Computational Study of Water Adsorption and Dissociative Mechanisms Impacting g-C3N4's Optical and Electronic Properties

Abstract

In the quest for sustainable energy solutions, water splitting emerges as a crucial process for generating clean hydrogen a versatile and renewable fuel essential for energy storage, emissions reduction, and achieving sustainability goals. This study employs a comprehensive computational approach, utilizing atomistic simulations to systematically investigate the effects of water absorption on the electronic and optical properties of g-C3N4 nanosheets. Our methodology integrates ab initio computations grounded in density functional theory (DFT), which allows for a detailed characterization of the nanosheet and serves as a benchmark for self-consistent charge density functional tight binding (SCC-DFTB) simulations. This approach provides valuable insights into the behavior of the nanosheet under the influence of absorbed OH and H2O molecules by considering calculated parameters for photocatalytic efficiency. Additionally, we extend our investigation to classical molecular dynamics simulations within the ReaxFF framework, modeling the emission of multiple H2O molecules and assessing the subsequent rate of H2 evolution. A key finding of our study reveals that the dissociation of H2O into HO and O molecules significantly enhances both the optical absorbance and conductance of the nanosheet compared to its pristine state. These results underscore the potential of g-C3N4 nanosheets as effective materials for water splitting applications.