Pyrochlore Compounds From Atomistic Simulations

Frontiers in Chemistry, vol. 9, pp. 733321

Abstract

) have a large applicability in various branches of science and technology. These materials are considered for use as effective ionic conductors for solid state batteries or as matrices for immobilization of actinide elements, amongst many other applications. In this contribution we discuss the simulation-based effort made in the Institute of Energy and Climate Research at Forschungszentrum Jülich and partner institutions regarding reliable computation of properties of pyrochlore and defect fluorite compounds. In the scope of this contribution, we focus on the investigation of dopant incorporation, defect formation and anion migration, as well as understanding of order-disorder transitions in these compounds. We present new, accurate simulated data on incorporation of U, Np, Pu, Am and Cm actinide elements into pyrochlores, activation energies for oxygen migration and radiation damage-induced structural changes in these materials. All the discussed simulation results are combined with available experimental data to provide a reliable description of properties of investigated materials. We demonstrate that a synergy of computed and experimental data leads to a superior characterization of pyrochlores, which could not be easily achieved by either of these methods when applied separately.

Authors 10

1. Oskar Cheong Aachen Chair of Theory and Computation of Energy Materials Faculty of Georesources and Materials Engineering

   Forschungszentrum Jülich · Jülich Aachen Research Alliance · RWTH Aachen University

   Affiliation as printed

   Chair of Theory and Computation of Energy Materials, Faculty of Georesources and Materials Engineering, RWTH Aachen University, Aachen, Germany

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

   Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany

2. Thomas Bornhake Aachen Chair of Theory and Computation of Energy Materials Faculty of Georesources and Materials Engineering

   Forschungszentrum Jülich · Jülich Aachen Research Alliance · RWTH Aachen University

   Affiliation as printed

   Chair of Theory and Computation of Energy Materials, Faculty of Georesources and Materials Engineering, RWTH Aachen University, Aachen, Germany

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

   Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany

3. Alison C. Shad

   Colorado State University

   Affiliation as printed

   Walter Scott Jr. College of Engineering, Colorado State University, Fort Collins, CO, United States

4. Rebekka Tesch Aachen Chair of Theory and Computation of Energy Materials Faculty of Georesources and Materials Engineering

   Forschungszentrum Jülich · Jülich Aachen Research Alliance · RWTH Aachen University

   Affiliation as printed

   Chair of Theory and Computation of Energy Materials, Faculty of Georesources and Materials Engineering, RWTH Aachen University, Aachen, Germany

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

   Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany

5. Mengli Sun

   Jülich Aachen Research Alliance · Lanzhou University

   Affiliation as printed

   Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany

   School of Nuclear Science and Technology, Lanzhou University, Lanzhou, China

6. Zhengda He

   Forschungszentrum Jülich · Jülich Aachen Research Alliance

   Affiliation as printed

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

   Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany

7. Andrey Bukayemsky

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-6, Nuclear Waste Management and Reactor Safety, Jülich, Germany

8. Victor L. Vinograd

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-6, Nuclear Waste Management and Reactor Safety, Jülich, Germany

9. Sarah C. Finkeldei

   Forschungszentrum Jülich · University of California, Irvine

   Affiliation as printed

   Department of Chemistry, Chemical and Biomolecular Engineering, and Materials Science and Engineering, University of California, Irvine, Irvine, CA, United States

   Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

10. Piotr M. Kowalski corresponding

    Forschungszentrum Jülich · Jülich Aachen Research Alliance

    Affiliation as printed

    Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research - IEK-13, Theory and Computation of Energy Materials, Jülich, Germany

    Jülich Aachen Research Alliance, JARA Energy & Center for Simulation and Data Science (CSD), Jülich, Germany