DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Quantitative Analysis of Multi-Scale Heterogeneities in Complex Electrode Microstructures

Abstract

The model was developed analyzing data from five large-volume physical reconstructions – collected using Xe-plasma focused ion beam with SEM (PFIB-SEM) – of several commercial cell electrodes and from unique sets of synthetic microstructures designed to have controlled distributions in particle size and local volume fractions. When comparing physical reconstructions from distinct regions of the same electrode, millimeter length scale heterogeneities are also observed, even in microstructures with limited mesoscale variability. While the model is developed using synthetic microstructures, it is used to quantify three different types of heterogeneities in the commercial cells. The potential origins are discussed with respect to variations in particle size distributions in feedstocks and to phase distributions related to fabrication processes; the potential performance impacts are discussed with respect to two effective medium theory models. The characterization and analytical methodologies and model presented can support the design and development of improved electrodes.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [3];  [4];  [4];  [3];  [5]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States); Carnegie Mellon Univ., Pittsburgh, PA (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States); Leidos Research Support Team, Morgantown, WV (United States)
  3. Leidos Research Support Team, Morgantown, WV (United States); National Energy Technology Lab. (NETL), Morgantown, WV (United States)
  4. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  5. National Energy Technology Lab. (NETL), Morgantown, WV (United States)
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Org.:
Carnegie Mellon Univ.; National Science Foundation (NSF)
OSTI Identifier:
1607755
Grant/Contract Number:  
MCF-677785; 89243318CFE000003; DMR 1428480
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online); Journal Volume: 167; Journal Issue: 5; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Mahbub, Rubayyat, Epting, William K., Hsu, Tim, Mason, Jerry H., Feng, Minzheng, Nuhfer, Noel T., Abernathy, Harry W., Hackett, Gregory A., Litster, Shawn, Rollett, Anthony D., and Salvador, Paul A. Quantitative Analysis of Multi-Scale Heterogeneities in Complex Electrode Microstructures. United States: N. p., 2019. Web. doi:10.1149/2.0102005JES.
Mahbub, Rubayyat, Epting, William K., Hsu, Tim, Mason, Jerry H., Feng, Minzheng, Nuhfer, Noel T., Abernathy, Harry W., Hackett, Gregory A., Litster, Shawn, Rollett, Anthony D., & Salvador, Paul A. Quantitative Analysis of Multi-Scale Heterogeneities in Complex Electrode Microstructures. United States. https://doi.org/10.1149/2.0102005JES
Mahbub, Rubayyat, Epting, William K., Hsu, Tim, Mason, Jerry H., Feng, Minzheng, Nuhfer, Noel T., Abernathy, Harry W., Hackett, Gregory A., Litster, Shawn, Rollett, Anthony D., and Salvador, Paul A. Mon . "Quantitative Analysis of Multi-Scale Heterogeneities in Complex Electrode Microstructures". United States. https://doi.org/10.1149/2.0102005JES. https://www.osti.gov/servlets/purl/1607755.
@article{osti_1607755,
title = {Quantitative Analysis of Multi-Scale Heterogeneities in Complex Electrode Microstructures},
author = {Mahbub, Rubayyat and Epting, William K. and Hsu, Tim and Mason, Jerry H. and Feng, Minzheng and Nuhfer, Noel T. and Abernathy, Harry W. and Hackett, Gregory A. and Litster, Shawn and Rollett, Anthony D. and Salvador, Paul A.},
abstractNote = {The model was developed analyzing data from five large-volume physical reconstructions – collected using Xe-plasma focused ion beam with SEM (PFIB-SEM) – of several commercial cell electrodes and from unique sets of synthetic microstructures designed to have controlled distributions in particle size and local volume fractions. When comparing physical reconstructions from distinct regions of the same electrode, millimeter length scale heterogeneities are also observed, even in microstructures with limited mesoscale variability. While the model is developed using synthetic microstructures, it is used to quantify three different types of heterogeneities in the commercial cells. The potential origins are discussed with respect to variations in particle size distributions in feedstocks and to phase distributions related to fabrication processes; the potential performance impacts are discussed with respect to two effective medium theory models. The characterization and analytical methodologies and model presented can support the design and development of improved electrodes.},
doi = {10.1149/2.0102005JES},
journal = {Journal of the Electrochemical Society (Online)},
number = 5,
volume = 167,
place = {United States},
year = {Mon Dec 16 00:00:00 EST 2019},
month = {Mon Dec 16 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Rendered images of the segmented data for (a) the active anode, A1, (b) the active cathode, C1, and (c) the active cathode, C2. In each, yellow represents the ICP and red {blue} represents the ECP in the anode {cathodes}. In all images, the segmented pore regions have beenmore » rendered as transparent.« less

Save / Share:

Works referenced in this record:

Three-dimensional microstructural changes in the Ni–YSZ solid oxide fuel cell anode during operation
journal, May 2012


3D phase mapping of solid oxide fuel cell YSZ/Ni cermet at the nanoscale by holographic X-ray nanotomography
journal, December 2013


