Two-dimensional Pd₃(AsSe₄)₂ as a photocatalyst for the solar-driven oxygen evolution reaction: a first-principles...

Area of Science:

• Materials Science
• Condensed Matter Physics
• Computational Chemistry

Background:

• The structure-property relationship is central to materials research.
• Previous work focused on bulk and 2D layered materials like Pd3(PS4)2.
• Exploration of similar 2D materials is inspired by prior successes.

Purpose of the Study:

• To investigate novel two-dimensional (2D) Pd3(AsX4)2 materials (X = S, Se, Te) using first-principles calculations.
• To determine their electronic, optical, and catalytic properties.
• To assess their potential for photocatalysis and water splitting.

Main Methods:

• Density Functional Theory (DFT) calculations with the HSE06 hybrid functional.
• Electronic band structure and carrier mobility calculations.
• Optical property analysis and reaction mechanism investigation.

Main Results:

• Pd3(AsS4)2 and Pd3(AsSe4)2 monolayers are identified as indirect semiconductors with HSE06 band gaps of 2.37 eV and 1.36 eV, respectively.
• These materials exhibit superior carrier mobilities (523.23 cm2 V-1 s-1 and 440.6 cm2 V-1 s-1) compared to MoS2.
• Pd3(AsSe4)2 shows suitable band edge positions for visible-light water splitting and efficient oxygen evolution at 0.14 V.

Conclusions:

• The synthesized 2D Pd3(AsX4)2 materials possess excellent semiconductor properties and high carrier mobilities.
• Pd3(AsSe4)2 demonstrates significant potential for efficient solar-driven water splitting and oxygen evolution reactions.
• The mechanistic understanding may guide the design of advanced photocatalysts for practical applications.