Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 23, Issue 67, Pages 16941-+Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201703895
Keywords
bis(aryl) tetrasulfide; catholyte; density functional theory calculations; organopolysulfide; rechargeable lithium battery
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Funding
- Office of the Vice Chancellor for Research
- Integrated Nanosystems Development Institute [NSF MRI-1229514, NSF MRI-1429241]
- Materials Science and Engineering Center at the University of Wisconsin-Eau Claire
- NSF [CHE-1454747]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1454747] Funding Source: National Science Foundation
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An organotetrasulfide consists of a linear chain of four sulfur atoms that could accept up to 6e(-) in reduction reactions, thus providing a promising high-capacity electrode material. Herein, we study three bis(aryl) tetrasulfides as cathode materials in lithium batteries. Each tetrasulfide exhibits two major voltage regions in the discharge. The high voltage slope region is governed by the formation of persulfides and thiolates, and the low voltage plateau region is due to the formation of Li2S2/Li2S. Based on theoretical calculations and spectroscopic analysis, three reduction reaction processes are revealed, and the discharge products are identified. Lithium half cells with tetrasulfide catholytes deliver high specific capacities over 200 cycles. The effects of the functional groups on the electrochemical characteristics of tetrasulfides are investigated, which provides guidance for developing optimum aryl polysulfides as cathode materials for high energy lithium batteries.
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