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Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [4];  [1];  [1];  [5];  [1];  [6];  [6];  [7];  [6];  [6];  [3];  [1];  [8]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. China Univ. of Petroleum-Beijing (China). State Key Lab. of Heavy Oil Processing. Inst. of New Energy
  3. Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  6. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States). Materials Science and Engineering
+ Show Author Affiliations

Lithium/selenium-sulfur batteries have recently received considerable attention due to their relatively high specific capacities and high electronic conductivity. Different from the traditional encapsulation strategy for suppressing the shuttle effect, an alternative approach to directly bypass polysulfide/polyselenide formation via rational solid-electrolyte interphase (SEI) design is demonstrated here. It is found that the robust SEI layer that in situ forms during charge/discharge via interplay between rational cathode design and optimal electrolytes could enable solid-state (de)lithiation chemistry for selenium-sulfur cathodes. Hence, Se-doped S22.2Se/Ketjenblack cathodes can attain a high reversible capacity with minimal shuttle effects during long-term and high rate cycling. Moreover, the underlying solid-state (de)lithiation mechanism, as evidenced by in situ 7Li NMR and in operando synchrotron X-ray probes, further extends the optimal sulfur confinement pore size to large mesopores and even macropores that have been long considered as inferior sulfur or selenium host materials, which play a crucial role in developing high volumetric energy density batteries. It is expected that the findings in this study will ignite more efforts to tailor the compositional/structure characteristics of the SEI layers and the related ionic transport across the interface by electrode structure, electrolyte solvent, and electrolyte additive screening.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1494801
Alternate ID(s):
OSTI ID: 1507728
OSTI ID: 1557857
OSTI ID: 1482139
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 2 Vol. 9; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (5)

Ether-compatible sulfurized polyacrylonitrile cathode with excellent performance enabled by fast kinetics via selenium doping journal March 2019
A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free‐Energy Relationship in Lithium–Sulfur Batteries journal June 2019
A Selection Rule for Hydrofluoroether Electrolyte Cosolvent: Establishing a Linear Free-Energy Relationship in Lithium-Sulfur Batteries journal June 2019
A 3D-printed ultra-high Se loading cathode for high energy density quasi-solid-state Li–Se batteries journal January 2020
Building Better Batteries in the Solid State: A Review journal November 2019

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Related Subjects

(de)lithiation chemistry
25 ENERGY STORAGE
cathode
electrolytes
selenium-sulfur
solid-electrolyte interphase