Generation of statistically representative synthetic three-dimensional microstructures
journal, March 2018


Degradation analysis and durability improvement for SOFC 1-cell stack
journal, August 2016


Microstructural design considerations for Li-ion battery systems
journal, August 2012


Microstructural analysis of a solid oxide fuel cell anode using focused ion beam techniques coupled with electrochemical simulation
journal, August 2010


Mesoscale characterization of local property distributions in heterogeneous electrodes
journal, May 2018


The Effect of Porous Composite Electrode Structure on Solid Oxide Fuel Cell Performance
journal, January 1997

  • Tanner, Cameron W.
  • Journal of The Electrochemical Society, Vol. 144, Issue 1
  • DOI: 10.1149/1.1837360

3D Microstructural characterization of a solid oxide fuel cell anode reconstructed by focused ion beam tomography
journal, September 2011


Effect of Aging on the Electrochemical Performance of LSM-YSZ Cathodes
journal, January 2015

  • Baqué, L. C.; Jørgensen, P. S.; Zhang, W.
  • Journal of The Electrochemical Society, Vol. 162, Issue 9
  • DOI: 10.1149/2.0181509jes

Using Synchrotron X-Ray Nano-CT to Characterize SOFC Electrode Microstructures in Three-Dimensions at Operating Temperature
journal, January 2011

  • Shearing, P. R.; Bradley, R. S.; Gelb, J.
  • Electrochemical and Solid-State Letters, Vol. 14, Issue 10
  • DOI: 10.1149/1.3615824

Three-dimensional numerical analysis of mixed ionic and electronic conducting cathode reconstructed by focused ion beam scanning electron microscope
journal, March 2011


A three-dimensional heterogeneity analysis of electrochemical energy conversion in SOFC anodes using electron nanotomography and mathematical modeling
journal, May 2018


Three-dimensional reconstruction of a solid-oxide fuel-cell anode
journal, June 2006

  • Wilson, James R.; Kobsiriphat, Worawarit; Mendoza, Roberto
  • Nature Materials, Vol. 5, Issue 7
  • DOI: 10.1038/nmat1668

3D Non-destructive morphological analysis of a solid oxide fuel cell anode using full-field X-ray nano-tomography
journal, November 2012


Three-dimensional reconstruction and analysis of an entire solid oxide fuel cell by full-field transmission X-ray microscopy
journal, July 2013


Quantification of SOFC anode microstructure based on dual beam FIB-SEM technique
journal, February 2010


Long-Term Stability of LSM-YSZ Based Cathodes
journal, October 2013

  • Baque, L. C.; Jorgensen, P. S.; Hansen, K. V.
  • ECS Transactions, Vol. 57, Issue 1
  • DOI: 10.1149/05701.2027ecst

On the accuracy of triple phase boundary lengths calculated from tomographic image data
journal, September 2014


The Orientation Distributions of Lines, Surfaces, and Interfaces around Three-Phase Boundaries in Solid Oxide Fuel Cell Cathodes
journal, June 2011


Performance Degradation Predictions Based on Microstructural Evolution Due to Grain Coarsening Effects in Solid Oxide Fuel Cell Electrodes
journal, January 2018

  • Mason, Jerry; Celik, Ismail; Lee, Shiwoo
  • Journal of The Electrochemical Society, Vol. 165, Issue 2
  • DOI: 10.1149/2.0721802jes

Resolving the Three-Dimensional Microstructure of Polymer Electrolyte Fuel Cell Electrodes using Nanometer-Scale X-ray Computed Tomography
journal, November 2011

  • Epting, William K.; Gelb, Jeff; Litster, Shawn
  • Advanced Functional Materials, Vol. 22, Issue 3
  • DOI: 10.1002/adfm.201101525

Observing the microstructural evolution of Ni-Yttria-stabilized zirconia solid oxide fuel cell anodes
journal, January 2016


Three-Dimensional Microstructural Evolution of Ni- Yttria-Stabilized Zirconia Solid Oxide Fuel Cell Anodes At Elevated Temperatures
journal, January 2013

  • Kennouche, David; Chen-Wiegart, Yu-chen Karen; Cronin, J. Scott
  • Journal of The Electrochemical Society, Vol. 160, Issue 11
  • DOI: 10.1149/2.084311jes

Percolation theory in SOFC composite electrodes: Effects of porosity and particle size distribution on effective properties
journal, November 2011


Fundamental mechanisms limiting solid oxide fuel cell durability
journal, August 2008


Education hubs: international, regional and local dimensions of scale and scope
journal, July 2013


Quantifying intermediate-frequency heterogeneities of SOFC electrodes using X-ray computed tomography
journal, March 2017

  • Epting, William K.; Mansley, Zachary; Menasche, David B.
  • Journal of the American Ceramic Society, Vol. 100, Issue 5
  • DOI: 10.1111/jace.14775

3D reconstruction of SOFC anodes using a focused ion beam lift-out technique
journal, September 2009


