Abstract
A generic method to estimate the relative feasibility of formation of high-entropy compounds in a single phase, directly from first principles, is developed. As a first step, the relative formation abilities of 56 multicomponent, AO, oxides were evaluated. These were constructed from five cation combinations chosen from A = {Ca, Co, Cu, Fe, Mg, Mn, Ni, Zn}. Candidates for multicomponent oxides are predicted from descriptors related to the enthalpy and configurational entropy obtained from the mixing enthalpies of two-component oxides. The utility of this approach is evaluated by comparing the predicted combinations with the experimentally realized entropy-stabilized oxide, (MgCoCuNiZn)O. In the second step, Monte Carlo simulations are utilized to investigate the phase composition and local ionic segregation as a function of temperature. This approach allows for the evaluation of potential secondary phases, thereby making realistic predictions of novel multicomponent compounds that can be synthesized.
| Original language | English |
|---|---|
| Pages (from-to) | 7507-7515 |
| Number of pages | 9 |
| Journal | Chemistry of Materials |
| Volume | 32 |
| Issue number | 17 |
| DOIs | |
| State | Published - Sep 8 2020 |
Funding
This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States government retains and the publisher, by accepting the article for publication, acknowledges that the United States government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript or allow others to do so for United States government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Acknowledgments This work was supported by the LDRD Program of ORNL, managed by UT-Battelle, LLC, for the U.S. DOE. Work by V.R.C., C.A.B., and M.E. after 2020 was funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S. KC acknowledges the faculty startup grant provided by the Davidson College of Engineering at San José State University. This research used resources of the Oak Ridge Leadership Facility, which is a DOE Office of Science User Facility supported under contract DE-AC05-00OR22725, as well as National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. K.C.P. and V.R.C. acknowledge James Morris for helpful discussions. K.C.P. acknowledges helpful discussions with German D. Samolyuk and Xianglin Liu.
| Funders | Funder number |
|---|---|
| Davidson College of Engineering at San José State University | |
| V.R.C. | |
| U.S. Department of Energy | |
| Office of Science | DE-AC05-00OR22725, DE-AC02-05CH11231 |
| Basic Energy Sciences | |
| Oak Ridge National Laboratory | |
| Laboratory Directed Research and Development | |
| Division of Materials Sciences and Engineering |