Local Multimodal Electro-Chemical-Structural Characterization of Solid-Electrolyte Grain Boundaries

Xu, Xin; Carr, Connor; Chen, Xinqi; Myers, Benjamin D.; Huang, Ruiyun; Yuan, Weizi; Choi, Sihyuk; Yi, Dezhi; Phatak, Charudatta; Haile, Sossina M.

doi:10.1002/aenm.202003309

Title: Local Multimodal Electro-Chemical-Structural Characterization of Solid-Electrolyte Grain Boundaries

Journal Article · Mon Jan 25 00:00:00 EST 2021 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202003309· OSTI ID:1779862

^[1]; Carr, Connor ^[2]; Chen, Xinqi ^[3]; Myers, Benjamin D. ^[2]; Huang, Ruiyun ^[2]; Yuan, Weizi ^[2]; Choi, Sihyuk ^[2]; Yi, Dezhi ^[2]; Phatak, Charudatta ^[4]; Haile, Sossina M. ^[5]

Northwestern Univ., Evanston, IL (United States). Applied Physics
Northwestern Univ., Evanston, IL (United States). Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Mechanical Engineering
Northwestern Univ., Evanston, IL (United States). Materials Science and Engineering; Northwestern Univ., Evanston, IL (United States). Northwestern Argonne Institute of Science and Engineering
Northwestern Univ., Evanston, IL (United States). Applied Physics; Northwestern Univ., Evanston, IL (United States). Materials Science and Engineering

Abstract Typical models of polycrystalline ionic materials treat the grain boundary properties as single valued, without consideration of the full range of values that define the macroscopically measured average. Here a unique experimental platform suitable for local multimodal characterization of individual grain boundaries in bicrystal fibers is reported. A variation of three orders of magnitude in the grain boundary conductivity of ceria is observed, as measured across six individual bicrystals by both alternating current impedance spectroscopy and direct current (D.C.) linear sweep voltammetry. Nonlinear behavior of the D.C. measurements is consistent with resistance due to a space charge effect. Time‐of‐flight secondary ion beam spectroscopy reveals a correlation between grain boundary resistance and the concentration of impurities Si, Al, and Ca segregated at the grain boundaries, although the bulk concentrations of these impurities are negligible. Electron backscatter diffraction analysis of the crystal orientations suggests a correlation between the misorientation across the grain boundaries and grain boundary resistance. These correlations point towards a grain boundary resistance that arises from impurity‐generated space charge effects and variations in impurity concentration and hence resistivity driven by the energetics of impurity segregation to grain boundaries of differing surface energies.

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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:: 1779862

Alternate ID(s):: OSTI ID: 1804578

Journal Information:: Advanced Energy Materials, Vol. 11, Issue 10; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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