TY - JOUR
T1 - Molybdenum polysulfide chalcogels as high-capacity, anion-redox-driven electrode materials for Li-ion batteries
AU - Doan-Nguyen, Vicky V.T.
AU - Subrahmanyam, Kota S.
AU - Butala, Megan M.
AU - Gerbec, Jeffrey A.
AU - Islam, Saiful M.
AU - Kanipe, Katherine N.
AU - Wilson, Catrina E.
AU - Balasubramanian, Mahalingam
AU - Wiaderek, Kamila M.
AU - Borkiewicz, Olaf J.
AU - Chapman, Karena W.
AU - Chupas, Peter J.
AU - Moskovits, Martin
AU - Dunn, Bruce S.
AU - Kanatzidis, Mercouri G.
AU - Seshadri, Ram
N1 - Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/11/22
Y1 - 2016/11/22
N2 - 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.
AB - 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.
UR - https://www.scopus.com/pages/publications/84997610674
U2 - 10.1021/acs.chemmater.6b03656
DO - 10.1021/acs.chemmater.6b03656
M3 - Article
AN - SCOPUS:84997610674
SN - 0897-4756
VL - 28
SP - 8357
EP - 8365
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 22
ER -