MoS₂-supported gold nanoparticle for CO hydrogenation.

Area of Science:

• Computational materials science
• Surface chemistry
• Catalysis

Background:

• Gold nanoparticles (Au NPs) are crucial catalysts, but their performance is highly dependent on support interactions.
• Molybdenum disulfide (MoS2) is a promising 2D material for catalysis, especially when engineered with defects.
• Understanding the interplay between Au NPs and MoS2 supports is key to designing efficient catalytic systems.

Purpose of the Study:

• To investigate the structural, electronic, and reactivity changes of a 13-atom gold nanoparticle (Au13) supported on defect-laden single-layer MoS2.
• To elucidate the charge transfer mechanisms and identify catalytically active sites.
• To evaluate the potential of the Au13/MoS2 system for methanol synthesis.

Main Methods:

• Dispersion-corrected density functional theory (DFT) calculations were employed.
• Analysis of geometric structure, electronic band structure, and charge distribution.
• Comparison of reactivity with other supported gold systems, such as Au13/TiO2.

Main Results:

• The planar Au13 structure transforms into a 3D structure upon support on MoS2.
• Charge transfer occurs from MoS2 to Au13, with electron density redistribution away from the interface.
• Au sites distant from the interface become catalytically active, with narrower Au d states and frontier states near the Fermi level.

Conclusions:

• Defect-laden MoS2 significantly alters the properties of supported Au13 nanoparticles.
• The Au13/MoS2 system demonstrates high activity for methanol synthesis through CO hydrogenation, contrasting with methanol decomposition activity on Au13/TiO2.
• This work highlights the potential of engineered MoS2 supports for tuning gold nanoparticle catalysis.