Liu Zhong-Liu, Lei Bao, Zhu Zhi-Li, Tao Lei, Qi Jing, Bao De-Liang, Wu Xu, Huang Li, Zhang Yu-Yang, Lin Xiao, Wang Ye-Liang, Du Shixuan, Pantelides Sokrates T, Gao Hong-Jun
Institute of Physics and University of Chinese Academy of Sciences , Chinese Academy of Sciences , Beijing 100190 , China.
Department of Physics and Astronomy , Vanderbilt University , Nashville , Tennessee 37235 , United States.
Nano Lett. 2019 Aug 14;19(8):4897-4903. doi: 10.1021/acs.nanolett.9b00889. Epub 2019 Apr 15.
Creation of functional patterns in two-dimensional (2D) materials provides opportunities to extend their potential for applications. Transition-metal dichalcogenides (TMDCs) are suitable 2D materials for pattern generation because of properties including alterable polymorphic phases, easy chalcogen-vacancy formation, metal-atom insertion, and alloying. Such patterning can be used for selective functionalization. Here we report the spontaneous formation of long-range, well-ordered 1D patterns in monolayer vanadium diselenide (VSe) by a single annealing stage during growth. Atomic-resolution images in real space combined with density-functional-theory (DFT) calculations reveal the 1D features of patterned VSe. Further experimental characterization of the intermediate states in the growth process confirm the spontaneous formation of the 1D pattern by annealing-induced Se-deficient linear defects. The 1D pattern can be reversibly transformed to homogenous VSe monolayer by reintroducing Se atoms. Moreover, additional experiments demonstrate that a dispersive deposition of Pt atoms along the 1D structures of patterned VSe is achieved, while DFT calculations find that their catalytic activity for hydrogen evolution reaction (HER) is as good as that of Pt surfaces. The formation of long-range, well-ordered 1D patterns not only demonstrates an effective way of dimension modulation in 2D materials but also enriches the potential of intrinsically patterned 2D materials for promising catalytic activities.
在二维(2D)材料中创建功能图案为扩展其应用潜力提供了机会。过渡金属二硫属化物(TMDCs)是适用于图案生成的二维材料,因为其具有包括可变多晶型相、易于形成硫属元素空位、金属原子插入和合金化等特性。这种图案化可用于选择性功能化。在此,我们报告了在单层二硒化钒(VSe)生长过程中通过单一退火阶段自发形成长程、有序的一维图案。实空间中的原子分辨率图像与密度泛函理论(DFT)计算揭示了图案化VSe的一维特征。对生长过程中中间态的进一步实验表征证实了通过退火诱导的缺硒线性缺陷自发形成一维图案。通过重新引入硒原子,一维图案可以可逆地转变为均匀的VSe单层。此外,额外的实验表明,实现了铂原子沿图案化VSe的一维结构的分散沉积,而DFT计算发现它们对析氢反应(HER)的催化活性与铂表面相当。长程、有序的一维图案的形成不仅展示了二维材料中尺寸调制的有效方法,也丰富了具有本征图案的二维材料在有前景的催化活性方面的潜力。