A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery

Research output: Contribution to journalArticleResearchpeer review

Authors

  • P. Jeevan Kumar
  • K. Nishimura
  • M. Senna
  • A. Düvel
  • P. Heitjans
  • T. Kawaguchi
  • N. Sakamoto
  • N. Wakiya
  • H. Suzuki

External Research Organisations

  • Shizuoka University
  • Nitte Meenakshi Institute of Technology
  • Keio University
View graph of relations

Details

Original languageEnglish
Pages (from-to)62656-62667
Number of pages12
JournalRSC Advances
Volume6
Issue number67
Publication statusPublished - 2016

Abstract

We present a novel approach to the solid-state synthesis of garnet-type cubic Li7La3Zr2O12 (c-LLZO) nanostructured particles with 1.0 mass% Al at 750 °C within 3 h. In contrast to conventional solid-state processes, a highly reactive precursor was prepared in two steps: (i) by homogenizing the stoichiometric mixture without Li, and (ii) subsequent addition of Li in the form of an ethanolic solution of lithium acetate. The actual composition determined by ICP analysis was Li6.61La3Zr2Al0.13O11.98. Sintering these nanoparticles at 1100 °C for 3 h in air after cold isostatic pressing brought a dense ceramic pellet with a relative density of 90.5%. The corresponding ionic conductivity with Au electrodes was 1.6 × 10-4 S cm-1 at room temperature. To study its electrochemical behavior as an electrolyte, a model cell of Li//(1 M LiPF6 + c-LLZO)//LiCoO2 configuration was constructed. Cyclic voltammetry of the cell delivered one set of redox couple with narrow voltage separation (15 mV) with a Li+ diffusion coefficient at room temperature of about 2 × 10-11 cm2 s-1 at the interface between LiCoO2 and 1 M LiPF6 + c-LLZO. The cell received an average discharge capacity of 64.4, 60.3, 56.1, 51.9 and 46.9 μA h cm-2 μm-1 at discharge rates 0.5C, 1C, 2C, 4C and 6C, respectively. The cell exhibited complete oxidation and reduction reactions with an average initial discharge capacity of about 64 μA h cm-2 μm-1, which is 92.7% of LiCoO2 theoretical value. These observations indicate the applicability of the present c-LLZO as an electrolyte for a solid-state Li-ion battery.

ASJC Scopus subject areas

Cite this

A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery. / Kumar, P. Jeevan; Nishimura, K.; Senna, M. et al.
In: RSC Advances, Vol. 6, No. 67, 2016, p. 62656-62667.

Research output: Contribution to journalArticleResearchpeer review

Kumar, PJ, Nishimura, K, Senna, M, Düvel, A, Heitjans, P, Kawaguchi, T, Sakamoto, N, Wakiya, N & Suzuki, H 2016, 'A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery', RSC Advances, vol. 6, no. 67, pp. 62656-62667. https://doi.org/10.1039/c6ra09695f
Kumar, P. J., Nishimura, K., Senna, M., Düvel, A., Heitjans, P., Kawaguchi, T., Sakamoto, N., Wakiya, N., & Suzuki, H. (2016). A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery. RSC Advances, 6(67), 62656-62667. https://doi.org/10.1039/c6ra09695f
Kumar PJ, Nishimura K, Senna M, Düvel A, Heitjans P, Kawaguchi T et al. A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery. RSC Advances. 2016;6(67):62656-62667. doi: 10.1039/c6ra09695f
Kumar, P. Jeevan ; Nishimura, K. ; Senna, M. et al. / A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery. In: RSC Advances. 2016 ; Vol. 6, No. 67. pp. 62656-62667.
Download
@article{b69c34f378a7488e8a0dc09ac9b83296,
title = "A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery",
abstract = "We present a novel approach to the solid-state synthesis of garnet-type cubic Li7La3Zr2O12 (c-LLZO) nanostructured particles with 1.0 mass% Al at 750 °C within 3 h. In contrast to conventional solid-state processes, a highly reactive precursor was prepared in two steps: (i) by homogenizing the stoichiometric mixture without Li, and (ii) subsequent addition of Li in the form of an ethanolic solution of lithium acetate. The actual composition determined by ICP analysis was Li6.61La3Zr2Al0.13O11.98. Sintering these nanoparticles at 1100 °C for 3 h in air after cold isostatic pressing brought a dense ceramic pellet with a relative density of 90.5%. The corresponding ionic conductivity with Au electrodes was 1.6 × 10-4 S cm-1 at room temperature. To study its electrochemical behavior as an electrolyte, a model cell of Li//(1 M LiPF6 + c-LLZO)//LiCoO2 configuration was constructed. Cyclic voltammetry of the cell delivered one set of redox couple with narrow voltage separation (15 mV) with a Li+ diffusion coefficient at room temperature of about 2 × 10-11 cm2 s-1 at the interface between LiCoO2 and 1 M LiPF6 + c-LLZO. The cell received an average discharge capacity of 64.4, 60.3, 56.1, 51.9 and 46.9 μA h cm-2 μm-1 at discharge rates 0.5C, 1C, 2C, 4C and 6C, respectively. The cell exhibited complete oxidation and reduction reactions with an average initial discharge capacity of about 64 μA h cm-2 μm-1, which is 92.7% of LiCoO2 theoretical value. These observations indicate the applicability of the present c-LLZO as an electrolyte for a solid-state Li-ion battery.",
author = "Kumar, {P. Jeevan} and K. Nishimura and M. Senna and A. D{\"u}vel and P. Heitjans and T. Kawaguchi and N. Sakamoto and N. Wakiya and H. Suzuki",
note = "Publisher Copyright: {\textcopyright} 2016 The Royal Society of Chemistry.",
year = "2016",
doi = "10.1039/c6ra09695f",
language = "English",
volume = "6",
pages = "62656--62667",
journal = "RSC Advances",
issn = "2046-2069",
publisher = "Royal Society of Chemistry",
number = "67",

