Pushing Lithium–Sulfur Batteries towards Practical Working Conditions through a Cathode–Electrolyte Synergy

Zhao, Chen; Daali, Amine; Hwang, Inhui; Li, Tianyi; Huang, Xingkang; Robertson, David; Yang, Zhenzhen; Trask, Steve; Xu, Wenqian; Sun, Cheng‐Jun; Xu, Gui‐Liang; Amine, Khalil

doi:10.1002/ange.202203466

Title: Pushing Lithium–Sulfur Batteries towards Practical Working Conditions through a Cathode–Electrolyte Synergy

Journal Article · 04 May 2022 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202203466 · OSTI ID:1866651

Zhao, Chen ^[1]; Daali, Amine ^[1]; Hwang, Inhui ^[2]; Li, Tianyi ^[2]; Huang, Xingkang ^[1]; Robertson, David ^[1]; Yang, Zhenzhen ^[1]; Trask, Steve ^[1]; Xu, Wenqian ^[2]; Sun, Cheng‐Jun ^[2];

^[1]; Amine, Khalil ^[3]

Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
X-ray Sciences Division, Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA
Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S Cass Ave Lemont IL 60439 USA, Materials Science and Engineering Stanford University Stanford CA 94305 USA, Institute for Research&, Medical Consultations Imam Abdulrahman Bin Faisal University (IAU) Dammam Saudi Arabia

Abstract The commercialization of lithium–sulfur (Li−S) batteries is still hindered by the unsatisfactory cell performance under practical working conditions, which is mainly caused by the sluggish cathode redox kinetics, severe polysulfide shuttling, and poor Li stripping/plating reversibility. Herein, we report an effective strategy by combining Se‐doped S hosted in an ordered macroporous framework with a highly fluorinated ether (HFE)‐based electrolyte to simultaneously address the aforementioned issues in both cathode and anode. A reversible and stable high areal capacity of >5.4 mAh cm ⁻² with high Coulombic efficiency >99.2 % can be achieved under high areal Se/S loading (5.8 mg cm ⁻² ), while the underlying mechanism was further revealed through synchrotron X‐ray probes and Time‐of‐Flight Secondary Ion Mass Spectrometry (ToF‐SIMS). The practical application potential was further evaluated at low (0 °C) and high (55 °C) temperatures under high areal Se/S loading (>5.0 mg cm ⁻² ) and thin Li metal (40 μm).

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1866651

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 27 Vol. 134; ISSN 0044-8249

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

Country of Publication:: Germany

Language:: English

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