Correlating Transport and Structural Properties in Li 1+xAlxGe2–x(PO 4)3 (LAGP) Prepared from Aqueous Solution
Abstract
Li1+xAlxGe2–x(PO4)3 (LAGP) is a solid lithium-ion conductor belonging to the NASICON family, representing the solid solution of LiGe2(PO4)3 and AlPO4. The typical syntheses of LAGP either involve high-temperature melt-quenching, which is complicated and expensive, or a sol–gel process requiring costly organic germanium precursors. Herein, we report a simple method based on aqueous solutions without the need of ethoxide precursors. Using synchrotron and neutron diffraction, the crystal structure, the occupancies for Al and Ge, and the distribution of lithium were determined. Substitution of germanium by aluminum allows for an increased Li+ incorporation in the material and the actual Li+ content in the sample increases with the nominal Li+ content and a solubility limit is observed for higher aluminum content. By means of impedance spectroscopy, an increase in the ionic conductivity with increasing lithium content is observed. Whereas the lithium ionic conductivity improves, due to the increasing carrier density, the bulk activation energy increases. This correlation suggests that changes in the transport mechanism and correlated motion may be at play in the Li1+xAlxGe2–x(PO4)3 solid solution.
- Authors:
-
[1];
[1]
- Justus-Liebig-Univ., Gießen (Germany)
- Technische Univ. Munchen, Garching (Germany)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- BASF SE; International Network for Electrochemistry and Batteries; Justus-Liebig-University Giessen; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1434719
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 13; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- ENGLISH
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; NASICON; synthesis; superionic conductors; structural analysis; transport properties
Citation Formats
Weiss, Manuel, Weber, Dominik A., Senyshyn, Anatoliy, Janek, Jürgen, and Zeier, Wolfgang G. Correlating Transport and Structural Properties in Li 1+xAlxGe2–x(PO 4)3 (LAGP) Prepared from Aqueous Solution. United States: N. p., 2018.
Web. doi:10.1021/acsami.8b00842.
Weiss, Manuel, Weber, Dominik A., Senyshyn, Anatoliy, Janek, Jürgen, & Zeier, Wolfgang G. Correlating Transport and Structural Properties in Li 1+xAlxGe2–x(PO 4)3 (LAGP) Prepared from Aqueous Solution. United States. https://doi.org/10.1021/acsami.8b00842
Weiss, Manuel, Weber, Dominik A., Senyshyn, Anatoliy, Janek, Jürgen, and Zeier, Wolfgang G. Thu .
"Correlating Transport and Structural Properties in Li 1+xAlxGe2–x(PO 4)3 (LAGP) Prepared from Aqueous Solution". United States. https://doi.org/10.1021/acsami.8b00842. https://www.osti.gov/servlets/purl/1434719.
@article{osti_1434719,
title = {Correlating Transport and Structural Properties in Li 1+xAlxGe2–x(PO 4)3 (LAGP) Prepared from Aqueous Solution},
author = {Weiss, Manuel and Weber, Dominik A. and Senyshyn, Anatoliy and Janek, Jürgen and Zeier, Wolfgang G.},
abstractNote = {Li1+xAlxGe2–x(PO4)3 (LAGP) is a solid lithium-ion conductor belonging to the NASICON family, representing the solid solution of LiGe2(PO4)3 and AlPO4. The typical syntheses of LAGP either involve high-temperature melt-quenching, which is complicated and expensive, or a sol–gel process requiring costly organic germanium precursors. Herein, we report a simple method based on aqueous solutions without the need of ethoxide precursors. Using synchrotron and neutron diffraction, the crystal structure, the occupancies for Al and Ge, and the distribution of lithium were determined. Substitution of germanium by aluminum allows for an increased Li+ incorporation in the material and the actual Li+ content in the sample increases with the nominal Li+ content and a solubility limit is observed for higher aluminum content. By means of impedance spectroscopy, an increase in the ionic conductivity with increasing lithium content is observed. Whereas the lithium ionic conductivity improves, due to the increasing carrier density, the bulk activation energy increases. This correlation suggests that changes in the transport mechanism and correlated motion may be at play in the Li1+xAlxGe2–x(PO4)3 solid solution.},
doi = {10.1021/acsami.8b00842},
journal = {ACS Applied Materials and Interfaces},
number = 13,
volume = 10,
place = {United States},
year = {Thu Mar 08 00:00:00 EST 2018},
month = {Thu Mar 08 00:00:00 EST 2018}
}
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Figures / Tables:
Figure 1: (a) Polyhedral representation of the crystal structure of Li1+xAlxGe2−x(PO4)3 (M = Al/Ge). The Wyckoff 6b position for Li(1) is shown in green and the 18e position for Li(2) is depicted in yellow. The split pair site around the Li(2) position (a 36f position) is shown as smaller greenmore »
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