![]() Li containing flux media (eutectic molten salts or ionic liquids) can serve as both Li sources and solvents to restore Li in spent NMC under relatively low temperatures (below 300☌), because the highly charged flux media favor for transporting ionic reactants ( Li et al., 2016 Yuan et al., 2018 Parnham and Morris, 2007). Because the irreversible structure change in spent NMC is mainly caused by irreversible Li loss, the relithiation process is critical and has been achieved in some direct recycling works by flux methods ( Wang et al., 2020 Shi et al., 2019). Here, targeting the direct upcycling of spent NMC 111 to Ni-rich NMC cathodes, we developed a “reciprocal ternary molten salts” (RTMS) system to simultaneously realize the addition of Ni and relithiation in spent NMC 111, where RTMS are those molten salts containing two cation species and two anion species. Thus, beyond direct recycling, direct upcycling of spent cathodes to the next-generation cathodes is critical to maximize the value of spent materials. The direct recycling of spent cathodes to their pristine states easily falls behind the fast development of cathode materials, because recycling of EOL LIBs generally happens years later after production ( Beaudet et al., 2020 2018b). NMC 622, NMC 811) for replacing present NMC 111 in the near future ( Noh et al., 2013 Yoon et al., 2015 Kim et al., 2020). The next-generation cathodes of automotive LIBs were predicted as Ni-rich and Co-lean cathodes (e.g. Nowadays, LiNi 1/3Mn 1/3Co 1/3O 2 (NMC 111) with a lower content of Co takes the baton from LiCoO 2 to achieve balanced cost, capacity, and stability for commercial automotive LIBs ( Ding et al., 2019). Goodenough in 1980s, was widely used in portable devices ( Mizushima et al., 1980 Lyu et al., 2021). For example, LiCoO 2, proposed as the cathode materials by Prof. As the main force of cathode materials, NMC cathodes keep changing their chemical compositions to pursue lower cost, higher capacity, and cycling stability ( Manthiram, 2020 2018b). To overcome the drawbacks of pyrometallurgical and hydrometallurgical recycling process, direct recycling stands out as an emerging technology to retrain the added value of compound structure by healing the compositional and structural defects in spent cathode materials, or using the spent graphite anodes for other energy storage devices, such as Na/K-ion batteries ( Yang et al., 2020 Xu et al., 2020 Li et al., 2020 Larouche et al., 2020 Sloop et al., 2018 Fan et al., 2021 Liang et al., 2019 Divya et al., 2020 Meng et al., 2022). Moreover, the resynthesis of cathode compounds from metals requires energy-intensive processes, which incur extra costs and greenhouse gas emissions ( Ciez and Whitacre, 2019). Though the recovered metals can serve as raw materials in supply chains, the destruction of cathode materials consumes significant energy and results in the loss of compound structure added value ( Zhang et al., 2018a Li et al., 2018a Gao et al., 2017). Most of current facilities and processes to recover EOL LIBs are to recover valuable metals, especially cobalt by pyrometallurgical and hydrometallurgical recycling methods ( Ciez and Whitacre, 2019 Mansur et al., 2021 Atia et al., 2019 Velázquez-Martínez et al., 2019). Recovering materials especially high-value cathodes from EOL LIBs not only relieves the pressure on the raw material supply chain but also minimizes environmental pollution of EOL LIBs ( Mossali et al., 2020 Chen et al., 2019 Du et al., 2021). Along with the scaled production of LIBs, end-of-life (EOL) LIBs are causing serious environmental contaminations due to their hazardous components, such as toxic lithium compounds, heavy metals, and electrolytes ( Wang et al., 2020 Duarte Castro et al., 2021 Bai et al., 2020). To meet this high demand, minerals containing lithium, cobalt, manganese, and nickel are massively needed and becoming a bottle neck in scale-up production of commercial lithium nickel manganese cobalt oxide (LiNi xMn 圜o zO 2, x + y + z = 1) cathodes, resulting in constantly increasing costs from raw materials ( Robinson, 2020 Olivetti et al., 2017). The cumulative lithium-ion battery demand has soared from 0.5 GW-hours (GWh) in 2010 to 526 GWh in 2020, and been predicted to 9300 GWh in 2030 ( Statista, 2020). Lithium-ion batteries (LIBs) are widely used in portable devices and electrical vehicles because of their high energy density, which has changed people’s lifestyle in last decades ( Manthiram, 2017, 2020 Yoshino, 2012).
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