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Title: Sulfonic Acid Based Complex Framework Materials (CFM): Nanostructured Polysulfide Immobilization Systems for Rechargeable Lithium–Sulfur Battery

Journal Article · · Journal of the Electrochemical Society
DOI:https://doi.org/10.1149/2.0251910jes· OSTI ID:1524478

Lithium-sulfur (Li-S) secondary batteries with sulfur cathodes and theoretical energy density of ~2600 Wh/kg, are promising high energy-density system for next-generation electric-vehicles (EVs) potentially mitigating the gravimetric and volumetric energy density limitations of existing lithium-ion (Li-ion) batteries. Herein, a chemically synthesized sulfonic acid-based complex framework material (CFM) termed as (SCFM), was used as sulfur host (S-SCFM) to prevent polysulfide dissolution in Li-S batteries. The S-SCFM based CFM cathodes show an initial capacity of 1190 mAh/g and a capacity of 1044 mAh/g after 100 cycles. In addition, the S-SCFM based CFM cathodes exhibited good cycling stability with a minimal fade rate of ~0.0012% per cycle. XPS analysis of the cycled separators with the S-SCFM electrodes shows complete absence of polysulfide species after 100 charge-discharge cycles. It was also identified that the SCFM based CFM chemically binds sulfur via -C-S- linkages thereby exhibiting an affinity for the polysulfide species formed during the charge-discharge cycles. As a result, the SCFM based CFM prevent polysulfide species from dissolving and diffusing into the electrolyte. A thorough understanding of these engineered SCFM based CFM sulfur host in Li-S battery outlined herein will be vital in designing promising sulfur hosts for next generation sulfur cathodes in Li-S batteries.

Research Organization:
Univ. of Pittsburgh, PA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
EE0006825; EE0007797; EE000819; EE0008199
OSTI ID:
1524478
Alternate ID(s):
OSTI ID: 1613998; OSTI ID: 1640023
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 166 Journal Issue: 10; ISSN 0013-4651
Publisher:
IOP Publishing - The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 44 works
Citation information provided by
Web of Science

References (91)

