State Key Laboratory of Analytical Chemistry for Life Science and Collaborative Innovation Center of Chemistry for Life Sciences, School of Chemistry and Chemical Engineering, Nanjing University, 22 Hankou Road, Nanjing 210093, China.
J Am Chem Soc. 2015 Jun 17;137(23):7365-70. doi: 10.1021/jacs.5b01732. Epub 2015 Jun 8.
Efficient water splitting through electrocatalysis holds great promise for producing hydrogen fuel in modern energy devices. Its real application however suffers from sluggish reaction kinetics due to the lack of high-performance catalysts except noble metals such as platinum. Herein, we report an active system of plasmonic-metal Au nanorods/molybdenum disulfide (MoS2) nanosheets hybrids for the hydrogen evolution reaction (HER). The plasmonic Au-MoS2 hybrids dramatically improve the HER, leading to a ∼3-fold increase of current under excitation of Au localized surface plasmon resonance (LSPR). A turnover of 8.76 s(-1) at 300 mV overpotential is measured under LSPR excitation, which by far exceeds the activity of MoS2 catalysts reported recently. The HER enhancement can be largely attributed to the increase of carrier density in MoS2 induced by the injection of hot electrons of Au nanorods. We demonstrate that the synergistic effect of the hole scavengers can further facilitate electron-hole separation, resulting in a decrease of the overpotential of HER at MoS2 to ∼120 mV. This study highlights how metal LSPR activates the HER and promises novel opportunities for enhancing intrinsic activities of semiconducting materials.
通过电催化实现高效水分解有望在现代能源设备中生产氢气燃料。然而，除了贵金属如铂之外，由于缺乏高性能催化剂，其实际应用受到反应动力学缓慢的限制。在此，我们报告了一种等离子体金属 Au 纳米棒/二硫化钼（MoS2）纳米片杂化用于析氢反应（HER）的活性体系。等离子体 Au-MoS2 杂化极大地提高了 HER，在 Au 局域表面等离子体共振（LSPR）激发下导致电流增加约 3 倍。在 LSPR 激发下，在 300 mV 过电势下测量到 8.76 s(-1)的周转率，这远远超过了最近报道的 MoS2 催化剂的活性。HER 增强可归因于 Au 纳米棒注入的热电子引起的 MoS2 中载流子密度的增加。我们证明了空穴清除剂的协同效应可以进一步促进电子-空穴分离，导致 MoS2 上 HER 的过电势降低到约 120 mV。这项研究强调了金属 LSPR 如何激活 HER，并为增强半导体材料的本征活性提供了新的机会。
