Enhancing Electron Conductivity and Electron Density of Single Atom Based Core–Shell Nanoboxes for High Redox Activity in Lithium Sulfur Batteries

Herein, an integrated structure of single Fe atom doped core-shell carbon nanoboxes wrapped by self-growing carbon nanotubes (CNTs) is designed. Within the nanoboxes, the single Fe atom doped hollow cores are bonded to the shells via the carbon needles, which act as the highways for the electron transport between cores and shells. Moreover, the single Fe atom doped nanobox shells is further wrapped and connected by self-growing carbon nanotubes. Simultaneously, the needles and carbon nanotubes act as the highways for electron transport, which can improve the overall electron conductivity and electron density within the nanoboxes. Finite element analysis verifies the unique structure including both internal and external connections realize the integration of active sites in nano scale, and results in significant increase in electron transfer and the catalytic performance of Fe-N₄ sites in both Li₂ S_n lithiation and Li₂ S delithiation. The Li-S batteries with the double-shelled single atom catalyst delivered the specific capacity of 702.2 mAh g^-1 after 550 cycles at 1.0 C. The regional structure design and evaluation method provide a new strategy for the further development of single atom catalysts for more electrochemical processes.