Journal
ENERGY STORAGE MATERIALS
Volume 28, Issue -, Pages 325-333Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2020.03.014
Keywords
All-solid-state battery; Sulfide electrolyte; Phosphorus sulfide molecule; Interfacial; Ionic conductivity
Funding
- Natural Sciences and Engineering Research Council of Canada
- GLABAT Solid-State Battery Inc.
- Canada Research Chair Program (CRC)
- Canada Foundation for Innovation
- Ontario Research Fund
- Canada Light Source at University of Saskatchewan (CLS)
- University of Western Ontario
- Canada Mitacs
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All-solid-state lithium sulfur batteries (ASSLSBs) are considered promising candidates for next-generation energy-storage systems due to their enhanced safety and high theoretical energy density. However, usually both solid-state electrolyte (SSE) and conductive carbon need to be incorporated into the cathode composite to provide Li+/electron pathways, leading to the reduced energy density and inevitable SSE decomposition. Moreover, the real electrochemical behavior of S or Li2S cathodes can not be reflected due to the partially overlapped redox reaction of SSE. Herein, a series of unique P4S10+n cathodes for high-performance ASSLSBs that totally do not need any extra SSE additives are reported. Synchrotron-based X-ray absorption near edge structure coupled with other analyses confirmed that ionic conductive Li3PS4 together with Li4P2S6 components can be electrochemically self-generated during lithiation process and partially maintained to provide fast Li+ transport pathways within the cathode layer. This is further evidenced by a 30-43-fold higher reversible capacity for P4S10+n/C cathodes compared to a S/C cathode. Bulk-type ASSLSBs based on the P4S34/C cathode show a highly reversible capacity of 883 mAh g(-1) and stable cycling performance over 180 cycles with a high active material content of 70 wt%. The present study provides a promising approach for generating ionic conductive components from the electrode itself to facilitate Li+ migration within electrodes in ASSLSBs.
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