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Glasses and glass–ceramics of composition Na3+3x−yRE1−xPySi3−yO9 were synthesized using RE = Sc and Y, x = 0.4, and y = 0.0 and 0.3 to obtain multiple‐phase glass–ceramics containing the highly conducting Na5RESi4O12 (N5) phase. In addition, the two model compounds Na5ScSi4O12 and Na5InSi4O12 were synthesized. Samples were characterized at two distinct annealing stages using X‐ray powder diffraction,...