Optimized LiFePO[sub 4] for Lithium Battery Cathodes journal January 2001
Lithium-Sulfur Battery Technology Readiness and Applications—A Review journal November 2017
Challenges for Rechargeable Li Batteries journal February 2010
Ordered mesoporous carbon/sulfur nanocomposite of high performances as cathode for lithium–sulfur battery journal November 2011
Contributions to screening in the solid state by electron systems of remote atoms: Effects to photoelectron and Auger transitions journal January 1982
Porous Carbon Paper as Interlayer to Stabilize the Lithium Anode for Lithium–Sulfur Battery journal November 2016
Effects of novel silane modification of zeolite surface on polymer chain rigidification and partial pore blockage in polyethersulfone (PES)–zeolite A mixed matrix membranes journal April 2006
Porous Hollow Carbon@Sulfur Composites for High-Power Lithium-Sulfur Batteries journal May 2011
Role of LiNO3 in rechargeable lithium/sulfur battery journal May 2012
Heterostructures for Improved Stability of Lithium Sulfur Batteries journal January 2014
Electronically conductive phospho-olivines as lithium storage electrodes journal September 2002
Ionic liquid decorated mesoporous silica nanoparticles: a new high-performance hybrid electrolyte for lithium batteries journal January 2016
Highly reversible Li/dissolved polysulfide batteries with binder-free carbon nanofiber electrodes journal January 2013
High-performance lithium battery anodes using silicon nanowires journal December 2007
Understanding the Nature of Absorption/Adsorption in Nanoporous Polysulfide Sorbents for the Li–S Battery journal September 2012
MOFs as acid catalysts with shape selectivity properties journal January 2008
Optimization of mesoporous carbon structures for lithium–sulfur battery applications journal January 2011
A dual coaxial nanocable sulfur composite for high-rate lithium–sulfur batteries journal January 2014
Lithium/sulfur batteries with high specific energy: old challenges and new opportunities journal January 2013
Graphene-wrapped sulfur/metal organic framework-derived microporous carbon composite for lithium sulfur batteries journal December 2014
Effect of Natural Organic Substances on the Surface and Adsorptive Properties of Environmental Black Carbon (Char):  Pseudo Pore Blockage by Model Lipid Components and Its Implications for N 2 -Probed Surface Properties of Natural Sorbents journal October 2005
Electrochemical properties of sulfur electrode containing nano Al 2 O 3 for lithium/sulfur cell journal November 2007
Stabilizing lithium–sulphur cathodes using polysulphide reservoirs journal May 2011
Sulfur embedded in metal organic framework-derived hierarchically porous carbon nanoplates for high performance lithium–sulfur battery journal January 2013
Carbon with hierarchical pores from carbonized metal–organic frameworks for lithium sulphur batteries journal January 2013
The mechanism of the desulfurization of benzenethiol by nickel (110) journal May 1992
Spatially heterogeneous carbon-fiber papers as surface dendrite-free current collectors for lithium deposition journal February 2012
Embedding Sulfur in MOF-Derived Microporous Carbon Polyhedrons for Lithium-Sulfur Batteries journal June 2013
Nanomaterials for Rechargeable Lithium Batteries journal April 2008
Sulfonic Acid Analogs of Terephthalic and Trimesic Acid as Linkers in Metal-Organic Frameworks – Synthesis of Thermally Robust MOFs journal December 2009
The Lewis acidic and basic character of the internal HKUST-1 surface determined by inverse gas chromatography journal January 2015
Li-ion battery materials: present and future journal June 2015
Encapsulating Sulfur into Hierarchically Ordered Porous Carbon as a High-Performance Cathode for Lithium-Sulfur Batteries journal November 2012
A Metal–Organic Framework with Open Metal Sites for Enhanced Confinement of Sulfur and Lithium–Sulfur Battery of Long Cycling Life journal October 2013
Analysis of oxyanion (BO 3 3? , CO 3 2? , SO 4 2? , PO 4 3? , SeO 4 4- ) substitution in Y123 compounds studied by X-ray photoelectron spectroscopy journal February 1996
A hierarchical micro/mesoporous carbon fiber/sulfur composite for high-performance lithium–sulfur batteries journal January 2016
ESCA characterization of heparin-like fluoropolymers obtained by functionalization after grafting induced by swift heavy ion irradiation
  • Dapoz, Sylvie; Betz, Natacha; Guittet, Marie-Jo
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 105, Issue 1-4 https://doi.org/10.1016/0168-583X(95)00823-3
journal November 1995
Understanding the Origin of Irreversible Capacity loss in Non-Carbonized Carbonate − based Metal Organic Framework (MOF) Sulfur hosts for Lithium − Sulfur battery journal March 2017
Tuning the Adsorption of Polysulfides in Lithium–Sulfur Batteries with Metal–Organic Frameworks journal May 2017
Tunable porous structure of metal organic framework derived carbon and the application in lithium–sulfur batteries journal January 2016
Auger parameters for sulfur-containing compounds using a mixed aluminum-silver excitation source journal January 1990
A simple melting-diffusing-reacting strategy to fabricate S/NiS 2 –C for lithium–sulfur batteries journal January 2016
Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes journal September 2016
Graphene-wrapped chromium-MOF(MIL-101)/sulfur composite for performance improvement of high-rate rechargeable Li–S batteries journal January 2014
