The electrification of transportation and the transition of society towards low or net-zero carbon emissions has led to a skyrocketing global demand for Li-ion batteries. After a service life of three to ten years, Li-ion batteries have less than 80 % of their initial capacities and draw near to the end of their lives for practical utilization. Due to potential supply chain shortages and the value embodied in Li-ion batteries, it is imperative to recycle them, to recover the materials, and to improve the circularity and the sustinability of the industry. How to cost-effectively purify spent batteries while reducing time, energy, and waste emissions is a challenge faced by Li-ion battery recyclers. The first electrochemical membrane reactor reported in our group hasa high selectivity towards lower Cu2+, Al3+ and Fe3+ ions (<5 ppm) and retains > 95 % of the Ni2+, Co2+ and Mn2+ ions in the leachate. An advanced electrochemical membrane reactor was developed in this study. Not only does the new reactor have the same selectivity as the original reactor, but other advantages including a faster leachate processing rate (up to 10X faster). The advanced reactor can also directly generate acid at the anode side; eliminating the reactor restoration step. The prominent advantages that this electrodialysis technology has over chemical-precipitation methods include: (1) ion recovery efficiencies do not diminish after removing the impurities, Ni2+, Co2+ and Mn2+, even at a higher initial Ni2+ ion concentrations; in comparison, chemical precipitation has Ni2+, Co2+ and Mn2+ ion recovery efficiencies reduced significantly when the initial Ni2+, Co2+ and Mn2+ ion concentrations increase. (2) electrodialysis does not change the concentrations of Ni2+, Co2+ and Mn2+ ions significantly, but chemical precipitation could reduce Ni2+ and Co2+ ions to less than half of their initial values. Through electro-dialyzing the leachate, the H2 evolution reaction mechanism was found to switch from the Volmer-acid Heyrovsky mechanism to the Volmer-alkaline Heyrovsky mechanism at a pH of around 3.7.
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