Qian Haixia, Huang Nanjun, Zheng Jinhong, An Zhenchao, Yin Xiaoshuang, Liu Ying, Yang Wenzhong, Chen Yun
School of Chemistry and Molecular Engineering, Nanjing Tech University, No. 30 Puzhu Road (S), Nanjing 211816, China.
School of Chemistry and Molecular Engineering, Nanjing Tech University, No. 30 Puzhu Road (S), Nanjing 211816, China.
J Colloid Interface Sci. 2021 Oct;599:100-108. doi: 10.1016/j.jcis.2021.04.052. Epub 2021 Apr 14.
Modification of MoS-based catalysts is effective in solving the overdependence of hydrogen evolution reactions (HERs) on noble metal catalysts. In this work, a Zn-doped molybdenum disulfide-reduced graphene oxide (Zn-MoS-RGO) hybrid was synthesized in one step employing a hydrothermal method. By substituting the position of Mo, uniform doping with Zn improved the catalytic activity of MoS for HER. The interlayer spacing of MoS increased from 0.65 to 0.75 nm, demonstrating RGO effectively interpolate into MoS nanosheets. This prevented aggregation and exposed more edge active sites of MoS. According to density functional theory (DFT) calculations, the layered structure of the MoS nanosheets doped with Zn and intercalated with RGO promoted charge transfer and resulted in outstanding hydrogen evolution activity. Compared with MoS (6.86 eV), the Zn-MoS-RGO hybrid (5.47 eV) with a considerably lower energy level value exhibited excellent electrocatalytic performance. Under optimal conditions, at a potential of -0.3 V vs. RHE, the current density reached -169 mA cm in a 0.5 M HSO solution, 4.78 μmol of H was produced in 6 h, and the Faraday efficiency reached 92%. The results obtained herein indicated that Zn-MoS-RGO was a promising candidate for application in electrocatalytic HER.
基于二硫化钼的催化剂改性对于解决析氢反应(HERs)对贵金属催化剂的过度依赖是有效的。在这项工作中,采用水热法一步合成了锌掺杂的二硫化钼-还原氧化石墨烯(Zn-MoS-RGO)杂化物。通过取代钼的位置,锌的均匀掺杂提高了二硫化钼对析氢反应的催化活性。二硫化钼的层间距从0.65纳米增加到0.75纳米,表明氧化石墨烯有效地插入到二硫化钼纳米片中。这防止了团聚并暴露了更多二硫化钼的边缘活性位点。根据密度泛函理论(DFT)计算,掺杂锌并插入氧化石墨烯的二硫化钼纳米片的层状结构促进了电荷转移,并产生了出色的析氢活性。与二硫化钼(6.86电子伏特)相比,能级值低得多的Zn-MoS-RGO杂化物(5.47电子伏特)表现出优异的电催化性能。在最佳条件下,相对于可逆氢电极(RHE),在-0.3伏的电位下,在0.5 M硫酸溶液中的电流密度达到-169毫安/平方厘米,6小时内产生了4.78微摩尔的氢气,法拉第效率达到92%。本文获得的结果表明,Zn-MoS-RGO是用于电催化析氢反应的有前途的候选材料。