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

Vicky V. T. Doan-Nguyen; Kota S. Subrahmanyam; Megan M. Butala; Jeffrey A. Gerbec; Saiful M. Islam; Katherine N. Kanipe; Catrina E. Wilson; Mahalingam Balasubramanian; Kamila M. Wiaderek; Olaf J. Borkiewicz; Karena W. Chapman; Peter J. Chupas; Martin Moskovits; Bruce S. Dunn; Mercouri G. Kanatzidis; Ram Seshadri

doi:10.1021/acs.chemmater.6b03656

journal article·2016-11-22Open access

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

Vicky V. T. Doan-Nguyen, Kota S. Subrahmanyam, Megan M. Butala, Jeffrey A. Gerbec, Saiful M. Islam, Katherine N. Kanipe, Catrina E. Wilson, Mahalingam Balasubramanian, Kamila M. Wiaderek, Olaf J. Borkiewicz, Karena W. Chapman, Peter J. Chupas, Martin Moskovits, Bruce S. Dunn, Mercouri G. Kanatzidis, Ram Seshadri

Chemistry of Materials· Volume 28· Issue 22

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Source abstract

Abstract

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. We find the redox state of Mo remains unchanged across the electrochemical cycling and, correspondingly, the redox is anion-driven.

Source: openalex_inverted_index · Quality: baseline

Research context

Energy storage

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Supercapacitor Materials and Fabrication

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

California NanoSystems Institute, University of California, Santa Barbara, California 93106, United States

Materials Research Laboratory, University of California, Santa Barbara, California 93106, United States

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States

Materials Department, University of California, Santa Barbara, California 93106, United States

Mitsubishi Chemical Center for Advanced Materials, Santa Barbara, California 93106, United States

Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106, United States

X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States

Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States

Funding

University of California, Santa Barbara · University of California · Office of Science · Division of Materials Research · California NanoSystems Institute

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