Based on solid electrolyte instead of traditional liquid electrolyte, all-solid-state battery technology leads to the next generation of high performance sodium ion batteries. In this work, we propose a metal intermixing in the P2-type layered compounds ${\text{Na}}_2$${\text{X}}_2$${\text{TeO}}_6$ (X = Mg, Zn), resulting in ${\text{Na}}_2$(${\text{Mg}}_{2-x}$${\text{Zn}}_x$)${\text{TeO}}_6$ ($x=0,0.125,1.875,2$), for advanced solid-state electrolyte and Na ion conductor, based on first-principles calculations of electrochemical stability and Na ion diffusion. Our calculations reveal that Zn intermixing in a low content with Mg in ${\text{Na}}_2$${\text{Mg}}_2$${\text{TeO}}_6$ can effectively improve the electrochemically stable window and Na ion conductivity, whereas Mg intermixing with Zn in ${\text{Na}}_2$${\text{Zn}}_2$${\text{TeO}}_6$ slightly reduces the performance. The atom-resolved electronic density of states and electron density differences are analyzed to give an understanding of performance enhancement or deterioration by intermixing. This work highlights the possibility of improving the performance of metal oxide-based solid electrolyte by intermixing metals.

全固态电池技术以固态电解质代替传统的液态电解质，引领下一代高性能钠离子电池。在这项工作中，我们提出了 P2 型层状化合物中的金属混合${\text{钠}}_2$${\text{X}}_2$${\text{TeO}}_6$(X = Mg, Zn)，导致${\text{钠}}_2$(${\text{镁}}_{2-X}$${\text{锌}}_X$)${\text{TeO}}_6$($X=0,0.125,1.875,2$)，对于先进的固态电解质和钠离子导体，基于电化学稳定性和钠离子扩散的第一性原理计算。我们的计算表明，低含量的 Zn 与 Mg 在${\text{钠}}_2$${\text{镁}}_2$${\text{TeO}}_6$可以有效提高电化学稳定窗口和 Na 离子电导率，而 Mg 与 Zn 混合${\text{钠}}_2$${\text{锌}}_2$${\text{TeO}}_6$稍微降低性能。分析原子分辨的电子态密度和电子密度差异，以了解混合导致的性能增强或劣化。这项工作强调了通过混合金属来提高金属氧化物基固体电解质性能的可能性。