Regulating Atomically-Precise Pt Sites for Boosting Light-Driven Dry Reforming of Methane

Area of Science:

• Materials Science
• Catalysis
• Renewable Energy

Background:

• Light-driven dry reforming of methane offers a mild pathway to convert greenhouse gases (methane and carbon dioxide) into valuable syngas.
• Achieving precise control over active catalyst sites and ensuring stable syngas production remain significant challenges.

Purpose of the Study:

• To develop a strategy for atomically precise regulation of platinum species on TiO2 surfaces.
• To investigate the impact of single atoms and nanoclusters on catalytic activity and syngas production.

Main Methods:

• Spatial confinement approach to control platinum species (single atoms to nanoclusters) on TiO2.
• Characterization of electronic metal-support interactions and interfacial states.
• Evaluation of catalytic performance in light-driven dry reforming of methane.

Main Results:

• The catalyst configuration with single atoms and sub-nanoclusters demonstrated strong electronic metal-support interactions and surface charge rearrangement.
• The unique properties of the atom-cluster assemblies facilitated efficient activation of methane and carbon dioxide, promoting intermediate coupling and reducing side reactions.
• An outstanding syngas generation rate of 34.41 mol gPt-1 h-1, high apparent quantum yield (9.1% at 365 nm), and turnover frequency (1289 h-1) were achieved with superior durability.

Conclusions:

• The spatial confinement approach enables precise control over platinum species, leading to enhanced catalytic performance.
• Atomically precise catalyst design is crucial for optimizing syngas production via light-driven dry reforming.
• This work provides a foundation for designing advanced multi-component catalysts at the atomic scale.