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Advanced inorganic solid electrolytes (SEs) are critical for all‐solid‐state alkaline metal batteries with high safety and high energy densities. A new interphase design to address the urgent interfacial stability issues against all‐solid‐state sodium metal batteries (ASSMBs) is proposed. The grain boundary phase of a Mg2+‐doped Na3Zr2Si2PO12 conductor (denoted as NZSP‐xMg) is manipulated to introduce...
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