Abstract
Chalcogenide superionic sodium (Na) conductors have great potential as solid electrolytes (SEs) in all-solid-state Na batteries with advantages of high energy density, safety, and cost effectiveness. The crystal structures and ionically conductive properties of solid Na-ion conductors are strongly influenced by synthetic approaches and processing parameters. Thus, understanding the synthesis process is essential to control the structures and phases and to obtain Na-ion conductors with desirable properties. Thanks to the high-flux and deep-penetrating time-of-flight neutron diffraction (ND), in-situ experiments were able to track real-time structural changes of two chalcogenide SEs (Na3SbS4 and Na3SbS3.5Se0.5) during the solid-state synthesis. For these two conductors, the ND results revealed a fast one-step reaction for the synthesis and the molten process when heating up, and the recrystallization as well as the cubic-to-tetragonal phase transition up on cooling. Moreover, Se-doping was found to influence the reaction temperatures, lattice parameter, and structure stability based on neutron experimental observations and theoretical simulation. This work presents a detailed structural study using in-situ ND technology for the solid synthesis process of chalcogenide Na-ion conductors, beneficial for the design and synthesis of new solid-state conductors.
| Original language | English |
|---|---|
| Pages (from-to) | 5161-5166 |
| Number of pages | 6 |
| Journal | ChemSusChem |
| Volume | 14 |
| Issue number | 23 |
| DOIs | |
| State | Published - Dec 6 2021 |
Funding
The authors thank the support from U.S. Department of Energy, Office of Basic Energy Science under Award Number DE‐SC0021257, National Science Foundation EPSCoR RII Track 4 under Award Number 2033397, Conn Center for Renewable Energy Research and the EVPRI Internal Grant at University of Louisville. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors thank Dr. Dunji Yu and Mrs. Mills at SNS for the technique support. We also acknowledge the resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231. The authors thank the support from U.S. Department of Energy, Office of Basic Energy Science under Award Number DE-SC0021257, National Science Foundation EPSCoR RII Track 4 under Award Number 2033397, Conn Center for Renewable Energy Research and the EVPRI Internal Grant at University of Louisville. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors thank Dr. Dunji Yu and Mrs. Mills at SNS for the technique support. We also acknowledge the resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
| Funders | Funder number |
|---|---|
| Conn Center for Renewable Energy Research | |
| EVPRI | |
| National Science Foundation | 2033397 |
| U.S. Department of Energy | |
| Office of Science | DE‐AC02‐05CH11231 |
| Basic Energy Sciences | DE‐SC0021257 |
| Oak Ridge National Laboratory | |
| University of Louisville | |
| SNS Nordic Forest Research |
Keywords
- Na-ion conductors
- batteries
- energy storage
- neutron diffraction
- solid electrolytes
