation of inoculum is shown in Fig. 2. The successful acclimation of inoculation is the keynote in setting up the BE system (Vicari et al., 2018). Before optimizing the three MFC subsystems, the successive startup should be guaranteed. Considering the direct counting for the anaerobic bacterial consortia was impractical, some strategies including anode potentials, polarization curves, the maximum power densities, and internal
Conclusions
Co and Li can be effectively separated and recovered from the cathodic materials of spent LIBs by the BE recycling system assembled from three subsystems. Lower initial pH and smaller loading ratios of LiCoO2 were favorably chosen in MFC-A. The initial pH of 1 and the loading ratios of LiCoO2 of 200 – 500 mg/L were demonstratively recommended in strengthening the leaching rates of Li and Co and guaranteeing the high electricity production in MFC-A. The thickness of 0.15 cm was quantitively
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgments
This work was financially supported by the Natural Science Foundation of Jiangsu Province (BK20201054), the China Postdoctoral Science Foundation (2020M681774) and the Natural Science Foundation of the Jiangsu Higher Education institutions of China (20KJB490001).
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