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Title: Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate

Abstract

Proton-conducting perovskites have been widely studied because of their potential application as solid electrolytes in intermediate temperature solid oxide fuel cells. Structural and chemical heterogeneities can develop during synthesis, device fabrication, or service, which can profoundly affect proton transport. Here, we use time-resolved Kelvin probe force microscopy, scanning transmission electron microscopy, atom probe tomography, and density functional theory calculations to intentionally introduce Ba-deficient planar and spherical defects and link the resultant atomic structure with proton transport behavior in both stoichiometric and nonstoichiometric epitaxial, yttrium-doped barium zirconate thin films. The defects were intentionally induced through high-temperature annealing treatment, while maintaining the epitaxial single crystalline structure of the films, with an overall relaxation in the atomic structure. The annealed samples showed smaller magnitudes of local lattice distortions because of the formation of proton polarons, thereby leading to decreased proton-trapping effect. Here, this resulted in a decrease in the activation energy for proton transport, leading to faster proton transport.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3];  [4]; ORCiD logo [3]; ORCiD logo [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Shell Technology Center, Bangalore (India)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Georgia Inst. of Technology, Atlanta, GA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory, Oak Ridge Leadership Computing Facility (OLCF); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1422374
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 5; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atom probe tomography; density functional theory; Kelvin probe force microscopy; proton-conducting solid oxide fuel cells; scanning transmission electron microscopy; yttrium-doped barium zirconate

Citation Formats

Ding, Jilai, Balachandran, Janakiraman, Sang, Xiahan, Guo, Wei, Veith, Gabriel M., Bridges, Craig A., Rouleau, Christopher M., Poplawsky, Jonathan D., Bassiri-Gharb, Nazanin, Ganesh, Panchapakesan, and Unocic, Raymond R. Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate. United States: N. p., 2018. Web. doi:10.1021/acsami.7b16900.
Ding, Jilai, Balachandran, Janakiraman, Sang, Xiahan, Guo, Wei, Veith, Gabriel M., Bridges, Craig A., Rouleau, Christopher M., Poplawsky, Jonathan D., Bassiri-Gharb, Nazanin, Ganesh, Panchapakesan, & Unocic, Raymond R. Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate. United States. doi:10.1021/acsami.7b16900.
Ding, Jilai, Balachandran, Janakiraman, Sang, Xiahan, Guo, Wei, Veith, Gabriel M., Bridges, Craig A., Rouleau, Christopher M., Poplawsky, Jonathan D., Bassiri-Gharb, Nazanin, Ganesh, Panchapakesan, and Unocic, Raymond R. Thu . "Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate". United States. doi:10.1021/acsami.7b16900.
@article{osti_1422374,
title = {Influence of Nonstoichiometry on Proton Conductivity in Thin-Film Yttrium-Doped Barium Zirconate},
author = {Ding, Jilai and Balachandran, Janakiraman and Sang, Xiahan and Guo, Wei and Veith, Gabriel M. and Bridges, Craig A. and Rouleau, Christopher M. and Poplawsky, Jonathan D. and Bassiri-Gharb, Nazanin and Ganesh, Panchapakesan and Unocic, Raymond R.},
abstractNote = {Proton-conducting perovskites have been widely studied because of their potential application as solid electrolytes in intermediate temperature solid oxide fuel cells. Structural and chemical heterogeneities can develop during synthesis, device fabrication, or service, which can profoundly affect proton transport. Here, we use time-resolved Kelvin probe force microscopy, scanning transmission electron microscopy, atom probe tomography, and density functional theory calculations to intentionally introduce Ba-deficient planar and spherical defects and link the resultant atomic structure with proton transport behavior in both stoichiometric and nonstoichiometric epitaxial, yttrium-doped barium zirconate thin films. The defects were intentionally induced through high-temperature annealing treatment, while maintaining the epitaxial single crystalline structure of the films, with an overall relaxation in the atomic structure. The annealed samples showed smaller magnitudes of local lattice distortions because of the formation of proton polarons, thereby leading to decreased proton-trapping effect. Here, this resulted in a decrease in the activation energy for proton transport, leading to faster proton transport.},
doi = {10.1021/acsami.7b16900},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 5,
volume = 10,
place = {United States},
year = {2018},
month = {1}
}