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Ab initio evaluation of oxygen diffusivity in LaFeO3: the role of lanthanum vacancies

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Abstract

Solid oxide fuel cells (SOFCs) are attractive for clean and efficient electricity generation, but high operating temperatures (Top > 800 °C) limit their widespread usage. Oxygen ion conducting cathode materials (mixed ion-electron conductors, MIECs), such as La1−xSrxCo1−yFeyO3 (LSCF), enable lower Top by reducing cathode polarization losses. Understanding how composition affects oxygen diffusion in LaFeO3 is vitally important for designing high-performance LSCF cathodes. To do this, we employ first-principles density functional theory plus U (DFT+U) calculations to show how lanthanum vacancies in LaFeO3 dramatically change the oxygen diffusion coefficient. Our ab initio results show that A-site substoichiometry is a viable route to increased oxygen diffusion and higher SOFC performance.

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Acknowledgments

HeteroFoaM, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under the award DE-SC0001061 provided funding for this work. The simulations carried out in this work were performed (in part) on computational resources supported by the Princeton Institute for Computational Science and Engineering (PICSciE) and the Office of Information Technology’ s High Performance Computing Center at Princeton University. Research was carried out in part at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract No. DE-AC02-98CH10886.

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Authors and Affiliations

  1. Department of Chemical and Biological Engineering, Princeton University, Princeton, 08544, New Jersey, USA

    Andrew M. Ritzmann

  2. Department of Chemical Sciences, University of Naples Federico II, Naples, 80126, Italy

    Ana B. Muñoz-García & Michele Pavone

  3. Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, 08544, New Jersey, USA

    John A. Keith

  4. Department of Mechanical and Aerospace Engineering, Program in Applied and Computational Mathematics, and Andlinger Center for Energy and Environment, Princeton University, Princeton, 08544, New Jersey, USA

    Emily A. Carter

Authors
  1. Andrew M. Ritzmann
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  2. Ana B. Muñoz-García
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  3. Michele Pavone
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  4. John A. Keith
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  5. Emily A. Carter
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Corresponding author

Correspondence to Emily A. Carter.

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For supplementary material for this article, please visit {rs|http://dx.doi.org/10.1557/mrc.2013.28|url|}

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Ritzmann, A.M., Muñoz-García, A.B., Pavone, M. et al. Ab initio evaluation of oxygen diffusivity in LaFeO3: the role of lanthanum vacancies. MRS Communications 3, 161–166 (2013). https://doi.org/10.1557/mrc.2013.28

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  • DOI: https://doi.org/10.1557/mrc.2013.28

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