4.7 Article

Rare-Earth Element Substitution of Na1+XZr2SiXP3-XO12 (X=2) Solid Electrolyte: Implications for All-Solid-State Na Ion Batteries

Journal

ACS APPLIED NANO MATERIALS
Volume 5, Issue 10, Pages 13894-13902

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.2c01928

Keywords

NASICON; solid electrolytes; sodium ion conductor; rare-earth element doping; reaction sintering

Funding

  1. Australian Research Council [DE210101618]
  2. National Research Foundation of Korea (NRF) - Korea Government (MSIP) [2020R1A2B5B0200224713]
  3. Ministry of Trade, Industry & Energy (MOTIE, Korea) [20012341]
  4. Australian Research Council [DE210101618] Funding Source: Australian Research Council
  5. Korea Evaluation Institute of Industrial Technology (KEIT) [20012341] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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With the increasing application and market size of energy storage devices, the development of cost-effective and safe rechargeable batteries has become a major challenge. This study investigated a facile method for preparing a sodium superionic conductor and successfully improved its structural properties and ionic conductivity by employing reaction sintering and rare-earth element substitution. The results suggest that this approach is effective for obtaining an impurity-free and highly dense compound.
Along with the widening application and growing market size of energy storage devices, the development of costeffective rechargeable batteries with a high level of operational safety has become a major challenge. To this end, an all-solid-state battery (ASSB), which is composed of a thin film instead of a liquid, is an attractive candidate. In this study, we investigated a facile method for preparing sodium superionic conductor structured Na1+xZr2SixP3-xO12 (0 <= x <= 3, NZSP). Various attempts were made to improve the sinterability of NZSP, but the results are still unsatisfactory. We employed the reaction sintering method so that the phase formation and densification proceeded simultaneously, resulting in the densification of NZSP with minimal impurities. Furthermore, we successfully substituted rare-earth elements (REs) into the Zr site of the NZSP to tune its structural properties in the nanoscale and improve its ionic conductivity. Electrochemical impedance spectroscopy results confirmed the improvement of the ionic conductivity of both the pristine NZSP and the RE-doped variant, indicating the effectiveness of reaction sintering. When reaction sintering and RE substitution were employed together, La-doped NZSP was an attractive solid electrolyte for application in ASSBs. Our results highlight the effectiveness of reaction sintering for obtaining an impurity-free and highly dense multicomponent compound.

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