Nitrogen and sulfur co-doped coal-based carbon quantum dots enhance the photocatalytic hydrogen evolution of Co-Fe-P derived from MOF

Abstract

In order to explore the functional application of coal and realize the high-value application of low-quality coal. Therefore, low-cost coal as a carbon source into environmental protection, high-value coal-based carbon quantum dots (CQDs). This study employed high-sulfur coal as the carbon source and urea as the nitrogen source to successfully synthesize nitrogen and sulfur co-doped coal-based carbon quantum dots (NSCQDs) via a one-pot hydrothermal method. These NSCQDs were utilized as co-catalysts to assist the photocatalytic water splitting and hydrogen evolution of metal phosphides (Co-P and Fe-P). The obtained catalysts were subjected to systematic structural and property analyses, and the photocatalytic hydrogen evolution activity and stability were investigated, along with an analysis of the photocatalytic mechanism. The results revealed that the novel composite photocatalyst exhibited high hydrogen evolution activity, with a maximum hydrogen evolution rate of 28.41 mmol·g−1·h−1 at pH 10. Under a wavelength of 520 nm, the apparent quantum efficiency (AQE) reached 4.93%, and the solar-to-hydrogen (STH) conversion efficiency reached 0.46%. The semiconductor type (n-type) of the monophasic catalyst was determined through Mott-Schottky analysis, and the band structure was analyzed accordingly. The conduction and valence band positions for Co-P were determined to be -0.44 eV and 1.31 eV, respectively, while those for Fe-P were found to be -0.51 eV and 1.17 eV, respectively. Based on these results, it is inferred that an S-type heterojunction is formed between Co-P and Fe-P, and NSCQDs enhanced photocatalytic hydrogen evolution as an auxiliary catalyst. This research advances the synthesis of coal-based carbon quantum dots and provides the key information for the photocatalytic decomposition of water and hydrogen evolution using coal-based CQDs.