Pentagonal PdTe2 Monolayer for Sustainable Solar-driven Hydrogen Production

TL;DR

This study shows that strained pentagonal PdTe2 monolayers are highly effective 2D photocatalysts for solar-driven hydrogen production, with tunable bandgaps and high efficiency exceeding previous catalysts.

Contribution

The paper introduces strain-engineered pentagonal PdTe2 monolayers as a novel, highly efficient 2D photocatalyst for water splitting, demonstrating superior performance through theoretical calculations.

Findings

Strain tuning enables spontaneous water splitting in penta-PdTe2.

Achieved a solar-to-hydrogen efficiency of 20.40%.

Overpotentials for HER and OER are minimized at +3% tensile strain.

Abstract

This investigation demonstrates that the pentagonal PdTe2 (penta-PdTe2) monolayer is a highly tunable two-dimensional (2D) photocatalyst, characterized by the bandgap of 1.75 eV and high hole mobility. Using density functional theory calculations with the HSE06 functional, we show that tensile strain engineering (particularly at +2% and +3%) is essential for enabling spontaneous water splitting. At these strain values, the valence-band maximum and conduction-band maximum straddle the water redox potentials (H+/H2 and O2/H2O) in both acidic (pH=0) and neutral (pH=7) conditions. The monolayer's low hole effective mass facilitates rapid charge extraction, mitigating recombination and driving the oxygen evolution reaction (OER) more effectively than many hexagonal and pentagonal counterparts. The Gibbs free energy ({\Delta}G) pathways indicate that overpotentials for the hydrogen evolution reaction (HER) and OER are highly sensitive to mechanical deformation, specifically biaxial strain, through which +3% tensile strain, yielding an optimized balance of overpotentials of {\eta}HER = 0.70 V and {\eta}OER = 0.72 V at pH=7. Finally, integrating optical absorption with thermodynamic driving forces results in a Solar-to-Hydrogen (STH) efficiency of 20.40% at pH 7. This exceeds the performance of several previously reported 2D catalysts, positioning penta-PdTe2 as a superior candidate for sustainable, solar-driven hydrogen production.