Electrothermal Coupling Enables Defect‐Targeted Topological Repair for Rapid Graphite Upcycling
Abstract
ABSTRACT Spent graphite (SG) from end‐of‐life lithium‐ion batteries suffers from persistent structural disorder, yet the defect chemistry governing its regeneration remains poorly understood. Here, we identify carbon vacancies and quasi‐sp 3 topological defects as the dominant degradation motifs and leverage this insight to devise a defect‐targeted regeneration strategy. Under electrothermal coupling enabled by flash Joule heating in a CoCl 2 molten‐salt medium, cobalt species are selectively directed to defect sites, where strong Co‐defect interactions reduce the energy barrier for topological reconstruction. The resulting Co‐induced charge redistribution activates quasi‐sp 3 ‐carbon via population of π * antibonding states, while thermally assisted and field‐directed carbon migration promotes its conversion into a more ordered sp 2 ‐rich lattice. Concurrently, residual interphases and impurities are eliminated, lattice stress is relieved, and the cobalt catalyst is efficiently recovered. The regenerated graphite (RG) delivers a capacity of 257 mAh g −1 after 1000 cycles at 1 A g −1 , corresponding to 83% retention relative to the post‐activation capacity, and outperforms commercial graphite under identical conditions. This work establishes a chemically informed route for the rapid upcycling of SG through defect‐selective topological repair.
Article Details
Authors (15)
Shen Wang
Na Li
Yangyang Liu
State Key Laboratory for Mechanical Behavior of Materials, School of Instrument Science and Technology
ZhiJie Zhang
Sen Dang
School of Chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education National Innovation Platform (Center) for Industry‐Education Integration of Energy Storage Technology State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Material and Chemistry Universities of Shaanxi Province Xi'an Jiaotong University Xi'an China
Hongyang Zhao
Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry
Bo Wen
School of Physics and Electronics
Xiaolong Lv
Limin Liu
National Synchrotron Radiation Laboratory
Chenzhaosha Li
School of Chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education National Innovation Platform (Center) For Industry‐Education Integration of Energy Storage Technology State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Material and Chemistry Universities of Shaanxi Province Xi'an Jiaotong University Xi'an China
Lanya Zhao
School of Chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education National Innovation Platform (Center) for Industry‐Education Integration of Energy Storage Technology State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Material and Chemistry Universities of Shaanxi Province Xi'an Jiaotong University Xi'an China
Hu Wu
Kai Xi
Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, Department of Applied Chemistry, School of Chemistry
Shujiang Ding
Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, School of Chemistry
Guorui Yang
School of Chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education National Innovation Platform (Center) for Industry‐Education Integration of Energy Storage Technology State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Material and Chemistry Universities of Shaanxi Province Xi'an Jiaotong University Xi'an China