Department of Materials, University of Oxford , Parks Road, Oxford OX1 3PH, U.K.
ACS Appl Mater Interfaces. 2018 Feb 7;10(5):4630-4639. doi: 10.1021/acsami.7b14861. Epub 2018 Jan 23.
The edge sites of MoS are catalytically active for the hydrogen evolution reaction (HER), and growing monolayer structures that are edge-rich is desirable. Here, we show the production of large-area highly branched MoS dendrites on amorphous SiO/Si substrates using an atmospheric pressure chemical vapor deposition and explore their use in electrocatalysis. By tailoring the substrate construction, the monolayer MoS evolves from triangular to dendritic morphology because of the change of growth conditions. The rough edges endow dendritic MoS with a fractal dimension down to 1.54. The highly crystalline basal plane and the edge of the dendrites are visualized at atomic resolution using an annular dark field scanning transmission electron microscope. The monolayer dendrites exhibit strong photoluminescence, which is indicative of the direct band gap emission, which is preserved after being transferred. Post-transfer sulfur annealing restores the structural defects and decreases the n-type doping in MoS monolayers. The annealed MoS dendrites show good and highly durable HER performance on the glassy carbon with a large exchange current density of 32 μA cm, demonstrating its viability as an efficient HER catalyst.
边缘位点的 MoS 对析氢反应(HER)具有催化活性,因此希望生长富含边缘的单层结构。在这里,我们使用常压化学气相沉积法在非晶硅/硅衬底上制备大面积高度分支的 MoS 树枝状结构,并探索其在电催化中的应用。通过调整衬底结构,由于生长条件的变化,单层 MoS 从三角形演变为树枝状形态。粗糙的边缘使树枝状 MoS 的分形维数降至 1.54。使用环形暗场扫描透射电子显微镜以原子分辨率可视化高度结晶的基面和树枝的边缘。单层树枝状结构表现出强烈的光致发光,这表明其具有直接带隙发射,在转移后得以保留。转移后硫退火可以恢复结构缺陷并降低 MoS 单层中的 n 型掺杂。经过退火处理的 MoS 树枝状结构在玻璃碳上表现出良好且高度持久的 HER 性能,交换电流密度大到 32 μA cm,表明其作为高效 HER 催化剂的可行性。