Effect of Hydrofluoroether Cosolvent Addition on Li Solvation in Acetonitrile-Based Solvate Electrolytes and Its Influence on S Reduction in a Li–S Battery

See, Kimberly A.; Wu, Heng -Liang; Lau, Kah Chun; Shin, Minjeong; Cheng, Lei; Balasubramanian, Mahalingam; Gallagher, Kevin G.; Curtiss, Larry A.; Gewirth, Andrew A.

doi:10.1021/acsami.6b11358

Title: Effect of Hydrofluoroether Cosolvent Addition on Li Solvation in Acetonitrile-Based Solvate Electrolytes and Its Influence on S Reduction in a Li–S Battery

Journal Article · Wed Nov 16 00:00:00 EST 2016 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.6b11358· OSTI ID:1374850

See, Kimberly A. ^[1]; Wu, Heng -Liang ^[1]; Lau, Kah Chun ^[2]; Shin, Minjeong ^[1]; Cheng, Lei ^[3]; Balasubramanian, Mahalingam ^[3]; Gallagher, Kevin G. ^[3]; Curtiss, Larry A. ^[3];

^[1]

Joint Center for Energy Storage Research, Argonne, IL (United States); Univ. of Illinois at Urbana - Champaign, Urbana, IL (United States)
Joint Center for Energy Storage Research, Argonne, IL (United States); California State Univ., Northridge, CA (United States)
Joint Center for Energy Storage Research, Argonne, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Li-S batteries are a promising next-generation battery technology. Due to the formation of soluble polysulfides during cell operation, the electrolyte composition of the cell plays an active role in directing the formation and speciation of the soluble lithium polysulfides. Recently, new classes of electrolytes termed "solvates" that contain stoichiometric quantities of salt and solvent and form a liquid at room temperature have been explored due to their sparingly solvating properties with respect to polysulfides. The viscosity of the solvate electrolytes is understandably high limiting their viability; however, hydrofluoroether cosolvents, thought to be inert to the solvate structure itself, can be introduced to reduce viscosity and enhance diffusion. Nazar and co-workers previously reported that addition of 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) to the LiTFSI in acetonitrile solvate, (MeCN)₂-LiTFSI, results in enhanced capacity retention compared to the neat solvate. Here, we evaluate the effect of TTE addition on both the electrochemical behavior of the Li-S cell and the solvation structure of the (MeCN)₂-LiTFSI electrolyte. Contrary to previous suggestions, Raman and NMR spectroscopy coupled with ab initio molecular dynamics simulations show that TTE coordinates to Li⁺ at the expense of MeCN coordination, thereby producing a higher content of free MeCN, a good polysulfide solvent, in the electrolyte. Furthermore, the electrolytes containing a higher free MeCN content facilitate faster polysulfide formation kinetics during the electrochemical reduction of S in a Li-S cell likely as a result of the solvation power of the free MeCN.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1374850

Journal Information:: ACS Applied Materials and Interfaces, Vol. 8, Issue 50; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 42 works

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Title: Effect of Hydrofluoroether Cosolvent Addition on Li Solvation in Acetonitrile-Based Solvate Electrolytes and Its Influence on S Reduction in a Li–S Battery

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