Key Laboratory for Soft Chemistry and Functional Materials, Ministry of Education, Nanjing University of Science and Technology, Nanjing 210094, China.
Nanoscale. 2018 Jan 25;10(4):1766-1773. doi: 10.1039/c7nr07213a.
The exploration of highly active catalysts for hydrogen evolution reaction (HER) is beneficial to realize high catalytic activity and enhance kinetics for water splitting. Herein, flower-like molybdenum disulfide/carbon nitride (MoS/CN) nanosheets with thickness of 4.6 nm and enlarged interlayer spacing of 0.64 nm were synthesized via a facile hydrothermal method. As expected, the ultrathin thickness endowed MoS/CN with abundant active sites, ensuring outstanding catalytic activity and excellent stability for HER in alkaline electrolyte. MoS/CN nanocomposites can offer an onset overpotential of 153 mV versus reversible hydrogen electrode (RHE). Notably, the Tafel slope value is only 43 mV dec, which is significantly better than those of reported MoS-based hydrogen evolution catalysts, revealing superior HER performance of MoS/CN, particularly in catalytic kinetics. More significantly, density functional theory (DFT) calculations further verify that rich active sites confined in ultrathin nanostructure of g-CN nanolayers could increase the activity of MoS/CN and result in enhanced HER efficiency. This study indicates that rational interaction between two different 2D materials can significantly facilitate H generation, which endows extraordinary HER activity.
探索具有高效析氢反应(HER)活性的催化剂有利于实现高催化活性和增强水分解动力学。在此,通过简便的水热法合成了具有 4.6nm 厚度和 0.64nm 增大层间距的花状二硫化钼/氮化碳(MoS/CN)纳米片。正如预期的那样,超薄厚度赋予了 MoS/CN 丰富的活性位点,确保了其在碱性电解质中对 HER 具有出色的催化活性和优异的稳定性。MoS/CN 纳米复合材料可以提供 153mV 相对于可逆氢电极(RHE)的起始过电势。值得注意的是,Tafel 斜率值仅为 43mV dec,明显优于已报道的基于 MoS 的析氢催化剂,表明 MoS/CN 具有优异的 HER 性能,特别是在催化动力学方面。更重要的是,密度泛函理论(DFT)计算进一步验证了富活性位点被限制在 g-CN 纳米层的超薄纳米结构中,可以提高 MoS/CN 的活性,从而提高 HER 效率。本研究表明,两种不同二维材料之间的合理相互作用可以显著促进 H 的生成,从而赋予其非凡的 HER 活性。