Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries

Dysart, Arthur Dence; Cardoza, Neal Amadeus; Mitchell, Garrett; Ortalan, Volkan; Pol, Vilas Ganpat

doi:10.1002/ente.201900194

Title: Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries

Abstract

The role of physically restrained, noncrystalline sulfur species in rechargeable lithium–sulfur batteries is examined by electrochemical and high‐resolution material characterizations. Carbon–sulfur composites are created by melting and sublimation of sulfur in an isochoric reactor via the autogenic process. These noncrystalline sulfur cathodes demonstrate a high specific capacity of ≈1000 Ah kg ⁻¹ after 100 cycles with a gravimetric current of 557 A kg ⁻¹ . Interestingly, this high‐performance sulfur allotrope lacks a long‐range structural order: high‐resolution X‐ray diffraction, performed at the Advanced Photon Source, indicates the lack of crystalline (i.e., orthorhombic or monoclinic) sulfur in the nanoscale domain. Electrochemical and material characterizations suggest that noncrystalline sulfur is a consequence of synthesis and not necessarily evidence of electrochemical efficacy. Rather, a high rate capacity depends on sulfur distribution, in turn, controlled by synthesis pathway. At higher sulfur content, the performance of carbon–sulfur composites is limited by the available surface area in which crystalline sulfur coincides with reduced gravimetric capacity and greater charge transport impedance, suggesting suboptimal sulfur containment.

Authors:

Dysart, Arthur Dence ^[1]; Cardoza, Neal Amadeus ^[1]; Mitchell, Garrett ^[1]; Ortalan, Volkan ^[2];

^[1]

Davidson School of Chemical Engineering Purdue University West Lafayette IN 47907 USA
School of Materials Engineering Purdue University West Lafayette IN 47907 USA

Publication Date:: Tue May 14 00:00:00 EDT 2019

Sponsoring Org.:: USDOE

OSTI Identifier:: 1512811

Grant/Contract Number:: SC0014664

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Energy Technology

Additional Journal Information:: Journal Name: Energy Technology Journal Volume: 7 Journal Issue: 12; Journal ID: ISSN 2194-4288

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Dysart, Arthur Dence, Cardoza, Neal Amadeus, Mitchell, Garrett, Ortalan, Volkan, and Pol, Vilas Ganpat. Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries.  Germany: N. p., 2019. 
Web.  doi:10.1002/ente.201900194.

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                    Dysart, Arthur Dence, Cardoza, Neal Amadeus, Mitchell, Garrett, Ortalan, Volkan, & Pol, Vilas Ganpat. Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries.  Germany.  https://doi.org/10.1002/ente.201900194

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                    Dysart, Arthur Dence, Cardoza, Neal Amadeus, Mitchell, Garrett, Ortalan, Volkan, and Pol, Vilas Ganpat. Tue .  
"Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries".  Germany.  https://doi.org/10.1002/ente.201900194.

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@article{osti_1512811,

  title        = {Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries},

  author       = {Dysart, Arthur Dence and Cardoza, Neal Amadeus and Mitchell, Garrett and Ortalan, Volkan and Pol, Vilas Ganpat},

  abstractNote = {The role of physically restrained, noncrystalline sulfur species in rechargeable lithium–sulfur batteries is examined by electrochemical and high‐resolution material characterizations. Carbon–sulfur composites are created by melting and sublimation of sulfur in an isochoric reactor via the autogenic process. These noncrystalline sulfur cathodes demonstrate a high specific capacity of ≈1000 Ah kg −1 after 100 cycles with a gravimetric current of 557 A kg −1 . Interestingly, this high‐performance sulfur allotrope lacks a long‐range structural order: high‐resolution X‐ray diffraction, performed at the Advanced Photon Source, indicates the lack of crystalline (i.e., orthorhombic or monoclinic) sulfur in the nanoscale domain. Electrochemical and material characterizations suggest that noncrystalline sulfur is a consequence of synthesis and not necessarily evidence of electrochemical efficacy. Rather, a high rate capacity depends on sulfur distribution, in turn, controlled by synthesis pathway. At higher sulfur content, the performance of carbon–sulfur composites is limited by the available surface area in which crystalline sulfur coincides with reduced gravimetric capacity and greater charge transport impedance, suggesting suboptimal sulfur containment.},

  doi          = {10.1002/ente.201900194},

  journal      = {Energy Technology},

  number       = 12,

  volume       = 7,

  place        = {Germany},

  year         = {Tue May 14 00:00:00 EDT 2019},

  month        = {Tue May 14 00:00:00 EDT 2019}

}

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Title: Effect of Synthesis Method Using Varying Types of Micropore Level Sulfur Infiltration on Electrochemical Performance in Lithium–Sulfur Batteries

