Direct regeneration of degraded lithium-ion battery cathodes with a multifunctional organic lithium salt

The recycling of spent lithium-ion batteries is an effective approach to alleviating environmental concerns and promoting resource conservation. LiFePO₄ batteries have been widely used in electric vehicles and energy storage stations. Currently, lithium loss, resulting in formation of Fe(III) phase, is mainly responsible for the capacity fade of LiFePO₄ cathode. Another factor is poor electrical conductivity that limits its rate capability. Here, we report the use of a multifunctional organic lithium salt (3,4-dihydroxybenzonitrile dilithium) to restore spent LiFePO₄ cathode by direct regeneration. The degraded LiFePO₄ particles are well coupled with the functional groups of the organic lithium salt, so that lithium fills vacancies and cyano groups create a reductive atmosphere to inhibit Fe(III) phase. At the same time, pyrolysis of the salt produces an amorphous conductive carbon layer that coats the LiFePO₄ particles, which improves Li-ion and electron transfer kinetics. The restored LiFePO₄ cathode shows good cycling stability and rate performance (a high capacity retention of 88% after 400 cycles at 5 C). This lithium salt can also be used to recover degraded transition metal oxide-based cathodes. A techno-economic analysis suggests that this strategy has higher environmental and economic benefits, compared with the traditional recycling methods.