Theoretical calculation guided design of single-atom catalysts toward fast kinetic and long-life Li–S batteries
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American Chemical Society
Abstract
Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge-charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g-1 at 3 C rate), and long-life Li-S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and provides solutions for the development of high energy/power density Li-S batteries. © 2019 American Chemical Society.
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Y.C. acknowledges the support from the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy, under the Battery Materials Research program and the Battery 500 Consortium program. G.Z. was supported by the Natural Key Research and Development Program of China (Number 2019YFA0705703). Q.Z. was supported by the National Natural Science Foundation of China (11404017), Beijing Natural Science Foundation (No. 2192029), the Technology Foundation for Selected Overseas Chinese Scholar, the Ministry of Human Resources and Social Security of China, and the program for New Century Excellent Talents in University (NCET-12-0033). S.Z. and S.J. acknowledge the support from the Australian Research Council under Discovery Project Scheme (Project Numbers DP150102044, DP180100731, and DP180100568). C.L. is thankful for the support from the National Natural Science Foundation of China (No. 51872293). The NEXAFS and XAS measurements were performed on the soft X-ray and XAS beamlines, respectively, of the Australian Synchrotron, Victoria, Australia, part of ANSTO. The electron microscopy done at Oak Ridge National Laboratory (S.Z.Y.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and performed in part as a user proposal at the ORNL Center for Nanophase Materials Sciences, which is a DOE Office of the Science User Facilities.
Citation
Zhou, G., Zhao, S., Wang, T., Yang, S.-Z., Johannessen, B., Chen, H., Liu, C., Ye, Y., Wu, Y., Peng, Y., Liu, C., Jiang, S. P., Zhang, Q., & Cui, Y. (2020). Theoretical calculation guided design of single-atom catalysts toward fast kinetic and long-life Li–S batteries. Nano Letters, 20(2), 1252-1261. doi:10.1021/acs.nanolett.9b04719