Interface Electronic Microenvironment Engineering in Pt@UiO-66 Composites for Regulating Interfacial Charge Transfer...

Area of Science:

• Materials Science
• Nanotechnology
• Electrochemistry

Background:

• Interface electronic microenvironment engineering is crucial for nanocomposite functionality.
• Tuning interfacial charge transfer and molecular recognition requires precise control over the local chemical environment.

Purpose of the Study:

• To develop a mechanism-guided interface engineering approach for Pt@UiO-66-X composites.
• To investigate the effect of linker functionalization on the electronic and chemical properties of the interface.
• To enhance molecular recognition and electrocatalytic activity in MOF-based nanocomposites.

Main Methods:

• Synthesis of core-shell Pt@UiO-66-X composites with varying linker functionalization (X = H, NH2, SO3H).
• Experimental characterization including adsorption studies and electrochemical measurements.
• Qualitative density functional theory (DFT) calculations to understand electronic and bonding interactions.

Main Results:

• The NH2-functionalized UiO-66 framework creates an electron-rich environment and a multipoint hydrogen-bonding network.
• This configuration significantly enhances ascorbic acid (AA) adsorption and recognition.
• The NH2-functionalized composite demonstrates improved charge transfer, superior electrocatalytic response, and reliable operational stability compared to other functionalized variants.

Conclusions:

• Linker electronic properties critically influence adsorption, molecular recognition, and electrochemical performance in Pt@MOF composites.
• The developed interface engineering strategy offers a potentially generalizable approach for designing advanced MOF-based interfacial systems.
• This work provides mechanistic insights into optimizing nanocomposite functionality through precise control of the interfacial microenvironment.