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Title: Thermodynamics and Kinetics of Sulfur Cathode during Discharge in MgTFSI2 -DME Electrolyte

Journal Article · · Advanced Materials
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [3];  [1]
  1. Univ. of Maryland, College Park, MD (United States). Chemical and Biomolecular Engineering
  2. Huazhong Univ. of Science and Technology, Wuhan, Hubei (China). School of Optical and Electronic Information
  3. U.S. Army Research Lab., Adelphi, MD (United States). Electrochemistry Branch, Power and Energy Division Sensor and Electron Devices Directorate
+ Show Author Affiliations

Rechargeable magnesium/sulfur battery is of significant interest because its energy density (1700 Wh kg-1 and 3200 Wh L-1) is among the highest of all battery chemistries (lower than Li/O2 and Mg/O2 but comparable to Li/S), and Mg metal allows reversible operation (100% Coulombic efficiency) with no dendrite formation. This great promise is already justified in some early reports. However, lack of mechanistic study of sulfur reaction in the Mg cation environment has severely hindered our understanding and prevents effective measures for performance improvement. In this work, the very first systematic fundamental study on Mg/S system is conducted by combining experimental methods with computational approach. The thermodynamics and reaction pathway of sulfur cathode in MgTFSI2–DME electrolyte, as well as the associated kinetics are thoroughly investigated. The results here reveal that sulfur undergoes a consecutive staging pathway in which the formation and chain-shortening of polysulfide occur at early stage accompanied by the dissolution of long-chain polysulfide, and solid-state transition from short-chain polysulfide to magnesium sulfide occurs at late stage. Finally, the former process is much faster than the latter due to the synergetic effect of the mediating effect of dissolved polysulfide and the fast diffusion of Mg ion in the amorphous intermediate.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001160
OSTI ID:
1470667
Alternate ID(s):
OSTI ID: 1410706
Journal Information:
Advanced Materials, Vol. 30, Issue 3; Related Information: NEES partners with University of Maryland (lead); University of California, Irvine; University of Florida; Los Alamos National Laboratory; Sandia National Laboratories; Yale University; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 106 works
Citation information provided by
Web of Science

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Cited By (10)

Rechargeable Magnesium–Sulfur Battery Technology: State of the Art and Key Challenges journal September 2019
A Polysulfide-Immobilizing Polymer Retards the Shuttling of Polysulfide Intermediates in Lithium-Sulfur Batteries journal September 2018
A Crosslinked Polytetrahydrofuran‐Borate‐Based Polymer Electrolyte Enabling Wide‐Working‐Temperature‐Range Rechargeable Magnesium Batteries journal January 2019
Theoretical versus Practical Energy: A Plea for More Transparency in the Energy Calculation of Different Rechargeable Battery Systems journal December 2018
Enhancing Catalytic Activity of Titanium Oxide in Lithium–Sulfur Batteries by Band Engineering journal May 2019
Rechargeable Iron–Sulfur Battery without Polysulfide Shuttling journal September 2019
A Review of Advanced Energy Materials for Magnesium-Sulfur Batteries journal September 2018
Rechargeable Magnesium Batteries using Conversion-Type Cathodes: A Perspective and Minireview journal July 2018
PVP incorporated MoS 2 as a Mg ion host with enhanced capacity and durability journal January 2019
Theoretical versus Practical Energy: A Plea for More Transparency in the Energy Calculation of Different Rechargeable Battery Systems journal June 2019

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Related Subjects

25 ENERGY STORAGE
bio-inspired
energy storage (including batteries and capacitors)
defects
charge transport
synthesis (novel materials)
synthesis (self-assembly)
synthesis (scalable processing)
kinetics
magnesium battery
reaction mechanism
sulfur
thermodynamics