Probing Grain-Boundary Chemistry and Electronic Structure in Proton-Conducting Oxides by Atom Probe Tomography

Daniel R. Clark; Huayang Zhu; David R. Diercks; Sandrine Ricote; Robert J. Kee; Ali Almansoori; Brian P. Gorman; Ryan P. O'Hayre

doi:10.1021/acs.nanolett.6b02918

Probing Grain-Boundary Chemistry and Electronic Structure in Proton-Conducting Oxides by Atom Probe Tomography

Daniel R. Clark, Huayang Zhu, David R. Diercks, Sandrine Ricote, Robert J. Kee, Ali Almansoori, Brian P. Gorman, Ryan P. O'Hayre

Chemical and Petroleum Engineering

The Payne Institute for Public Policy

Research output: Contribution to journal › Article › peer-review

34 Scopus citations

Abstract

A laser-assisted atom-probe-tomographic (LAAPT) method has been developed and applied to measure and characterize the three-dimensional atomic and electronic nanostructure at an yttrium-doped barium zirconate (BaZr_0.9Y_0.1O_3-δ, BZY10) grain boundary. Proton-conducting perovskites, such as BZY10, are attracting intense interest for a variety of energy conversion applications. However, their implementation has been hindered, in part, because of high grain-boundary (GB) resistance that is attributed to a positive GB space-charge layer (SCL). In this study, LAAPT is used to analyze BZY10 GB chemistry in three dimensions with subnanometer resolution. From this analysis, maps of the charge density and electrostatic potential arising at the GBs are derived, revealing for the first time direct chemical evidence that a positive SCL indeed exists at these GBs. These maps reveal new insights on the inhomogeneity of the SCL region and produce an average GB potential barrier of approximately 580 mV, agreeing with previous indirect electrochemical measurements.

Original language	British English
Pages (from-to)	6924-6930
Number of pages	7
Journal	Nano Letters
Volume	16
Issue number	11
DOIs	https://doi.org/10.1021/acs.nanolett.6b02918
State	Published - 9 Nov 2016

Keywords

Atom probe tomography
grain boundary characterization
proton-conducting ceramics
space-charge layer

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10.1021/acs.nanolett.6b02918

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@article{a21734c3407e4f1f978664d5ff02cd98,

title = "Probing Grain-Boundary Chemistry and Electronic Structure in Proton-Conducting Oxides by Atom Probe Tomography",

abstract = "A laser-assisted atom-probe-tomographic (LAAPT) method has been developed and applied to measure and characterize the three-dimensional atomic and electronic nanostructure at an yttrium-doped barium zirconate (BaZr0.9Y0.1O3-δ, BZY10) grain boundary. Proton-conducting perovskites, such as BZY10, are attracting intense interest for a variety of energy conversion applications. However, their implementation has been hindered, in part, because of high grain-boundary (GB) resistance that is attributed to a positive GB space-charge layer (SCL). In this study, LAAPT is used to analyze BZY10 GB chemistry in three dimensions with subnanometer resolution. From this analysis, maps of the charge density and electrostatic potential arising at the GBs are derived, revealing for the first time direct chemical evidence that a positive SCL indeed exists at these GBs. These maps reveal new insights on the inhomogeneity of the SCL region and produce an average GB potential barrier of approximately 580 mV, agreeing with previous indirect electrochemical measurements.",

keywords = "Atom probe tomography, grain boundary characterization, proton-conducting ceramics, space-charge layer",

author = "Clark, {Daniel R.} and Huayang Zhu and Diercks, {David R.} and Sandrine Ricote and Kee, {Robert J.} and Ali Almansoori and Gorman, {Brian P.} and O'Hayre, {Ryan P.}",

note = "Funding Information: This work has been supported by the National Science Foundation MRSEC program under Grant No. DMR-0820518, the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1057607, The Petroleum Institute in Abu Dhabi, UAE, the Colorado School of Mines Foundation, Protonic Capital Funds, and the Office of Naval Research Grant No. N00014-08-1-0539. The atom probe instrument used in this research was supported under NSF Award No. DMR-1040456. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

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doi = "10.1021/acs.nanolett.6b02918",

language = "British English",

volume = "16",

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journal = "Nano Letters",

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T1 - Probing Grain-Boundary Chemistry and Electronic Structure in Proton-Conducting Oxides by Atom Probe Tomography

AU - Clark, Daniel R.

AU - Zhu, Huayang

AU - Diercks, David R.

AU - Ricote, Sandrine

AU - Kee, Robert J.

AU - Almansoori, Ali

AU - Gorman, Brian P.

AU - O'Hayre, Ryan P.

N1 - Funding Information: This work has been supported by the National Science Foundation MRSEC program under Grant No. DMR-0820518, the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1057607, The Petroleum Institute in Abu Dhabi, UAE, the Colorado School of Mines Foundation, Protonic Capital Funds, and the Office of Naval Research Grant No. N00014-08-1-0539. The atom probe instrument used in this research was supported under NSF Award No. DMR-1040456. Publisher Copyright: © 2016 American Chemical Society.

PY - 2016/11/9

Y1 - 2016/11/9

N2 - A laser-assisted atom-probe-tomographic (LAAPT) method has been developed and applied to measure and characterize the three-dimensional atomic and electronic nanostructure at an yttrium-doped barium zirconate (BaZr0.9Y0.1O3-δ, BZY10) grain boundary. Proton-conducting perovskites, such as BZY10, are attracting intense interest for a variety of energy conversion applications. However, their implementation has been hindered, in part, because of high grain-boundary (GB) resistance that is attributed to a positive GB space-charge layer (SCL). In this study, LAAPT is used to analyze BZY10 GB chemistry in three dimensions with subnanometer resolution. From this analysis, maps of the charge density and electrostatic potential arising at the GBs are derived, revealing for the first time direct chemical evidence that a positive SCL indeed exists at these GBs. These maps reveal new insights on the inhomogeneity of the SCL region and produce an average GB potential barrier of approximately 580 mV, agreeing with previous indirect electrochemical measurements.

AB - A laser-assisted atom-probe-tomographic (LAAPT) method has been developed and applied to measure and characterize the three-dimensional atomic and electronic nanostructure at an yttrium-doped barium zirconate (BaZr0.9Y0.1O3-δ, BZY10) grain boundary. Proton-conducting perovskites, such as BZY10, are attracting intense interest for a variety of energy conversion applications. However, their implementation has been hindered, in part, because of high grain-boundary (GB) resistance that is attributed to a positive GB space-charge layer (SCL). In this study, LAAPT is used to analyze BZY10 GB chemistry in three dimensions with subnanometer resolution. From this analysis, maps of the charge density and electrostatic potential arising at the GBs are derived, revealing for the first time direct chemical evidence that a positive SCL indeed exists at these GBs. These maps reveal new insights on the inhomogeneity of the SCL region and produce an average GB potential barrier of approximately 580 mV, agreeing with previous indirect electrochemical measurements.

KW - Atom probe tomography

KW - grain boundary characterization

KW - proton-conducting ceramics

KW - space-charge layer

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DO - 10.1021/acs.nanolett.6b02918

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SN - 1530-6984

VL - 16

SP - 6924

EP - 6930

JO - Nano Letters

JF - Nano Letters

IS - 11

ER -

Probing Grain-Boundary Chemistry and Electronic Structure in Proton-Conducting Oxides by Atom Probe Tomography

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