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Title: Molybdenum polysulfide chalcogels as high-capacity, anion-redox-driven electrode materials for Li-ion batteries

Sulfur cathodes in conversion reaction batteries offer high gravimetric capacity but suffer from parasitic polysulfide shuttling. We demonstrate here that transition metal chalcogels of approximate formula MoS 3.4 achieve a high gravimetric capacity close to 600 mAh g –1 (close to 1000 mAh g –1 on a sulfur basis) as electrode materials for lithium-ion batteries. Transition metal chalcogels are amorphous and comprise polysulfide chains connected by inorganic linkers. The linkers appear to act as a “glue” in the electrode to prevent polysulfide shuttling. The Mo chalcogels function as electrodes in carbonate- and ether-based electrolytes, which further provides evidence of polysulfide solubility not being a limiting issue. We employ X-ray spectroscopy and operando pair distribution function techniques to elucidate the structural evolution of the electrode. Raman and X-ray photoelectron spectroscopy track the chemical moieties that arise during the anion-redox-driven processes. As a result, we find the redox state of Mo remains unchanged across the electrochemical cycling and, correspondingly, the redox is anion-driven.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [2] ;  [1] ;  [1] ;  [4] ;  [4] ;  [4] ;  [4] ;  [4] ;  [1] ;  [5] ;  [2] ;  [1]
  1. Univ. of California, Santa Barbara, CA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Mitsubishi Chemical Center for Advanced Materials, Santa Barbara, CA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Univ. of California, Los Angeles, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 22; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE
OSTI Identifier:
1345401