Abstract

Citation Formats

Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report) journal, October 2015

Ordered mesoporous carbon/sulfur nanocomposite of high performances as cathode for lithium–sulfur battery journal, November 2011

The low-pressure phase diagram of sulfur journal, February 2011

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Enabling High-Energy-Density Cathode for Lithium–Sulfur Batteries journal, June 2018

Ionic Liquid Electrolytes for Lithium–Sulfur Batteries journal, September 2013

A review of recent developments in rechargeable lithium–sulfur batteries journal, January 2016

Reactions under Autogenic Pressure at Elevated Temperature (RAPET) of Various Alkoxides: Formation of Metals/Metal Oxides-Carbon Core-Shell Structures journal, September 2004

An evaluation of the thermodynamic properties and the P, T phase diagram of carbon journal, January 1986

A method to eliminate the background in X-ray diffraction patterns of oriented clay mineral samples journal, December 1981

Healing High-Loading Sulfur Electrodes with Unprecedented Long Cycling Life: Spatial Heterogeneity Control journal, March 2017

Progress Towards Commercially Viable Li-S Battery Cells journal, April 2015

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Advances in Li–S batteries journal, January 2010

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Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report)
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Ordered mesoporous carbon/sulfur nanocomposite of high performances as cathode for lithium–sulfur battery
journal, November 2011

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journal, February 2011

Viability of Polysulfide-Retaining Barriers in Li–S Battery
journal, June 2017

High-performance lithium sulfur batteries enabled by a synergy between sulfur and carbon nanotubes
journal, January 2019

Core-shell meso/microporous carbon host for sulfur loading toward applications in lithium-sulfur batteries
journal, May 2014

Enabling High-Energy-Density Cathode for Lithium–Sulfur Batteries
journal, June 2018

Ionic Liquid Electrolytes for Lithium–Sulfur Batteries
journal, September 2013

A review of recent developments in rechargeable lithium–sulfur batteries
journal, January 2016

Reactions under Autogenic Pressure at Elevated Temperature (RAPET) of Various Alkoxides: Formation of Metals/Metal Oxides-Carbon Core-Shell Structures
journal, September 2004

An evaluation of the thermodynamic properties and the P, T phase diagram of carbon
journal, January 1986

A method to eliminate the background in X-ray diffraction patterns of oriented clay mineral samples
journal, December 1981

Healing High-Loading Sulfur Electrodes with Unprecedented Long Cycling Life: Spatial Heterogeneity Control
journal, March 2017

Progress Towards Commercially Viable Li-S Battery Cells
journal, April 2015

Review on Li-Sulfur Battery Systems: an Integral Perspective
journal, May 2015

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journal, January 2010

Enhancement of long stability of sulfur cathode by encapsulating sulfur into micropores of carbon spheres
journal, January 2010

Advances in Li–S batteries
journal, January 2010

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journal, September 2012

Rechargeable Lithium–Sulfur Batteries
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Novel Synthesis of High Surface Area Silicon Carbide by RAPET (Reactions under Autogenic Pressure at Elevated Temperature) of Organosilanes
journal, April 2005

Progress on the Critical Parameters for Lithium-Sulfur Batteries to be Practically Viable
journal, May 2018

Does the sulfur cathode require good mixing for a liquid electrolyte lithium/sulfur cell?
journal, June 2013

Advanced rechargeable aluminium ion battery with a high-quality natural graphite cathode
journal, February 2017

Reversibility of electrochemical reactions of sulfur supported on inverse opal carbon in glyme–Li salt molten complex electrolytes
journal, January 2011

Li–O₂ and Li–S batteries with high energy storage
journal, January 2012

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journal, September 2016

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