High-Performance Lithium-Sulfur Batteries with Atomic V- and Co-Modified Ketjen Black-Sulfur Composite Cathode

Abstract

Lithium-sulfur (Li-S) batteries are potential alternatives to lithium-ion batteries, which are known to have certain drawbacks. This has drawn special technological attention. Sulfur’s low electrical conductivity, shuttling of the intermediate polysulfides, the slow conversion reaction kinetics of various lithium polysulfides (LiPS), and the major volume change of sulfur in the lithiation reaction are some of the main issues that still need to be resolved before Li-S batteries can be used in practical applications. Additionally, it is likely because there are not enough prognostic models determining energy densities at the cell and pack level based on materials and cell design, most of the articles do not report system-level metrics, specific energy (Wh kg-1), and energy density (Wh L-1).To overcome these problems, atomic vanadium (V) and cobalt (Co) modified ketjen black-sulfur composite (VCKBS) was prepared and used as a cathode in Li-S batteries. The synthesized composite was characterized by various techniques, e.g., XRD, Raman, SEM, HR-TEM, HAADF-STEM, and XPS spectra. The polysulfide adsorption test showed that V had increased the adsorption ability, and cyclic voltammetry displayed the increased catalytic activity resulting from Co, offering a large number of interfacial active sites and ensuring smooth electron transfer. Cycling performance tests showed an initial specific capacity of 1329 mAh g−1, maintained at 1249 mAh g−1 after 100 cycles. Under a higher sulfur loading (2.4 mg cm−2), at 0.2 C, Li-S cells demonstrated an initial specific capacity of 1201 mAh g−1 and retained 985 mAh g−1 after 300 cycles with a low fading rate of 0.059% per cycle. The rate performance tests showed that the prior capacity is nearly recovered, going from 1C back to 0.1C, demonstrating the superiority of the VCKBS material.In addition to the experimental characterization of the Li-S cell performance, energy densities were also predicted by a proposed system-level performance model. The 1st and 100th discharge capacities were used to forecast the system-level specific energies and energy densities. The system-level specific energies and energy densities based on the 100th discharge capacity of VCKBS cathodes had improvements of 1342 and 568%, respectively. This suggests that an easy route to construct the highly stable cathode material may pave the way for the development of highly efficient Li-S batteries. Acknowledgments Hira Fazal acknowledges support from the Türkiye Scholarship/Research Fellowship Program sponsored by the Prime Ministry of Turkey Presidency for Turks Abroad and Related Communities (21PK070917). Damla Eroglu acknowledges support from the Istanbul Development Agency (Award No: TR10/21/YEP/0001). We also thank the National Natural Science Foundation of China (22171180) and the Science and Technology Commission of Shanghai Municipality (20520710400).