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Article Abstract
Although aliovalent ion substitution is an important strategy for enhancing ionic conductivity in halide electrolytes, the choice of doping ions is often restricted to tetravalent ions, and investigations into the intrinsic origin of the doping mechanism are lacking. In this work, we investigated the effects of Zr, Ta and W doping on the crystal structure and ionic conductivity of yttrium-based rare-earth halides. Only Zr achieves fast ion diffusion in both the (001) and (002) crystal planes by affecting the volume of the octahedron and the tetrahedral interstitial space, whereas Ta significantly enhances the ion diffusion rate in the (001) crystal plane while suppressing it in the (002) plane, and W does the opposite. As a result, an optimal ionic conductivity (0.437 mS cm) is obtained for Zr substitution, while the corresponding full battery also exhibits excellent capacity, cycling and rate performance.
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