A defect-chemistry-informed phase-field model of grain growth in oxide electroceramics

Abstract: Dopants can significantly affect the properties of oxide ceramics through their impact on the property-determined microstructure characteristics such as grain boundary segregation, space charge layer formation in the grain boundary vicinity, and the resultant microstructure features like bimodality due to abnormal grain growth. To support rational oxide ceramics design, we propose a multiphysics-based and defect-chemistry-informed phase-field grain growth model to simulate the microstructure evolution of oxide ceramics. It fully respects the thermodynamics of charged point defects (oxygen vacancies and dopants) in both the grain interior and boundaries and considers the competing kinetics of defect diffusion and grain boundary movement. The proposed phase-field model is benchmarked against well-known simplified bicrystal models, including the Mott-Schottky and Gouy-Chapman models. Various simulation results are presented to reveal the impacts of defect formation energy differences between the grain interior and the grain boundary core on the key microstructural aspects. In particular, simulation results confirm that the solute drag effect alone can lead to bimodal grain size distribution, without any contribution from grain misorientation and other anisotropy. Interestingly, abnormal grain growth simulations demonstrate that grain boundary potentials can vary substantially: grain boundaries of larger grains tend to have lower potentials than those of smaller grains. Such heterogeneous grain boundary potential distribution may inspire a new material optimization strategy through microstructure design. This study provides a comprehensive framework for defect-chemistry-consistent investigations of microstructure evolution in polycrystalline oxide ceramics, offering fundamental insights into in-situ processes during critical manufacturing stages.