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

Abstract

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.

Authors:

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

Publication Date:: Wed Aug 12 00:00:00 EDT 2020

Sponsoring Org.:: USDOE

OSTI Identifier:: 1647288

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 132 Journal Issue: 40; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, and Amine, Khalil. Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries.  Germany: N. p., 2020. 
Web.  doi:10.1002/ange.202007159.

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                    Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, & Amine, Khalil. Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries.  Germany.  https://doi.org/10.1002/ange.202007159

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                    Zhao, Chen, Xu, Gui‐Liang, Zhao, Tianshou, and Amine, Khalil. Wed .  
"Beyond the Polysulfide Shuttle and Lithium Dendrite Formation: Addressing the Sluggish Sulfur Redox Kinetics for Practical High‐Energy Li‐S Batteries".  Germany.  https://doi.org/10.1002/ange.202007159.

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@article{osti_1647288,

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

  author       = {Zhao, Chen and Xu, Gui‐Liang and Zhao, Tianshou and Amine, Khalil},

  abstractNote = {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.},

  doi          = {10.1002/ange.202007159},

  journal      = {Angewandte Chemie},

  number       = 40,

  volume       = 132,

  place        = {Germany},

  year         = {Wed Aug 12 00:00:00 EDT 2020},

  month        = {Wed Aug 12 00:00:00 EDT 2020}

}

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Abstract

Citation Formats

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Dendrite-Free and Performance-Enhanced Lithium Metal Batteries through Optimizing Solvent Compositions and Adding Combinational Additives
journal, February 2018

An Advanced Selenium-Carbon Cathode for Rechargeable Lithium-Selenium Batteries
journal, June 2013

High‐Performance Li–SeS _x All‐Solid‐State Lithium Batteries
journal, March 2019

Stabilization of Li Metal Anode in DMSO-Based Electrolytes via Optimization of Salt-Solvent Coordination for Li-O ₂ Batteries
journal, March 2017

Formulation of Blended‐Lithium‐Salt Electrolytes for Lithium Batteries
journal, December 2019

Thermal Conversion of Core–Shell Metal–Organic Frameworks: A New Method for Selectively Functionalized Nanoporous Hybrid Carbon
journal, January 2015

All solid-state polymer electrolytes for high-performance lithium ion batteries
journal, October 2016

Manipulating electrolyte and solid electrolyte interphase to enable safe and efficient Li-S batteries
journal, August 2018

Theoretical versus Practical Energy: A Plea for More Transparency in the Energy Calculation of Different Rechargeable Battery Systems
journal, December 2018

Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review
journal, July 2017

Ether-compatible sulfurized polyacrylonitrile cathode with excellent performance enabled by fast kinetics via selenium doping
journal, March 2019

Lithium‐Schwefel‐Batterien mit Magerelektrolyt: Herausforderungen und Perspektiven
journal, March 2020

The gap between long lifespan Li-S coin and pouch cells: The importance of lithium metal anode protection
journal, January 2017

Bisalt ether electrolytes: a pathway towards lithium metal batteries with Ni-rich cathodes
journal, January 2019

High-energy lithium metal pouch cells with limited anode swelling and long stable cycles
journal, May 2019

Stable cycling of high-voltage lithium metal batteries in ether electrolytes
journal, July 2018

High‐Fluorinated Electrolytes for Li–S Batteries
journal, February 2019

Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations
journal, June 2017

Amorphous S-rich S _1−x Se _x /C (x ≤ 0.1) composites promise better lithium–sulfur batteries in a carbonate-based electrolyte
journal, January 2015

An Advanced Selenium-Carbon Cathode for Rechargeable Lithium-Selenium Batteries
journal, June 2013

An Intrinsic Flame‐Retardant Organic Electrolyte for Safe Lithium‐Sulfur Batteries
journal, December 2018

Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries
journal, August 2018

Cycling and Failing of Lithium Metal Anodes in Carbonate Electrolyte
journal, August 2018

A Review of Solid Electrolyte Interphases on Lithium Metal Anode
journal, November 2015

Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization
journal, September 2019

High rate and stable cycling of lithium metal anode
journal, February 2015