Current progress in two-dimensional (2D) materials explorations leads to constant specie enrichments of possible advanced materials down to two dimensions. The metal chalcogenide-based 2D materials are promising grounds where many adjacent territories are waiting to be explored. Here, a stable monolayer Ni₃TeO₆ (NTO) structure was computationally predicted and its stacked 2D nanosheets experimentally synthesized. Theoretical design undergoes featuring coordination of metalloid chalcogen, slicing the bulk structure, geometrical optimizations and stability study. The predicted layered NTO structure is realized in nanometer-thick nanosheets via a one-pot shape-controlled hydrothermal synthesis. Compared to the bulk, the 2D NTO own a lowered bandgap energy, more sensitive wavelength selectivity and an emerging photocatalytic hydrogen evolution ability under visible light. Beside a new 2D NTO with the optoelectrical and photocatalytic merits, its existing polar space group, structural specification, and design route are hoped to benefit 2D semiconductor innovations both in species enrichment and future applications.

当前二维 (2D) 材料探索的进展导致可能的先进材料不断富集到二维。基于金属硫族化物的二维材料是有前景的领域，许多邻近领域有待探索。这里，稳定的单层 Ni ₃ TeO ₆（NTO）结构通过计算预测，并通过实验合成其堆叠的二维纳米片。理论设计经历了非金属硫属元素的配位、块体结构切片、几何优化和稳定性研究。通过一锅形状控制水热合成，在纳米厚的纳米片中实现了预测的层状 NTO 结构。与块体相比，2D NTO 具有更低的带隙能量、更灵敏的波长选择性以及在可见光下新兴的光催化析氢能力。除了具有光电和光催化优点的新型二维NTO之外，其现有的极性空间群、结构规格和设计路线有望有利于二维半导体在物种富集和未来应用方面的创新。