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Enhanced lithium ion transport in garnet-type solid state electrolytes

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Abstract

Al-substituted Li7La3Zr2O12 samples processed under argon show enhanced Li-ion transport and interfacial properties in symmetrical cells with lithium electrodes, compared to those prepared in air. In particular, the samples prepared under argon have higher ionic conductivities and lower interfacial impedances in symmetrical lithium cells, and show better DC cycling characteristics. The electronic conductivities are also somewhat higher. Pellets subjected to thermal treatment under the two types of atmospheres have different colors but exhibit similar microstructures. X-ray diffraction experiments suggest that there are slight structural differences between the two types of samples, but few dissimilarities were observed in elemental composition, distribution of ions, oxidation states, or bond lengths using laser-induced breakdown spectroscopy (LIBS), x-ray photoelectron spectroscopy (XPS), and extended x-ray absorption fine structure spectroscopy (EXAFS) to analyze the materials. Additionally, there was no evidence that La or Zr were reduced during the processing under Ar. Possible explanations for the improved electrochemical properties of the sample prepared under Ar compared to the one prepared in air include differences in grain boundary chemistries and conductivities and/or a small concentration of oxygen vacancies in the former.

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Acknowledgements

This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The work of Huaming Hou was supported by National Science Foundation of China (grant no. 61605161). Vassilia Zorba acknowledges support from the Chemical Science Division, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This document was prepared as an account of work sponsored by the United States Government. While this document is believed to contain correct information, neither the United States Government nor any agency thereof, nor the Regents of the University of California, nor any of their employees, makes any warranty, express or implied, or assumes any legal responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by its trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof, or the Regents of the University of California. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof or the Regents of the University of California.

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Authors and Affiliations

  1. Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA, 94720, USA

    Lei Cheng, Huaming Hou, Simon Lux, Robert Kostecki, Vassilia Zorba & Marca Doeff

  2. Department of Materials Sciences and Engineering, University of California at Berkeley, Berkeley, CA, 94720, USA

    Lei Cheng

  3. The Peac Institute of Multiscale Sciences, Chengdu, Sichuan, 610031, China

    Huaming Hou

  4. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA

    Ryan Davis & Apurva Mehta

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  1. Lei Cheng
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Correspondence to Marca Doeff.

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Cheng, L., Hou, H., Lux, S. et al. Enhanced lithium ion transport in garnet-type solid state electrolytes. J Electroceram 38, 168–175 (2017). https://doi.org/10.1007/s10832-017-0080-3

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  • DOI: https://doi.org/10.1007/s10832-017-0080-3

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