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<p>The research examines Au@MoS₂ core–shell nanostructures as excellent photoelectrocatalysts for hydrogen-evolving reactions (HER) by highlighting the importance of the MoS₂ shell’s thickness. Analysis by TEM and XRD verified that the fabricated nanoparticles had defined Au inner regions (around 20–30&#xa0;nm), the following layer of MoS₂ could be regulated (from 1.3 to 3.6&#xa0;nm), and these features were separated by an epitaxial interface and very pure phases. It was found that the LSPR peak was shifted from 528&#xa0;nm to 535–545&#xa0;nm and the MoS₂ Raman spacing measured between 19 and 23&#xa0;cm⁻<sup>1</sup>, establishing that the shell had around 2–6 layers. The time taken for the hot electrons to move and relax was found to be very short in S1 by ultrafast transient absorption spectroscopy, which means that charge transfer was very effective. The testing showed that, among all nanocatalysts, S1 had the oldest best performance during HER, as shown by a very low starting potential (− 0.11&#xa0;V vs RHE), Tafel slope (54&#xa0;mV/dec), and greatest current density (10.2&#xa0;mA/cm<sup>2</sup> at − 0.3&#xa0;V), which was made possible by the minimum resistance found by EIS. DFT simulation matched the experimental results, proving 0.25&#xa0;eV for the Schottky barrier height and almost 83% efficiency for injecting electrons in 2-layer MoS₂ structures. All in all, the research shows that careful adjustment of the MoS₂ shell thickness is necessary for achieving the highest plasmonic gain and best catalytic activity in Au@MoS₂ structures.</p>

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Ultrafast Hot Carrier Injection in Core–Shell Au@MoS₂ Systems for Plasmonic-Assisted Hydrogen Evolution

  • 期刊论文

  • 发表日期：

    2025年7月31日

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  • Rishab Chaturvedi,
  • N. Nagabhooshanam,
  • Prahalad Singh Parihar,
  • Navin Kedia,
  • Jemmy Christy H.,
  • G. Satya,
  • A. Rajaram

摘要

The research examines Au@MoS₂ core–shell nanostructures as excellent photoelectrocatalysts for hydrogen-evolving reactions (HER) by highlighting the importance of the MoS₂ shell’s thickness. Analysis by TEM and XRD verified that the fabricated nanoparticles had defined Au inner regions (around 20–30 nm), the following layer of MoS₂ could be regulated (from 1.3 to 3.6 nm), and these features were separated by an epitaxial interface and very pure phases. It was found that the LSPR peak was shifted from 528 nm to 535–545 nm and the MoS₂ Raman spacing measured between 19 and 23 cm⁻1, establishing that the shell had around 2–6 layers. The time taken for the hot electrons to move and relax was found to be very short in S1 by ultrafast transient absorption spectroscopy, which means that charge transfer was very effective. The testing showed that, among all nanocatalysts, S1 had the oldest best performance during HER, as shown by a very low starting potential (− 0.11 V vs RHE), Tafel slope (54 mV/dec), and greatest current density (10.2 mA/cm2 at − 0.3 V), which was made possible by the minimum resistance found by EIS. DFT simulation matched the experimental results, proving 0.25 eV for the Schottky barrier height and almost 83% efficiency for injecting electrons in 2-layer MoS₂ structures. All in all, the research shows that careful adjustment of the MoS₂ shell thickness is necessary for achieving the highest plasmonic gain and best catalytic activity in Au@MoS₂ structures.