Effect of composition of (La0.8Sr0.2MnO3–Y2O3-stabilized ZrO2) cathodes: Correlating three-dimensional microstructure and polarization resistance
journal, April 2010


Solid oxide electrolyte fuel cell review
journal, January 1996


Studies of Solid Oxide Fuel Cell Electrode Evolution Using 3D Tomography
journal, March 2013

  • Yakal-Kremski, K.; Cronin, J. S.; Chen-Wiegart, Y. -C. K.
  • Fuel Cells, Vol. 13, Issue 4
  • DOI: 10.1002/fuce.201200177

Microstructure Degradation of LSM/YSZ Cathodes for Solid Oxide Fuel Cells Aged in Stack after Long Operation Time
journal, January 2017

  • Zekri, Atef; Schnetger, Bernhard; Essafi, Mohamed Amine
  • Journal of The Electrochemical Society, Vol. 164, Issue 13
  • DOI: 10.1149/2.0581713jes

Fuel flexibility study of an integrated 25kW SOFC reformer system
journal, June 2005


Triple-Phase Boundary and Surface Transport in Mixed Conducting Patterned Electrodes
journal, January 2008

  • Lynch, Matthew E.; Mebane, David S.; Liu, Yingjie
  • Journal of The Electrochemical Society, Vol. 155, Issue 6
  • DOI: 10.1149/1.2898152

Mechanisms of Performance Degradation of (La,Sr)(Co,Fe)O 3-δ Solid Oxide Fuel Cell Cathodes
journal, January 2016

  • Wang, Hongqian; Yakal-Kremski, Kyle J.; Yeh, Ted
  • Journal of The Electrochemical Society, Vol. 163, Issue 6
  • DOI: 10.1149/2.0031607jes

Three-dimensional bicontinuous ultrafast-charge and -discharge bulk battery electrodes
journal, March 2011

  • Zhang, Huigang; Yu, Xindi; Braun, Paul V.
  • Nature Nanotechnology, Vol. 6, Issue 5, p. 277-281
  • DOI: 10.1038/nnano.2011.38

An efficient approach for prediction of Warburg-type resistance under working currents
journal, August 2018


Impact of pore microstructure evolution on polarization resistance of Ni-Yttria-stabilized zirconia fuel cell anodes
journal, March 2011


Microstructural Degradation of (La,Sr)MnO[sub 3]∕YSZ Cathodes in Solid Oxide Fuel Cells with Uncoated E-Brite Interconnects
journal, January 2011

  • Wang, S.; Cruse, T. A.; Krumpelt, M.
  • Journal of The Electrochemical Society, Vol. 158, Issue 2
  • DOI: 10.1149/1.3515073

Comparison of SOFC cathode microstructure quantified using X-ray nanotomography and focused ion beam–scanning electron microscopy
journal, June 2011

  • Nelson, George J.; Harris, William M.; Lombardo, Jeffrey J.
  • Electrochemistry Communications, Vol. 13, Issue 6
  • DOI: 10.1016/j.elecom.2011.03.016

Evaluation of SOFC anode polarization simulation using three-dimensional microstructures reconstructed by FIB tomography
journal, April 2011


Advanced anodes for high-temperature fuel cells
journal, January 2004

  • Atkinson, A.; Barnett, S.; Gorte, R. J.
  • Nature Materials, Vol. 3, Issue 1
  • DOI: 10.1038/nmat1040

Solid oxide fuel cells (SOFCs): a review of an environmentally clean and efficient source of energy
journal, October 2002


Towards intelligent engineering of SOFC electrodes: a review of advanced microstructural characterisation techniques
journal, November 2010


3D Electrode Microstructure Reconstruction and Modelling
conference, January 2009

  • Rüger, Bernd; Joos, Jochen; Weber, André
  • 216th ECS Meeting, ECS Transactions
  • DOI: 10.1149/1.3205650

Characterization of SOFC Electrode Microstructure Using Nano-Scale X-ray Computed Tomography and Focused Ion Beam Techniques: a Comparative Study
journal, May 2009

  • Shearing, Paul R.; Gelb, Jeff; Brandon, Nigel
  • ECS Transactions, Vol. 19, Issue 17
  • DOI: 10.1149/1.3242368

Modified Butler-Volmer Type Model Which Accounts for Triple and Double Phase Boundary Reaction Pathways
journal, May 2017

  • Mason, Jerry Hunter; Celik, Ismail Bektas; Abernathy, Harry
  • ECS Transactions, Vol. 78, Issue 1
  • DOI: 10.1149/07801.2855ecst

Towards Quantification of Local Electrochemical Parameters in Microstructures of Solid Oxide Fuel Cell Electrodes using High Performance Computations
journal, July 2017

  • Hsu, Tim; Mahbub, Rubayyat; Epting, William K.
  • ECS Meeting Abstracts, Vol. MA2017-03, Issue 1
  • DOI: 10.1149/ma2017-03/1/328