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Fluoro-Organosulfur Catholytes to Boost Lithium Primary Battery Energy

Gao, Haining and Sevilla, Alejandro and Hobold, Gustavo M. and Melemed, Aaron and Guo, Rui and Jones, Simon C. and Gallant, Betar M. (2022) Fluoro-Organosulfur Catholytes to Boost Lithium Primary Battery Energy. . (Unpublished)

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Discovery of new electrochemical redox motifs are essential to expand the design landscape for energy-dense batteries. We report a family of fluorinated reactants based on pentafluorosulfanyl arenes that allow for high electron-transfer numbers (up to 8-e⁻/reactant) by exploiting multiple coupled redox processes including extensive S–F bond breaking, yielding capacities of 861 mAh∙greactant⁻¹ and voltages up to ~2.9 V when used as catholytes in primary Li cells. At a cell level, gravimetric energies of 1085 Wh/kg are attained at moderate temperatures of 50 ºC, with 853 Wh/kg delivered at >100 W/kg, exceeding all leading primary batteries based on electrode + electrolyte (sub-stack) mass. Voltage compatibility of R-Ph-SF⁵ reactants and carbon monofluoride (CFₓ) conversion cathodes further enabled investigation of a hybrid battery containing both fluorinated catholyte and cathode. The hybrid cells reach extraordinarily high cell active mass loading (~80%) and allow for significant boosting of sub-stack gravimetric energy of Li−CFₓ cells by at least 20% while exhibiting good shelf life and safety characteristics.

Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription Paper
Gao, Haining0000-0001-7238-665X
Hobold, Gustavo M.0000-0001-6749-3370
Melemed, Aaron0000-0001-7646-3130
Jones, Simon C.0000-0002-1952-3720
Additional Information:The content is available under CC BY NC ND 4.0 License. The authors gratefully acknowledge funding from the MIT Lincoln Laboratory and from the Army Research Office under award number W911NF-19-1-0311. This work made use of the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation under award number DMR-14-19807. We gratefully acknowledge Dr. Kevin Tibbetts at MIT Lincoln Laboratory for insightful discussions. Author contributions: Conceptualization: H.G. and B.M.G.; Methodology: H.G., B.M.G., and 15 S.C.J.; Investigation: H.G., A.S., G.M.H., A.M., and R.G.; Visualization: H.G. and B.M.G.; Funding acquisition: B.M.G.; Writing – original draft: H.G. and B.M.G.; Writing – review & editing: H.G., B.M.G., S.C.J., and A.S. The authors declare that they have no competing interests
Funding AgencyGrant Number
Massachusetts Institute of Technology (MIT)UNSPECIFIED
Army Research Office (ARO)W911NF-19-1-0311
Subject Keywords:Li primary battery; high energy density; fluorinated catholyte; sulfur redox
Record Number:CaltechAUTHORS:20220517-356618000
Persistent URL:
Official Citation:Gao H, Sevilla A, Hobold G, et al. Fluoro-Organosulfur Catholytes to Boost Lithium Primary Battery Energy. ChemRxiv. 2022. doi:10.26434/chemrxiv-2022-l4bpp
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114776
Deposited By: George Porter
Deposited On:18 May 2022 14:37
Last Modified:18 May 2022 14:37

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