High-performance photocatalytic peroxymonosulfate activation by carbon quantum dots via precise surface chemistry regulation: Insight into the structure-function relations.

Abstract

Carbon quantum dots (CQDs) are considered promising metal-free green catalysts for the activation of persulfates, but direct experimental evidence to identify the true active sites on the surface of CQDs is still lacking. We prepared CQDs with different oxygen contents by controlling the carbonisation temperature, using a simple pyrolysis method. Photocatalytic activity experiments show that CQDs200 exhibits the best PMS activation performance. By investigating the relationship between the oxygen functional groups on CQDs surface and photocatalytic activity, it was postulated that the C=O groups might be the predominant active site, which was confirmed by selective chemical titrations of the C=O, C-OH and COOH groups. Furthermore, limited to the weak photocatalytic properties of the pristine CQDs, ammonia and phenylhydrazine were used to precisely nitrogen-modify the o-CQD surface. We found that phenylhydrazine-modified o-CQDs-PH promoted the absorption of visible light and the separation of photocarriers, thus enhancing the activation of PMS. Theoretical calculations provide more insights from different levels of the pollutant, fine-tuned CQDs, and their interactions.