Catechol Sensing Performance of Pd-Functionalized Two-Dimensional Polyaramid: A DFT Investigation

Area of Science:

• Materials Science
• Surface Chemistry
• Computational Chemistry

Background:

• Catechol (Cc) molecule detection is crucial for environmental and industrial monitoring.
• Pristine two-dimensional polyaramid (2DPA) exhibits weak adsorption and charge transfer with Cc, limiting its sensing potential.
• Transition metal (TM) functionalization is explored to enhance the adsorption and sensing properties of 2DPA.

Purpose of the Study:

• To systematically investigate catechol adsorption on pristine and TM-functionalized 2DPA using first-principles calculations.
• To identify the optimal TM for enhancing Cc adsorption and sensing capabilities of 2DPA.
• To evaluate the electronic, optical, and structural properties of the functionalized material for sensor applications.

Main Methods:

• First-principles density functional theory (DFT) calculations were employed to study Cc adsorption.
• Ab initio molecular dynamics simulations were performed to assess structural stability at 300 K.
• Analysis included adsorption energy, charge transfer, band gap changes, work function, optical properties, and diffusion energy barriers.

Main Results:

• Pristine 2DPA showed weak Cc physisorption (-0.29 eV) with a fast recovery time (150 μs), unsuitable for sensing.
• Palladium (Pd)-functionalized 2DPA demonstrated superior Cc adsorption (-1.39 eV) with significant charge transfer, indicating enhanced sensitivity.
• Pd-functionalized 2DPA exhibited stable electronic and optical property changes upon Cc adsorption, with efficient desorption under visible/UV light and no Pd atom diffusion.

Conclusions:

• Pd-functionalized 2DPA is a promising material for developing next-generation catechol sensors due to its enhanced adsorption and sensing capabilities.
• The study provides a theoretical foundation for designing high-performance sensors for catechol molecule detection.
• The material's stability and tunable electronic/optical properties make it suitable for practical sensor applications.