}

Download

TY - JOUR

T1 - A novel low-temperature solid-state route for nanostructured cubic garnet Li7La3Zr2O12 and its application to Li-ion battery

AU - Kumar, P. Jeevan

AU - Nishimura, K.

AU - Senna, M.

AU - Düvel, A.

AU - Heitjans, P.

AU - Kawaguchi, T.

AU - Sakamoto, N.

AU - Wakiya, N.

AU - Suzuki, H.

N1 - Publisher Copyright: © 2016 The Royal Society of Chemistry.

PY - 2016

Y1 - 2016

N2 - We present a novel approach to the solid-state synthesis of garnet-type cubic Li7La3Zr2O12 (c-LLZO) nanostructured particles with 1.0 mass% Al at 750 °C within 3 h. In contrast to conventional solid-state processes, a highly reactive precursor was prepared in two steps: (i) by homogenizing the stoichiometric mixture without Li, and (ii) subsequent addition of Li in the form of an ethanolic solution of lithium acetate. The actual composition determined by ICP analysis was Li6.61La3Zr2Al0.13O11.98. Sintering these nanoparticles at 1100 °C for 3 h in air after cold isostatic pressing brought a dense ceramic pellet with a relative density of 90.5%. The corresponding ionic conductivity with Au electrodes was 1.6 × 10-4 S cm-1 at room temperature. To study its electrochemical behavior as an electrolyte, a model cell of Li//(1 M LiPF6 + c-LLZO)//LiCoO2 configuration was constructed. Cyclic voltammetry of the cell delivered one set of redox couple with narrow voltage separation (15 mV) with a Li+ diffusion coefficient at room temperature of about 2 × 10-11 cm2 s-1 at the interface between LiCoO2 and 1 M LiPF6 + c-LLZO. The cell received an average discharge capacity of 64.4, 60.3, 56.1, 51.9 and 46.9 μA h cm-2 μm-1 at discharge rates 0.5C, 1C, 2C, 4C and 6C, respectively. The cell exhibited complete oxidation and reduction reactions with an average initial discharge capacity of about 64 μA h cm-2 μm-1, which is 92.7% of LiCoO2 theoretical value. These observations indicate the applicability of the present c-LLZO as an electrolyte for a solid-state Li-ion battery.

AB - We present a novel approach to the solid-state synthesis of garnet-type cubic Li7La3Zr2O12 (c-LLZO) nanostructured particles with 1.0 mass% Al at 750 °C within 3 h. In contrast to conventional solid-state processes, a highly reactive precursor was prepared in two steps: (i) by homogenizing the stoichiometric mixture without Li, and (ii) subsequent addition of Li in the form of an ethanolic solution of lithium acetate. The actual composition determined by ICP analysis was Li6.61La3Zr2Al0.13O11.98. Sintering these nanoparticles at 1100 °C for 3 h in air after cold isostatic pressing brought a dense ceramic pellet with a relative density of 90.5%. The corresponding ionic conductivity with Au electrodes was 1.6 × 10-4 S cm-1 at room temperature. To study its electrochemical behavior as an electrolyte, a model cell of Li//(1 M LiPF6 + c-LLZO)//LiCoO2 configuration was constructed. Cyclic voltammetry of the cell delivered one set of redox couple with narrow voltage separation (15 mV) with a Li+ diffusion coefficient at room temperature of about 2 × 10-11 cm2 s-1 at the interface between LiCoO2 and 1 M LiPF6 + c-LLZO. The cell received an average discharge capacity of 64.4, 60.3, 56.1, 51.9 and 46.9 μA h cm-2 μm-1 at discharge rates 0.5C, 1C, 2C, 4C and 6C, respectively. The cell exhibited complete oxidation and reduction reactions with an average initial discharge capacity of about 64 μA h cm-2 μm-1, which is 92.7% of LiCoO2 theoretical value. These observations indicate the applicability of the present c-LLZO as an electrolyte for a solid-state Li-ion battery.

UR - http://www.scopus.com/inward/record.url?scp=84977487497&partnerID=8YFLogxK

U2 - 10.1039/c6ra09695f

DO - 10.1039/c6ra09695f

M3 - Article

AN - SCOPUS:84977487497

VL - 6

SP - 62656

EP - 62667

JO - RSC Advances

JF - RSC Advances

SN - 2046-2069

IS - 67

ER -

By the same author(s)