Revealing the delithiation process of spent LiMn2O4 and LiNi0.6Co0.2Mn0.2O2 batteries during the biomass-assisted gasthermal and carbothermal reduction

Abstract

The utilization of biomass-assisted pyrolysis in the recycling of spent lithium-ion batteries has emerged as a promising and reliable process. This article furnishes theoretical underpinnings and analytical insights into this method, showcasing sawdust pyrolysis reduction as an efficient means to recycle spent LiMn2O4 and LiNi0.6Co0.2Mn0.2O2 batteries. Through advanced thermogravimetry-gas chromatography-mass spectrometry analysis complemented by traditional thermodynamic demonstration, the synergistic effects of biomass pyrolysis reduction are elucidated, with minor autodecomposition and major carbothermal and gasthermal reduction pathways identified. The controlled manipulation of transition metals has demonstrated the capability to modulate surface pyrolysis gas catalytic reactions and facilitate the preparation of composite materials with diverse morphologies. Optimization of process conditions has culminated in recovery efficiency exceeding 99.0 % for LiMn2O4 and 99.5 % for LiNi0.6Co0.2Mn0.2O2. Economic and environmental analyses underscore the advantages of biomass reduction and recycling for these two types of spent LIBs: low energy consumption, environmental compatibility, and high economic viability.