Molybdenum Polysulfide Chalcogels as High-Capacity, Anion-Redox-Driven Electrode Materials for Li-Ion Batteries

Autor: Olaf J. Borkiewicz, Kamila M. Wiaderek, Katherine N. Kanipe, Mercouri G. Kanatzidis, Karena W. Chapman, Megan M. Butala, Ram Seshadri, Saiful Islam, Vicky V. T. Doan-Nguyen, Mahalingam Balasubramanian, Catrina E. Wilson, Kota S. Subrahmanyam, Peter J. Chupas, Jeffrey A. Gerbec, Martin Moskovits, Bruce Dunn
Rok vydání: 2016
Předmět:
Zdroj: Chemistry of Materials. 28:8357-8365
ISSN: 1520-5002
0897-4756
DOI: 10.1021/acs.chemmater.6b03656
Popis: 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 rem...
Databáze: OpenAIRE