Nanoscale Mapping of Extrinsic Interfaces in Hybrid Solid Electrolytes

Marm B. Dixit, Wahid Zaman, Nicholas Hortance, Stella Vujic, Brice Harkey, Fengyu Shen, Wan Yu Tsai, Vincent De Andrade, X. Chelsea Chen, Nina Balke, Kelsey B. Hatzell

Research output: Contribution to journalArticlepeer-review

105 Scopus citations

Abstract

Inorganic-organic hybrid solid electrolytes are promising material systems for all solid-state batteries (ASSBs). These electrolytes contain numerous solid|solid interfaces that govern transport pathways, electrode|electrolyte compatibility, and durability. This paper evaluates the role that electrode|electrolyte interfaces and electrolyte structure have on electrochemical performance. Atomic force microscopy techniques reveal how mechanical, adhesion, and morphological properties transform in a series of model hybrid solid electrolytes. These measurements are mapped to sub-surface microstructural features using synchrotron nano-tomography. Hybrid solid electrolytes with shorter polymer chains demonstrate a higher adhesion (>100 nN), Young's Modulus (6.4 GPa), capacity (114.6 mAh/g), and capacity retention (92.9%) than hybrid electrolytes with longer polymer chains (i.e., higher molecular weight). Extrinsic interfacial properties largely dictate electrochemical performance in ASSBs. Microstructural control over inorganic constituents may provide a means for tailoring interfacial properties in hybrid solid electrolytes.

Original languageEnglish
Pages (from-to)207-221
Number of pages15
JournalJoule
Volume4
Issue number1
DOIs
StatePublished - Jan 15 2020

Funding

The authors were supported by the National Science Foundation under grant nos. 1727863 and 1847029 . The authors acknowledge the Vanderbilt Institute of Nanoscience and Engineering (VINSE) for access to their shared characterization facilities. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by the Argonne National Laboratory under contract no. DE-AC02-06CH11357. AFM measurements were supported by the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (W.-Y.T. and N.B.). The experiments and sample preparation in this work were performed and supported at the Center for Nanophase Materials Sciences in Oak Ridge National Lab, which is a DOE Office of Science user facility. Part of the electrochemical and materials characterization was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division (X.C.C.). The authors were supported by the National Science Foundation under grant nos. 1727863 and 1847029. The authors acknowledge the Vanderbilt Institute of Nanoscience and Engineering (VINSE) for access to their shared characterization facilities. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by the Argonne National Laboratory under contract no. DE-AC02-06CH11357. AFM measurements were supported by the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (W.-Y.T. and N.B.). The experiments and sample preparation in this work were performed and supported at the Center for Nanophase Materials Sciences in Oak Ridge National Lab, which is a DOE Office of Science user facility. Part of the electrochemical and materials characterization was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division (X.C.C.). K.B.H. conceived the concept and idea. W.-Y.T. and N.B. performed the AFM measurements. M.B.D. W.Z. N.H. and V.D.A. performed the synchrotron imaging experiments. M.D. completed the image processing and analysis from the synchrotron experiments. B.H. S.V. W.Z. F.S. M.B.D. N.H. and X.C.C. helped with the electrochemical and materials characterization. M.B.D. performed all of the theoretical and modeling efforts. K.B.H. and M.B.D. wrote the manuscript. There authors declare no competing interests.

Keywords

  • atomic force microscopy
  • characterization
  • experimentation
  • solid electrolyte
  • solid-state battery
  • synchrotron

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