Two-dimensional semiconductive Ni3TeO6: from theoretical prediction to shape-controlled synthesis Javier Fernández-Catalá 1 , 2 , Andrey A. Kistanov 1 , Yang Bai 3 , Harishchandra Singh 1 , Wei Cao 1 1 Nano and Molecular Systems Research Unit, University of Oulu, Finland 2 Inorganic Chemistry Department, Materials Science Institute, University of Alicante, Spain 3 Microelectronics Research Unit, University of Oulu Current progress in two-dimensional (2D) materials explorations leads to constant specie enrichments of possible advanced materials down to two dimensions1. The metal chalcogenide-based 2D materials are promising grounds where many adjacent territories are waiting to be explored2. In this work, 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 stabilities of optimized structures are assessed by lattice vibration in the output of phonon frequencies, indicating that the NTO material is stable in 2D. XRD result indicates that the single-phased NTO is synthesised successfully. The TEM analyse confirms the nanosheet morphology with a tich of 4.6 nm of 2D NTO samples. The XRD and TEM confirm the successful synthesis of novel NTO nanosheet material. Compared to the bulk (2.55 eV), the 2D NTO own a lowered bandgap energy (2.17 eV). The electronic structure and low-dimensional feature of the 2D NTO denotes possible differences of electric properties compared to these of the bulk form. The 2D NTO nanosheets are found photocatalytically active in hydrogen evolution reaction under visible light irradiation. An HER rate of 3.3 ± 0.3 µmol/g/h is obtained under low-power white LED irradiation (nominal power of 0.495 W) without any co-catalysts or scavenger with respect to the inactive bulk NTO. The activity of the photocatalyst does not decrease after ten cycles, indicating that 2D-NTO system is stable under condition of reaction. In conclusion, a new, stable and semiconductive 2D material of Ni3TeO6 in the morphology of nanosheets was invented for the first time. The DFT-predicted 2D slab, sliced from the bulk counterpart in the metal tellurate family, was experimentally synthesized and proved stable. The pristine 2D NTO nanosheets are found photocatalytically active in hydrogen evolution reaction without co-catalyst and scavenger under visible light. Along with potential utilities in the photocatalysis and electronics of the invented material itself, this work is hoped to debut explorations and realizations of 2D tellurates for various applications. The route combining computational prediction and experimental realizations is also hoped to inspire the enrichment of 2D materials library. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 101002219). JFC thanks European Union-Next Generation EU, MINECO, and University of Alicante for a postdoctoral researcher grant References 1. Manzeli, S. et al. Nat. Rev. Mater. 2017, 2, 17033. 2. Jiao, Y. et al. ACS Appl. Mater. Interfaces 2016, 8, 5385.
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