TY  - JOUR
AU  - Deng, Zeyu
AU  - Mishra, Tara P.
AU  - Mahayoni, Eunike
AU  - Ma, Qianli
AU  - Tieu, Aaron Jue Kang
AU  - Guillon, Olivier
AU  - Chotard, Jean-Noël
AU  - Seznec, Vincent
AU  - Cheetham, Anthony K.
AU  - Masquelier, Christian
AU  - Gautam, Gopalakrishnan Sai
AU  - Canepa, Pieremanuele
TI  - Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes
JO  - Nature Communications
VL  - 13
IS  - 1
SN  - 2041-1723
CY  - [London]
PB  - Nature Publishing Group UK
M1  - FZJ-2022-02976
SP  - 4470
PY  - 2022
AB  - Lithium and sodium (Na) mixed polyanion solid electrolytes for all-solid-statebatteries display some of the highest ionic conductivities reported to date.However, the effect of polyanion mixing on the ion-transport properties is stillnot fully understood. Here,we focus onNa1+xZr2SixP3−xO12 (0 ≤ x ≤ 3) NASICONelectrolyte to elucidate the role of polyanion mixing on the Na-ion transportproperties. Although NASICON is a widely investigated system, transportproperties derived from experiments or theory vary by orders of magnitude.We use more than 2000 distinct ab initio-based kinetic Monte Carlo simulationsto map the compositional space of NASICON over various time ranges,spatial resolutions and temperatures. Via electrochemical impedance spectroscopymeasurements on samples with different sodium content, we findthat the highest ionic conductivity (i.e., about 0.165 S cm–1 at 473 K) isexperimentally achieved in Na3.4Zr2Si2.4P0.6O12, in line with simulations (i.e.,about 0.170 S cm–1 at 473 K). The theoretical studies indicate that dopedNASICON compounds (especially those with a silicon content x ≥ 2.4) canimprove the Na-ion mobility compared to undoped NASICON compositions.
LB  - PUB:(DE-HGF)16
C6  - 35918385
UR  - <Go to ISI:>//WOS:000836703600023
DO  - DOI:10.1038/s41467-022-32190-7
UR  - https://juser.fz-juelich.de/record/909038
ER  -