3D Porous Cu Current Collector/Li-Metal Composite Anode for Stable Lithium-Metal Batteries journal March 2017
Mesoporous carbon/sulfur composite with polyaniline coating for lithium sulfur batteries journal September 2014
A strategic approach to recharging lithium-sulphur batteries for long cycle life journal December 2013
Tuning Transition Metal Oxide-Sulfur Interactions for Long Life Lithium Sulfur Batteries: The “Goldilocks” Principle journal December 2015
Confinement of polysulfides within bi-functional metal–organic frameworks for high performance lithium–sulfur batteries journal January 2018
Phospho-olivines as Positive-Electrode Materials for Rechargeable Lithium Batteries journal April 1997
Highly dispersed sulfur in ordered mesoporous carbon sphere as a composite cathode for rechargeable polymer Li/S battery journal April 2011
Effects of Nanosized Adsorbing Material on Electrochemical Properties of Sulfur Cathodes for Li/S Secondary Batteries journal January 2004
Lithium metal protection through in-situ formed solid electrolyte interphase in lithium-sulfur batteries: The role of polysulfides on lithium anode journal September 2016
Toward Low-Cost, High-Energy Density, and High-Power Density Lithium-Ion Batteries journal June 2017
Valence band structures and core-electron energy levels in the monochalcogenides of gallium. Photoelectron spectroscopic study journal January 1972
Hierarchical Free-Standing Carbon-Nanotube Paper Electrodes with Ultrahigh Sulfur-Loading for Lithium-Sulfur Batteries journal July 2014
Polysulfide Shuttle Study in the Li/S Battery System journal January 2004
ESCA study of molecular GeS3-x Tex As2 glasses journal January 1974
Confine sulfur in mesoporous metal–organic framework @ reduced graphene oxide for lithium sulfur battery journal January 2014
3D lithium metal embedded within lithiophilic porous matrix for stable lithium metal batteries journal July 2017
MOFomics: Computational pore characterization of metal–organic frameworks journal January 2013
Sulfur-Impregnated Activated Carbon Fiber Cloth as a Binder-Free Cathode for Rechargeable Li-S Batteries journal November 2011
Thermodynamics of solvent interaction with the metal–organic framework MOF-5 journal January 2016
Properties of surface film on lithium anode with LiNO3 as lithium salt in electrolyte solution for lithium–sulfur batteries journal November 2012
Ethylene sulfate as film formation additive to improve the compatibility of graphite electrode for lithium-ion battery journal December 2013
A solid future for battery development journal September 2016
Multi-walled carbon nanotubes @ mesoporous carbon hybrid nanocomposites from carbonized multi-walled carbon nanotubes @ metal–organic framework for lithium sulfur battery journal February 2014
Sulphur–TiO2 yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries journal January 2013
High “C” rate Li-S cathodes: sulfur imbibed bimodal porous carbons journal January 2011
Spherical Ordered Mesoporous Carbon Nanoparticles with High Porosity for Lithium-Sulfur Batteries journal March 2012
High Sulfur Loading Cathodes Fabricated Using Peapodlike, Large Pore Volume Mesoporous Carbon for Lithium–Sulfur Battery journal March 2013
Lewis Acid–Base Interactions between Polysulfides and Metal Organic Framework in Lithium Sulfur Batteries journal April 2014
Challenges in the development of advanced Li-ion batteries: a review journal January 2011
Effective Suppression of Dendritic Lithium Growth Using an Ultrathin Coating of Nitrogen and Sulfur Codoped Graphene Nanosheets on Polymer Separator for Lithium Metal Batteries journal October 2015
A highly efficient polysulfide mediator for lithium–sulfur batteries journal January 2015
Molecular Spectroscopy by Means of ESCA II. Sulfur compounds. Correlation of electron binding energy with structure journal May 1970
High-performance supercapacitors and batteries derived from activated banana-peel with porous structures journal December 2016
A proof-of-concept lithium/sulfur liquid battery with exceptionally high capacity density journal August 2012
Liquid electrolyte lithium/sulfur battery: Fundamental chemistry, problems, and solutions journal June 2013
Thermal treatment induced transition from Zn 3 (OH) 2 (BDC) 2 (MOF-69c) to Zn 4 O(BDC) 3 (MOF-5) journal January 2014
Stabilized Lithium–Metal Surface in a Polysulfide-Rich Environment of Lithium–Sulfur Batteries journal July 2014
Building better lithium-sulfur batteries: from LiNO3 to solid oxide catalyst journal September 2016
An Advanced Lithium-Sulfur Battery journal May 2012
Catalytic oxidation of Li 2 S on the surface of metal sulfides for Li−S batteries journal January 2017
Effect of Multiwalled Carbon Nanotubes on Electrochemical Properties of Lithium/Sulfur Rechargeable Batteries journal January 2003
Cost Projection of State of the Art Lithium-Ion Batteries for Electric Vehicles Up to 2030 journal September 2017
Li–O2 and Li–S batteries with high energy storage journal January 2012
Electronic structure of sulphur-containing conducting polymers journal August 1987
Recent advances in lithium ion battery materials journal May 2000
Insight into lithium–metal anodes in lithium–sulfur batteries with a fluorinated ether electrolyte journal January 2015
Conducting linear chains of sulphur inside carbon nanotubes journal July 2013