Construction and Microenvironment Regulation of Short Charge Transfer Tunnel at MOF/COF Heterointerfaces for...

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Improving electron transfer efficiency is vital for enhancing photocatalytic productivity.
• Developing short-distance electron transport pathways is key to efficient photocatalysis.

Purpose of the Study:

• To propose a strategy for anchoring single atoms and establishing short-distance electron transport pathways.
• To investigate the role of functional groups in regulating electron transfer and photocatalytic activity.

Main Methods:

• Incorporating nitrogen-containing monodentate ligands into UIO-66-NH2 to co-anchor Pt single atoms.
• Condensing Pt-containing UIO with TpPa-1 to establish a molecular-level electron transfer pathway.
• Adjusting functional group positions (-H, -Cl, -OCH3) on ligands to regulate electron relay effects.

Main Results:

• A molecular-level electron transfer pathway from TpPa to Pt was established at the heterointerface.
• Functional groups at the ortho-position of the amino group acted as effective electron relays.
• UPT-o-Cl achieved a maximum H2 yield of 14.21 mmol g-1 h-1, demonstrating superior performance.

Conclusions:

• The strategy precisely regulates the microenvironment adjacent to active sites, enhancing carrier mobility and utilization.
• Functional group positioning is crucial for optimizing electron transfer and photocatalytic efficiency.
• This work provides new insights into designing advanced photocatalysts for efficient hydrogen production.