期刊
ADVANCED FUNCTIONAL MATERIALS
卷 31, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202010046
关键词
electrolyte stability; hydroborate; LiB; H-11; (14); lithium tetradecahydroundecaborate; nido‐ hydroborate; solid‐ state batteries; solid‐ state electrolytes
类别
资金
- Swiss National Science Foundation (SNSF) [200021L_192191]
- EMPAPOSTDOCS-II program - European Union's Horizon 2020 research and innovation program under the Marie Skodowska-Curie Grant [754364]
- SNSF [206021_150638/1]
- NCN [2019/01/Y/ST5/00046]
- Swiss National Science Foundation (SNF) [200021L_192191] Funding Source: Swiss National Science Foundation (SNF)
This study introduces hydroborate-based solid electrolytes for high voltage all-solid-state sodium batteries and proposes the cost-effective building block LiB11H14 nido-hydroborate for lithium systems with high ionic conductivity. Strategies to improve stability by modifying chemical structure are discussed, and compatibility with metallic anodes is demonstrated through galvanostatic cycling. Additionally, the electrolyte Li-2(B11H14)(CB11H12) shows promising performance in a proof-of-concept half cell with TiS2 cathode.
Hydroborate-based solid electrolytes have recently been successfully employed in high voltage, room temperature all-solid-state sodium batteries. The transfer to analogous lithium systems has failed up to now due to the lower conductivity of the corresponding lithium compounds and their high cost. Here LiB11H14 nido-hydroborate as a cost-effective building block and its high-purity synthesis is introduced. The crystal structures of anhydrous LiB11H14 as well as of LiB11H14-based mixed-anion solid electrolytes are solved and high ionic conductivities of 1.1 x 10(-4) S cm(-1) for Li-2(B11H14)(CB11H12) and 1.1 x 10(-3) S cm(-1) for Li-3(B11H14)(CB9H10)(2) are obtained, respectively. LiB11H14 exhibits an oxidative stability limit of 2.6 V versus Li+/Li and the proposed decomposition products are discussed based on density functional theory calculations. Strategies are discussed to improve the stability of these compounds by modifying the chemical structure of the nido-hydroborate cage. Galvanostatic cycling in symmetric cells with two lithium metal electrodes shows a small overpotential increase from 22.5 to 30 mV after 620 h (up to 0.5 mAh cm(-2)), demonstrating that the electrolyte is compatible with metallic anodes. Finally, the Li-2(B11H14)(CB11H12)( ) electrolyte is employed in a proof-of-concept half cell with a TiS2 cathode with a capacity retention of 82% after 150 cycles at C/5.
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