Details
| Originalsprache | Englisch |
|---|---|
| Seiten (von - bis) | 1028-1033 |
| Seitenumfang | 6 |
| Fachzeitschrift | European Journal of Inorganic Chemistry |
| Jahrgang | 2021 |
| Ausgabenummer | 11 |
| Frühes Online-Datum | 14 Jan. 2021 |
| Publikationsstatus | Veröffentlicht - 15 März 2021 |
Abstract
Diffusion processes of small cations and anions play important roles in many applications such as batteries and sensors. Despite the enormous progress we have witnessed over the past years in characterizing the irregular movement of ions such as Li+, new methods able to sharpen our view and understanding of fast and slow diffusion phenomena are steadily developed. Still, very few techniques are, however, available to directly sense extremely slow Li+ diffusion processes. Here, we took advantage of 1D evolution-time resolved 7Li spin-alignment echo NMR that is able to probe the extremely slow interlayer Li+ hopping process in layer-structured Li3N, which served as a model substance for our purposes. The use of single crystals enabled us to study this translational process without being interfered by the fast intralayer Li+ motions. At 318 K the corresponding jump rate of interlayer dynamics turned out to be in the order of 2500(200) s−1 resulting in a diffusion coefficient as low as 1×10−17 m2 s−1, which is in excellent agreement with results from literature. The method, comparable to 1D and 2D NMR exchange spectroscopy, relies on temporal fluctuations of electric interactions the jumping ions are subjected to. 7Li single crystal 1D SAE NMR offers new opportunities to precisely quantify slow Li+ diffusion processes needed to validate theoretical models and to develop design principles for new solid electrolytes.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Anorganische Chemie
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in: European Journal of Inorganic Chemistry, Jahrgang 2021, Nr. 11, 15.03.2021, S. 1028-1033.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Direct Assessment of Ultralow Li+ Jump Rates in Single Crystalline Li3N by Evolution-Time-Resolved 7Li Spin-Alignment Echo NMR
AU - Gadermaier, Bernhard
AU - Hogrefe, Katharina
AU - Heitjans, Paul
AU - Wilkening, H. Martin R.
N1 - Funding Information: We thank the Deutsche Forschungsgemeinschaft for financial support in the frame of the research unit FOR1277 molife “Mobilität von Li–Ionen in Festkörpern” (WI3600 4–1 and 2‐1). In addition, the study received funding from the European Union's Horizon 2020 research and innovation program under the grant agreement no. 769929. P.H. is grateful to the State of Lower Saxony (Germany) for the Niedersachsen Professorship “Mobility of Ions in Solids”.
PY - 2021/3/15
Y1 - 2021/3/15
N2 - Diffusion processes of small cations and anions play important roles in many applications such as batteries and sensors. Despite the enormous progress we have witnessed over the past years in characterizing the irregular movement of ions such as Li+, new methods able to sharpen our view and understanding of fast and slow diffusion phenomena are steadily developed. Still, very few techniques are, however, available to directly sense extremely slow Li+ diffusion processes. Here, we took advantage of 1D evolution-time resolved 7Li spin-alignment echo NMR that is able to probe the extremely slow interlayer Li+ hopping process in layer-structured Li3N, which served as a model substance for our purposes. The use of single crystals enabled us to study this translational process without being interfered by the fast intralayer Li+ motions. At 318 K the corresponding jump rate of interlayer dynamics turned out to be in the order of 2500(200) s−1 resulting in a diffusion coefficient as low as 1×10−17 m2 s−1, which is in excellent agreement with results from literature. The method, comparable to 1D and 2D NMR exchange spectroscopy, relies on temporal fluctuations of electric interactions the jumping ions are subjected to. 7Li single crystal 1D SAE NMR offers new opportunities to precisely quantify slow Li+ diffusion processes needed to validate theoretical models and to develop design principles for new solid electrolytes.
AB - Diffusion processes of small cations and anions play important roles in many applications such as batteries and sensors. Despite the enormous progress we have witnessed over the past years in characterizing the irregular movement of ions such as Li+, new methods able to sharpen our view and understanding of fast and slow diffusion phenomena are steadily developed. Still, very few techniques are, however, available to directly sense extremely slow Li+ diffusion processes. Here, we took advantage of 1D evolution-time resolved 7Li spin-alignment echo NMR that is able to probe the extremely slow interlayer Li+ hopping process in layer-structured Li3N, which served as a model substance for our purposes. The use of single crystals enabled us to study this translational process without being interfered by the fast intralayer Li+ motions. At 318 K the corresponding jump rate of interlayer dynamics turned out to be in the order of 2500(200) s−1 resulting in a diffusion coefficient as low as 1×10−17 m2 s−1, which is in excellent agreement with results from literature. The method, comparable to 1D and 2D NMR exchange spectroscopy, relies on temporal fluctuations of electric interactions the jumping ions are subjected to. 7Li single crystal 1D SAE NMR offers new opportunities to precisely quantify slow Li+ diffusion processes needed to validate theoretical models and to develop design principles for new solid electrolytes.
KW - Diffusion
KW - Electrochemistry
KW - Lithium
KW - Solid electrolytes
KW - Spin-alignment echoes
UR - http://www.scopus.com/inward/record.url?scp=85100250815&partnerID=8YFLogxK
U2 - 10.1002/ejic.202000941
DO - 10.1002/ejic.202000941
M3 - Article
AN - SCOPUS:85100250815
VL - 2021
SP - 1028
EP - 1033
JO - European Journal of Inorganic Chemistry
JF - European Journal of Inorganic Chemistry
SN - 1434-1948
IS - 11
ER -