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Toward Quantum Confinement in Graphitic Carbon Nitride-Based Polymeric Monolayers.

Olatunde P Olademehin¹, Thomas L Ellington¹, Kevin L Shuford¹

¹Department of Chemistry and Biochemistry, Baylor University, One Bear Place #97348, Waco, Texas 76798-7348, United States.

The Journal of Physical Chemistry. A

|August 30, 2021

Summary

Graphitic carbon nitride (g-C3N4) quantum dots show promise as metal-free photocatalysts. Their optical gap increases with size reduction below specific thresholds, with nitrogen and carbon sites identified for water splitting and doping.

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Preparation of Carbon Nanosheets at Room Temperature

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Area of Science:

Materials Science
Photocatalysis
Quantum Chemistry

Background:

Graphitic carbon nitride (g-C3N4) is a promising metal-free photocatalyst.
Understanding the size-dependent properties of g-C3N4 is crucial for optimizing its performance.
Quantum dots and clusters of g-C3N4 are being explored to mimic extended monolayers.

Purpose of the Study:

To systematically investigate the structural, electronic, and optical properties of g-C3N4 building blocks.
To determine the critical sizes for observing quantum confinement effects in g-C3N4.
To identify active sites for photocatalysis and chemical modification.

Main Methods:

Density functional theory (DFT) calculations.
Bottom-up construction of polymeric g-C3N4 monolayers from melamine and heptazine units.
Analysis of electronic transitions using full natural transition orbital (NTO) and density of states (DOS).

Main Results:

Melamine-based g-C3N4 requires reduction to <2.74 nm, and heptazine-based to <4.00 nm, for optical gap increase with size reduction.
Electronic transitions and their nature were analyzed.
Nitrogen and carbon atoms were identified as preferential sites for water splitting and chemical doping, respectively.

Conclusions:

Size-dependent properties of g-C3N4 quantum dots and clusters are critical for photocatalytic applications.
DFT provides insights into the electronic structure and optical properties of g-C3N4.
Specific sites on g-C3N4 offer potential for targeted functionalization and enhanced catalytic activity.