Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries

Zhou, Guangmin; Zhao, Shiyong; Wang, Tianshuai; Yang, Shi-Ze; Johannessen, Bernt; Chen, Hao; Liu, Chenwei; Ye, Yusheng; Wu, Yecun; Peng, Yucan; Liu, Chang; Jiang, San Ping; Zhang, Qianfan; Cui, Yi

doi:10.1021/acs.nanolett.9b04719

Title: Theoretical Calculation Guided Design of Single-Atom Catalysts toward Fast Kinetic and Long-Life Li–S Batteries

Journal Article · Mon Dec 30 00:00:00 EST 2019 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.9b04719· OSTI ID:1617143

^[1]; Zhao, Shiyong ^[2]; Wang, Tianshuai ^[3];

^[4]; Johannessen, Bernt ^[5];

^[6]; Liu, Chenwei ^[6];

^[6];

^[6]; Peng, Yucan ^[6]; Liu, Chang ^[7];

^[2];

^[3];

^[8]

Stanford Univ., CA (United States); Tsinghua Univ., Beijing (China)
Curtin Univ., Perth, WA (Australia)
Beihang Univ., Beijing (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Australian Nuclear Science and Technology Organisation (ANSTO), Melbourne, VIC (Australia). Australian Synchrotron
Stanford Univ., CA (United States)
Chinese Academy of Sciences, Shenyang (China)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Lithium–sulfur (Li–S) batteries are enticing next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. Yet, 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 offers solutions for the development of high energy/power density Li–S batteries.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); Beijing Natural Science Foundation

Grant/Contract Number:: AC02-76SF00515; NCET-12-0033; DP150102044; DP180100568; DP180100731; 11404017; 51872293

OSTI ID:: 1617143

Journal Information:: Nano Letters, Vol. 20, Issue 2; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 265 works

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