期刊
APPLIED PHYSICS LETTERS
卷 110, 期 10, 页码 -出版社
AIP Publishing
DOI: 10.1063/1.4977885
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资金
- Tohoku University
- Collaborative Research Center on Energy Materials, Tohoku University
- JSPS KAKENHI [25220911, 16H04513, 16K06766]
- Grants-in-Aid for Scientific Research [16H04513, 16K06766] Funding Source: KAKEN
In the present work, we developed highly sodium-ion conductive Na2B10H10-Na2B12H12 pseudobinary complex hydride via mechanically ball-milling admixtures of the pure Na2B10H10 and Na2B12H12 components. Both of these components show a monoclinic phase at room temperature, but ball-milled mixtures partially stabilized highly ion-conductive, disordered cubic phases, whose fraction and favored structural symmetry (body-centered cubic or face-centered cubic) depended on the conditions of mechanical ball-milling and molar ratio of the component compounds. First-principles molecular-dynamics simulations demonstrated that the total energy of the closo-borane mixtures and pure materials is quite close, helping to explain the observed stabilization of the mixed compounds. The ionic conductivity of the closo-borane mixtures appeared to be correlated with the fraction of the body-centered-cubic phase, exhibiting a maximum at a molar ratio of Na2B10H10:Na2B12H12 = 1:3. A conductivity as high as log(sigma/S cm(-1)) = -3.5 was observed for the above ratio at 303 K, being approximately 2-3 orders of magnitude higher than that of either pure material. A bulk-type all-solid-state sodium-ion battery with a closo-borane-mixture electrolyte, sodium-metal negative-electrode, and TiS2 positive-electrode demonstrated a high specific capacity, close to the theoretical value of NaTiS2 formation and a stable discharge/charge cycling for at least eleven cycles, with a high discharge capacity retention ratio above 91% from the second cycle.
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