Elaborating the specific reactive oxygen species (ROS) involved in the photocatalytic degradation of atrazine (ATZ) is of great significance for elucidating the underlying mechanism. This study provided conclusive evidence that hydroxyl radicals (·OH) were the primary ROS responsible for the efficient photocatalytic degradation of ATZ, thereby questioning the reliability of widely adopted radical quenching techniques in discerning authentic ROS species. As an illustration, oxygen-modified g-C3N4 (OCN) was prepared to counteract the limitations of pristine g-C3N4 (CN). Comparative assessments between CN and OCN revealed a remarkable 10.44-fold improvement in the photocatalytic degradation of ATZ by OCN. This enhancement was ascribed to the increased content of C–O functional groups on the surface of the OCN, which facilitated the conversion of superoxide radicals (·O2–) into hydrogen peroxide (H2O2), subsequently leading to the generation of ·OH. The increased production of ·OH contributed to the efficient dealkylation, dechlorination, and hydroxylation of ATZ. Furthermore, toxicity assessments revealed a significant reduction in ATZ toxicity following its photocatalytic degradation by OCN. This study sheds light on the intricate interconversion of ROS and offers valuable mechanistic insights into the photocatalytic degradation of ATZ.
Presently, the hydroxyl radical oxidation mechanism is widely acknowledged for the degradation of organic pollutants based on hydrodynamic cavitation technology. The presence and production mechanism of other potential reactive oxygen species (ROS) in the cavitation systems are still unclear. In this paper, singlet oxygen (1O2) and superoxide radical (·O2-) were selected as the target ROS, and their generation rules and mechanism in vortex-based hydrodynamic cavitation (VBHC) were analyzed. Computational fluid dynamics (CFD) were used to simulate and analyze the intensity characteristics of VBHC, and the relationship between the generation of ROS and cavitation intensity was thoroughly revealed. The results show that the operating conditions of the device have a significant and complicated influence on the generation of 1O2 and ·O2-. When the inlet pressure reaches to 4.5 bar, it is more favorable for the generation of 1O2 and ·O2- comparing with those lower pressure. However, higher temperature (45℃) and aeration rate (15 (L/min)/L) do not always have positive effect on the 1O2 and ·O2- productions, and their optimal parameters need to be analyzed in combination with the inlet pressure. Through quenching experiments, it is found that 1O2 is completely transformed from ·O2-, and ·O2- comes from the transformation of hydroxyl radicals and dissolved oxygen. Higher cavitation intensity is captured and shown more disperse in the high-pressure flow region, which is consistent with the larger generation and stronger diffusion of 1O2 and ·O2-. This paper shed light to the generation mechanism of 1O2 and ·O2- in VBHC reactors and the relationship with cavitation intensity. The conclusion provides new ideas for the research of effective ROS in hydrodynamic cavitation process.
Compared to the bulk-CN, the quasi-2D-CN possesses a unique electronic structure, enlarged bandgap, prolonged lifetime, increased surface area and enhanced electronic transport, and exhibits highly efficient hydrogen production from water under visible light.
Most researchers believe that the high catalytic activity of FeOCl originates from its unique structure. In this study, we show that dissolved iron contributes significantly to the catalytic activity of FeOCl in the Fenton and photo-Fenton processes.
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