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Fast Na Ion Transport Triggered By Rapid Ion Exchange on Local Length Scales

13 Pages Posted: 4 Apr 2018 Sneak Peek Status: Review Complete

See all articles by S. Lunghammer

S. Lunghammer

Graz University of Technology - Christian Doppler Lab for Lithium Batteries; Graz University of Technology - Institute for Chemistry and Technology of Materials

D. Prutsch

Graz University of Technology - Institute for Chemistry and Technology of Materials; Graz University of Technology - Christian Doppler Lab for Lithium Batteries

S. Breuer

Graz University of Technology - Institute for Chemistry and Technology of Materials; Graz University of Technology - Christian Doppler Lab for Lithium Batteries

D. Rettenwander

Graz University of Technology - Institute for Chemistry and Technology of Materials; Graz University of Technology - Christian Doppler Lab for Lithium Batteries

I. Hanzu

Graz University of Technology - Institute for Chemistry and Technology of Materials; Graz University of Technology - Christian Doppler Lab for Lithium Batteries; ALISTORE European Research Institute (ALISTORE-ERI)

Q. Ma

Forschungszentrum Jülich GmbH - Department of Materials Synthesis and Processing

F. Tietz

Forschungszentrum Jülich GmbH - Department of Materials Synthesis and Processing; Forschungszentrum Jülich GmbH - Helmholtz-Institute Münster

M. Wilkening

Graz University of Technology - Institute for Chemistry and Technology of Materials; Graz University of Technology - Christian Doppler Lab for Lithium Batteries; ALISTORE European Research Institute (ALISTORE-ERI)

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Abstract

The realization of green and economically friendly energy storage systems needs materials with outstanding properties. Future batteries based on Na as an abundant element take advantage of nonflammable ceramic electrolytes with very high conductivities. Na3Zr2(SiO4)2PO4-type superionic conductors are expected to pave the way for inherently safe and sustainable all-solid-state batteries. So far, only little information has been extracted from spectroscopic measurements to clarify the origins of fast ionic hopping on the atomic length scale. Here we combined broadband conductivity spectroscopy and nuclear magnetic resonance (NMR) relaxation to study Na ion dynamics from the μm to the angstrom length scale. Spin-lattice relaxation NMR revealed a very fast Na ion exchange process in Na3.4Sc0.4Zr1.6(SiO4)2PO4 that is characterized by an unprecedentedly high self-diffusion coefficient of 9 ' 10−12 m2s−1 at –10 °C. Thus, well below ambient temperature the Na ions have access to elementary diffusion processes with a mean residence time τNMR of only 2 ns. The underlying asymmetric diffusion- induced NMR rate peak and the corresponding conductivity isotherms measured in the MHz range reveal correlated ionic motion. Obviously, local but extremely fast Na jumps, involving especially the transition sites in Sc-NZSP, trigger long-range ion transport and push ionic conductivity up to 2 mS/cm at room temperature.

Suggested Citation

Lunghammer, S. and Prutsch, D. and Breuer, S. and Rettenwander, D. and Hanzu, I. and Ma, Q. and Tietz, F. and Wilkening, M., Fast Na Ion Transport Triggered By Rapid Ion Exchange on Local Length Scales (2018). Available at SSRN: https://ssrn.com/abstract=3155540 or http://dx.doi.org/10.2139/ssrn.3155540
This is a paper under consideration at Cell Press and has not been peer-reviewed.

S. Lunghammer (Contact Author)

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

D. Prutsch

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

S. Breuer

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

D. Rettenwander

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

I. Hanzu

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

ALISTORE European Research Institute (ALISTORE-ERI)

33 Rue Saint Leu
Amiens, F-80039
France

Q. Ma

Forschungszentrum Jülich GmbH - Department of Materials Synthesis and Processing

Jülich, 52428
Germany

F. Tietz

Forschungszentrum Jülich GmbH - Department of Materials Synthesis and Processing

Jülich, 52428
Germany

Forschungszentrum Jülich GmbH - Helmholtz-Institute Münster

Jülich, 52425
Germany

M. Wilkening

Graz University of Technology - Institute for Chemistry and Technology of Materials

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

Graz University of Technology - Christian Doppler Lab for Lithium Batteries

Kopernikusgasse 24/IV
Graz, Styria A-8010
Austria

ALISTORE European Research Institute (ALISTORE-ERI)

33 Rue Saint Leu
Amiens, F-80039
France

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