Ultrahigh Single Au Atoms Loaded Porous Aromatic Frameworks for Enhanced Photocatalytic Hydrogen Evolution

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Supported single-atom catalysts (SACs) offer high atom economy and mechanistic clarity in heterogeneous catalysis.
• Current limitations in SACs include restricted metal single-atom (SA) loading, hindering catalytic efficiency.

Purpose of the Study:

• To develop a novel strategy for achieving ultrahigh loading of gold single-atom catalysts (SACs).
• To synthesize a new porous aromatic framework (PAF) material with exceptionally high gold SA loading.
• To evaluate the photocatalytic performance of the synthesized gold SACs for hydrogen evolution.

Main Methods:

• An in situ pre-metallated monomer-based preparation strategy was employed.
• Polymerization of single-atom loaded monomers to form a porous aromatic framework (PAF-164).
• Characterization of the material and assessment of its photocatalytic activity for hydrogen (H2) evolution.

Main Results:

• Achieved a record-high gold single-atom loading of 45.3 wt.% in the synthesized PAF-164.
• The resulting gold SACs (Au-PAFs) demonstrated excellent photocatalytic activity for H2 evolution.
• The H2 evolution rate reached 4.82 mmol g-1 h-1 with remarkable recyclability.

Conclusions:

• The in situ pre-metallated monomer strategy enables ultrahigh gold SA loading in PAFs.
• Gold SACs based on PAF-164 show significant potential for efficient photocatalytic hydrogen production.
• This approach overcomes limitations in SA loading for enhanced catalytic applications.