Investigating Multiscale Spatial Distribution of Sulfur in a CNT Scaffold and Its Impact on Li–S Cell Performance

Yang, Guang; Tao, Runming; Jafta, Charl J.; Shen, Chao; Zhao, Sheng; He, Lilin; Belharouak, Ilias; Nanda, Jagjit

doi:10.1021/acs.jpcc.1c02288

Title: Investigating Multiscale Spatial Distribution of Sulfur in a CNT Scaffold and Its Impact on Li–S Cell Performance

Journal Article · Fri Jun 11 00:00:00 EDT 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c02288· OSTI ID:1820781

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Electrification and Energy Infrastructures Division
MaxPower Inc., Harleysville, PA (United States)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division

Ever increasing demand on high energy density batteries positions sulfur as a very promising cathode material for next-generation energy storage due to its high theoretical capacity of 1675 mAh/g. Electronically sulfur is highly insulating, and therefore integration of a conducting framework such as a carbon nanotube (CNT) scaffold with sulfur is a key aspect of the cathode design. Despite numerous efforts dedicated to S-CNT cathode development, increasing sulfur loading to above 1 mg/cm² while maintaining the cycling stability of the Li–S cell remains challenging. This could be partly due to the lack of understanding of the spatial distribution of sulfur in the CNT matrix and its location with respect to the morphology of the CNT scaffold. We demonstrate herein that the sulfur has a hierarchical distribution in the CNT cathode at high sulfur loading (>5 mg/cm²) spanning multiple length scales (from nanometer to submillimeter). Sulfur infiltration into the CNT rather than the sulfur loading plays a key role in determining the redox reaction kinetics, Li⁺ ion diffusion, and the galvanostatic cycling capacity and stability of Li–S cells. This study provides new insights for the design and fabrication of high loading, binder-free sulfur–carbon-based cathode architectures for next-generation high energy Li–S batteries.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1820781

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 24; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Investigating Multiscale Spatial Distribution of Sulfur in a CNT Scaffold and Its Impact on Li–S Cell Performance

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