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Potential regulation strategy enables ferrocene as p-type redox mediator for direct regeneration of spent LiFePO4 cathode

Mingli Xu,Chen Wu,Fengxue Zhang,Yanhui Zhang,Jiaxin Ren,Chengyi Zhang,Xuanze Wang,Li Xiao,Olivier Fontaine,Jiangfeng Qian

Conventional metallurgical technologies for recycling cathode materials from retired Li-ion batteries go against carbon neutrality owing to massive material input and energy consumption. Although featuring with simplified process, direct regeneration technology still fails to bypass high-temperature driving forces for Li + compensation of degraded cathodes. Herein, chemical re-lithiation strategy mediated by ferrocene is proposed to directly regenerate the Li-deficient spent cathodes. Ferrocene and its derivatives, the so-called p-type redox mediators, can be oxidized spontaneously from neutral molecules to stable cations under ambient conditions, allowing them to function as electron donors . Meanwhile, lithium salts serve as Li + donors to ensure charge neutrality of the cathode lattice. The effects of solvation and substituent are thoroughly investigated to precisely regulate the potential of a series of ferrocene-based reductants. Chemical re-lithiation is driven thermodynamically by the intrinsic potential gap between ferrocene and degraded cathodes, thus fundamentally realizing a rapid lithiation reaction (taking less than 20 min at 25 °C), while avoiding the involvement of high-temperature operation. Diverse characterizations have been performed to explore the Li + -electron concerted re-lithiation mechanism. The regenerated LiFePO 4 cathode demonstrated comparable Li + storage capability to commercial cathode. Life-cycle analysis verifies the economical and environmental superiority of our chemical re-lithiation strategy to metallurgy in practical industry. The thermodynamically spontaneous chemical re-lithiation provides competitive options for greener recycling of retired batteries in the future.