Synthesis, Electronic Structure, and Redox Chemistry of Li 2 MnP 2 S 6 , a Candidate High-Voltage Cathode Material
Source abstract
Abstract
While significant efforts have been made to harness the large capacity of sulfide-based cathodes, there has been limited focus on increasing their voltage. Here, by a novel iodide-assisted synthesis route, we successfully synthesized lithium metal thiophosphates Li 2 M P 2 S 6 ( M = Mn, Fe, and Co), of which Li 2 MnP 2 S 6 is a new compound. Electrochemical extraction of Li from Li 2 FeP 2 S 6 and Li 2 MnP 2 S 6 was performed at ∼3 V, significantly higher than other sulfide-based cathodes. Despite the similar voltages, these two materials were found to operate by very different redox mechanisms. Density functional theory calculations and X-ray absorption spectroscopy show that while Li 2 FeP 2 S 6 exhibits mostly traditional cationic redox, Li 2 MnP 2 S 6 redox involves significant participation of anionic redox. Our analysis of Li 2 MnP 2 S 6 is also used to contextualize recent work on other Li-rich thiophosphate cathodes. This work introduces a new synthetic route to access sulfide-based materials and sheds insights into the high-voltage redox mechanism in thiophosphate-based cathodes.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Advancements in Battery Materials · Extraction and Separation Processes · Advanced Battery Materials and Technologies
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, Minnesota 55455, United States
Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japan
Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo 060-8628, Japan
Instituto de Cerámica y Vidrio, CSIC, Madrid 28049, Spain
Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
Graduate School of Advanced Science and Engineering, Hiroshima University, Hiroshima 739-8526, Japan
Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Osaka 560-8531, Japan
Spectroscopy Division, Japan Synchrotron Radiation Research Institute, Sayo, Hyogo 679-5198, Japan
Funding
Precursory Research for Embryonic Science and Technology · Japan Society for the Promotion of Science · University of Minnesota
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