Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries

Zhao, Chen; Xu, Gui‐Liang; Zhao, Tianshou; Amine, Khalil

doi:10.1002/ange.202007159

Title: Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries

Journal Article · Wed Aug 12 00:00:00 EDT 2020 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202007159· OSTI ID:1647288

Zhao, Chen ^[1]; Xu, Gui‐Liang ^[2]; Zhao, Tianshou ^[3];

^[4]

Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong, Chemical Science and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
Chemical Science and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong
Chemical Science and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA, Materials Science and Engineering Stanford University Stanford CA 94305 USA, IRMC, Imam Abdulrahman Bin Faisal University (IAU) Dammam 34212 Saudi Arabia

Abstract Electrolyte modulation simultaneously suppresses polysulfide the shuttle effect and lithium dendrite formation of lithium–sulfur (Li‐S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been ignored, which dramatically limits the cycle life and energy density of practical Li‐S pouch cells. Herein, we demonstrate that a rational combination of selenium doping, core–shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Thus, high areal capacity (>4 mAh cm ⁻² ) with excellent cycle stability and Coulombic efficiency were both demonstrated in Li metal anode and thick S cathode (4.5 mg cm ⁻² ) with a low electrolyte/sulfur ratio (10 μL mg ⁻¹ ). This research further demonstrates a durable Li‐Se/S pouch cell with high specific capacity, validating the potential practical applications.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1647288

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 132 Journal Issue: 40; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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