The Weakened Super‐Exchange Interaction Realizes the Direct Regeneration of Spent Lithium‐lon Battery Cathodes
Abstract
Abstract The direct regeneration of cathodes is an effective technique to address resource waste and environmental pollution caused by spent lithium‐ion batteries (LIBs). However, Li + migration within the rock‐salt phase of degraded LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathodes follows an energetically unfavorable 2‐transition metal (2‐TM) transport pathway (tetrahedral sites between face‐sharing octahedra), creating a kinetic barrier that fundamentally limits direct regeneration. A Na‐based molten salt pretreatment is applied to introduce Na atoms into the unoccupied tetrahedral sites of the rock‐salt phase, which alters the electronic state distribution of bridged oxygen anions and reduces super‐exchange interactions between TM atoms in adjacent layers, thereby triggering a phase transformation from rock‐salt to targeted layered structure. Consequently, the Li + migration pathway shifts from a high‐energy 2‐TM route to a more favorable low‐barrier 1‐TM route, enabling efficient lithiation and complete restoration of the cathode. The regenerated materials exhibit high structural uniformity and excellent electrochemical performance, achieving 78% capacity retention after 500 cycles. This study provides an insightful perspective on direct LIB recycling by regulating super‐exchange interactions within the degraded cathode structures.
Article Details
Authors (15)
Yuan‐Meng Li
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Shaanxi,Xi'an 710049 P. R. China
Yujia He
Kai Jia
State Key Laboratory of Chemical Engineering and Low-Carbon Technology, Department of Chemical Engineering, Tsinghua University, Haidian District, Beijing 100084, China
Haojie Dong
Xin‐Yu Zhang
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China
Hao Qin
Key Laboratory of Seed Innovation, Institute of Genetics and Developmental Biology, Chinese Academy of Sciences
Ling‐Jiao Hu
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China
Hao Zhang
Zhao‐Kun Guan
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China
Si‐Fan Chen
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China
Mengting Liu
Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering
Bing Xiao
Department of Orthopaedics
Shujiang Ding
Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry
Kai Xi
Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, Department of Applied Chemistry, School of Chemistry
Peng‐Fei Wang
Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China