@article{f38d5e61a93b4359bd0f2039319ad7fd,
title = "Designing Optimal Perovskite Structure for High Ionic Conduction",
abstract = "Solid-oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure–property relationships that would enable the rational design of better materials. Here, using epitaxial thin-film growth, synchrotron radiation, impedance spectroscopy, and density-functional theory, the impact of structural parameters (i.e., unit-cell volume and octahedral rotations) on ionic conductivity is delineated in La0.9Sr0.1Ga0.95Mg0.05O3– δ. As compared to the zero-strain state, compressive strain reduces the unit-cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit-cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit-cell volumes and octahedral rotations decrease migration barriers and create low-energy migration pathways, respectively. The desired combination of large unit-cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit-cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈2.5 at around 600 °C is observed, which sheds new light on the rational design of ion-conducting perovskite electrolytes.",
keywords = "crystal symmetry, energy conversion, ionic conduction, octahedral rotation, perovskite oxides, strain",
author = "Ran Gao and Jain, {Abhinav C.P.} and Shishir Pandya and Yongqi Dong and Yakun Yuan and Hua Zhou and Dedon, {Liv R.} and Vincent Thor{\'e}ton and Sahar Saremi and Ruijuan Xu and Aileen Luo and Ting Chen and Venkatraman Gopalan and Elif Ertekin and John Kilner and Tatsumi Ishihara and Perry, {Nicola H.} and Trinkle, {Dallas R.} and Martin, {Lane W.}",
note = "Funding Information: R.G., A.C.P.J., A.L., E.E., N.H.P., and D.R.T. acknowledge the support of the National Science Foundation under grant OISE-1545907. S.P. acknowledges support of the Army Research Office under grant W911NF-14-1-0104. Y.D. and H.Z. acknowledge the 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 Argonne National Laboratory under Contract No. DE-AC02-06CH11357. L.R.D., Y.Y., and V.G. acknowledge the support of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC-0012375 for development of the complex-oxide materials and chemical studies herein and the COBRA analysis. V.T. and T.I. acknowledge the financial support from a Grant-in-Aid for Specially Promoted Research (No.16H06293) from MEXT, Japan and through the Japan Society for the Promotion of Science and the Solid Oxide Interfaces for Faster Ion Transport JSPS Core-to-Core Program (Advanced Research Networks). S.S. acknowledges support of the National Science Foundation under grant DMR-1608938. R.X. acknowledges support from the National Science Foundation under grant DMR-1708615. T.C. acknowledges a JSPS doctoral fellowship. N.H.P. and T.C. also acknowledge the support of the International Institute for Carbon Neutral Energy Research (WPI-I2CNER), sponsored by the Japanese Ministry of Education, Culture, Sports, Science and Technology. L.W.M. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05-CH11231: Materials Project program KC23MP for development of functional complex-oxide materials. The computational work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1053575. Publisher Copyright: {\textcopyright} 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",
year = "2020",
month = jan,
day = "1",
doi = "10.1002/adma.201905178",
language = "English (US)",
volume = "32",
journal = "Advanced Materials",
issn = "0935-9648",
publisher = "Wiley-VCH",
number = "1",
}