Journal
CHEMISTRY OF MATERIALS
Volume 28, Issue 22, Pages 8357-8365Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.6b03656
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Funding
- California NanoSystems Institute (CNSI)
- National Science Foundation (NSF) [DMR-1410169]
- NSF [DMR 1121053]
- DOE Office of Science [DE-AC02-06CH11357]
- University of California
- University of California, Santa Barbara CNSI Elings Prize Fellowship
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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 MoS3.4 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. We find the redox state of Mo remains unchanged across the electrochemical cycling and, correspondingly, the redox is anion-driven.
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