College of Chemistry and Environmental Engineering , Shenzhen University , 1066 Xueyuan Avenue , Nanshan District, Shenzhen 518071 , PR China.
School of Materials Science and Engineering , Nanyang Technological University , 50 Nanyang Avenue , 639798 , Singapore.
ACS Appl Mater Interfaces. 2018 Jul 18;10(28):23731-23739. doi: 10.1021/acsami.8b04140. Epub 2018 Jul 6.
In this work, MoS-based hybrid tubular nanostructures are facilely synthesized via a self-assembly-assisted process and evaluated as a bifunctional electrocatalyst for hydrogen evolution reactions (HERs) and oxygen reduction reactions (ORRs). By simply mixing the reactants under ambient conditions, (NH)MoS/polydopamine (PDA) hybrid nanospheres are formed. The protonated dopamine is linked to tetrahedral [MoS] via weak N-H···S and O-H···S interactions, causing the PDA nanospheres merging together and forming nanorods under stirring-induced shear force. Moreover, the oxidative polymerization of dopamine proceeds on the surface of the nanorods, whereas it is prohibited inside the nanorods owing to lack of oxygen, leading to outward diffusion of dopamine and hence cavitation. After annealing, the tubular morphology is perfectly retained, while ultrafine MoS monolayers are formed due to the confinement of the framework. Benefiting from these unique structural features, the MoS/C hybrid nanotubes possess abundant active sites and high surface area, as well as boost electronic and ionic transport, remarkably enhancing their electrocatalytic activities. The onset and half-wave potentials are 0.91 and 0.82 V, respectively, for ORR, close to those of Pt/C. Moreover, low onset potential and small Tafel slope are also observed for HER, demonstrating the potential of the hybrid nanotubes as a promising non-noble metal bifunctional electrocatalyst.
在这项工作中,通过自组装辅助工艺,简便地合成了基于 MoS 的混合管状纳米结构,并将其评估为用于析氢反应 (HERs) 和氧还原反应 (ORRs) 的双功能电催化剂。通过在环境条件下简单混合反应物,形成(NH)MoS/聚多巴胺(PDA)混合纳米球。质子化的多巴胺通过弱 N-H···S 和 O-H···S 相互作用与四面体[MoS]相连,导致 PDA 纳米球在搅拌诱导的剪切力下融合在一起并形成纳米棒。此外,多巴胺的氧化聚合在纳米棒表面进行,而由于缺乏氧气,在纳米棒内部被禁止,导致多巴胺向外扩散并因此空化。退火后,管状形态完美保留,而由于框架的限制,形成了超细的 MoS 单层。得益于这些独特的结构特征,MoS/C 混合纳米管具有丰富的活性位点和高表面积,以及促进电子和离子传输,显著提高了它们的电催化活性。ORR 的起始电位和半波电位分别为 0.91 和 0.82 V,接近 Pt/C。此外,HER 还表现出低的起始电位和小的塔菲尔斜率,这表明混合纳米管作为一种有前途的非贵金属双功能电催化剂的潜力。