Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 15, Pages 17554-17564Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c01659
Keywords
solid-state electrolytes; ionic conductivity; interface; closo-decaborates; iodine substitution
Funding
- National Natural Science Foundation of China [U1804253, 21771057, 21975168]
- Danish Council for Independent Research, Technology and Production [DFF. 4181-00462]
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Solid-state electrolytes based on closo-decaborates are of interest due to their impressive room-temperature ionic conductivity, stability, and flexibility. Iodine substitution in closo-decaborates was found to increase thermal decomposition temperature. Li-2[B10I10] exhibits enhanced ionic conductivity compared to the parent compound, showing potential for high-temperature battery applications.
Solid-state electrolytes based on closo-decaborates have caught increasing interest owing to the impressive room-temperature ionic conductivity, remarkable thermal/chemical stability, and excellent deformability. In order to develop new solid-state ion conductors, we investigated the influence of iodine substitution on the thermal, structural, and ionic conduction properties of closo-decaborates. A series of iodinated closo-decaborates, M-2[B10H10-nIn] (M = Li, Na; n = 1, 2, 10), were synthesized and characterized by thermal analysis, powder X-ray diffraction, and electro-chemical impedance spectroscopy; the stability and ionic conductivity of these compounds were studied. It was found that with the increase of iodine substitution on the closo-decaborate anion cage, the thermal decomposition temperature increases. All M-2[B10H10-nIn] exhibit an amorphous structure. The ionic conductivity of Li-2[B10H10-nIn] is higher than that of the Li-2[B10H10] parent compound. An ionic conductivity of 2.96 x 10(-2) S cm(-1) with an activation energy of 0.23 eV was observed for Li-2[B10I10] at 300 degrees C, implying that iodine substitution can improve the ionic conductivity. However, the ionic conductivity of Na-2[B10H10-nIn] is lower than that of Na-2[B10H10] and increases with the increase of iodine substitution, which could be associated with the increase of the electrostatic potential, mass, and volume of the iodinated anions. Moreover, Li2[B10I10] offers a Li-ion transference number of 0.999, an electrochemical stability window of 3.3 V and good compatibility with the Li anode, demonstrating its potential for application in high-temperature batteries.
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