| Autor: |
Howard JD; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Evmenenko G; Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States., Kim JJ; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Warburton RE; Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States., Patel S; Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States., Fister TT; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Buchholz DB; Materials Research Science and Engineering Center (MRSEC), Northwestern University, 633 Clark Street, Evanston, Illinois 60208, United States., Greeley J; Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States., Curtiss LA; Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States., Fenter P; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States. |
| Abstrakt: |
Intermixing of atomic species at the electrode-electrolyte boundaries can impact the properties of the interfaces in solid-state batteries. Herein, this work uses first-principles statistical mechanics along with experimental characterization to understand intermixing at the electrode-electrolyte interface. For the model presented in this work, lithium manganese oxide (LiMn 2 O 4 , LMO) and lithium lanthanum titanate (Li 3 x La 2/3- x TiO 3 , LLTO) are employed as the cathode and electrolyte, respectively. The results of the computational work show that Ti-Mn intermixing at the interface is significant at synthesis temperatures. The experimental results in this work find that, at some critical temperatures between 600 and 700 °C for material preparation, the interface of LLTO-LMO becomes blurred. Calculations predict that the interface is unstable with regard to Ti-Mn intermixing starting at 0 K, suggesting that the critical temperature found in the experiment is related to kinetics. The work overall suggests that, in designing a solid-state battery, the fundamental reactions such as intermixing need to be considered. |
