• The MCNZVI is prepared as an interesting material for PS activation.• Graphitized carbon shells facilitate electron transfer from Fe0.• The MCNZVI exhibits excellent performance to degrade RB5 by 1O2.• The MCNZVI has high stability and reusability in the oxidation system. High-efficiency and cost-effective catalysts with available strategies for persulfate (PS) activation are critical for the complete mineralization of organic contaminants in the environmental remediation and protection fields. A nanoscale zero-valent iron-embedded modified mesoporous carbon (MCNZVI) with a core-shell structure is synthesized using the hydrothermal synthesis method and high-temperature pyrolysis. The results showed that nZVI could be impregnated within mesoporous carbon frameworks with a comparatively high graphitization degree, rich nitrogen doping content, and a large surface area and pore volume. This material was used as a persulfate activator for the oxidation removal of Reactive Black 5 (RB5). The effects of the material dosage, PS concentration, pH, and some inorganic anions (i.e., Cl−, SO42−) on RB5 degradation were then investigated. The highest degradation efficiency (97.3%) of RB5 was achieved via PS (20 mmol/L) activation by the MCNZVI (0.5 g/L). The pseudo-first-order kinetics (k = 2.11 × 10−2 min−1) in the MCNZVI/PS (0.5 g/L, 20 mmol/L) was greater than 100 times than that in the MCNZVI and PS. The reactive oxygen species (ROS), including 1O2, SO4·−, HO·, and ·O2−, were generated by PS activation with the MCNZVI. Singlet oxygen was demonstrated to be the primary ROS responsible for the RB5 degradation. The MCNZVI could be reused and regenerated for recycling. This work provides new insights into PS activation to remove organic contamination. 相似文献
Heterogeneous photocatalysis has long been considered to be one of the most promising approaches to tackling the myriad environmental issues. However, there are still many challenges for designing efficient and cost-effective photocatalysts and photocatalytic degradation systems for application in practical environmental remediation. In this review, we first systematically introduced the fundamental principles on the photocatalytic pollutant degradation. Then, the important considerations in the design of photocatalytic degradation systems are carefully addressed, including charge carrier dynamics, catalytic selectivity, photocatalyst stability, pollutant adsorption and photodegradation kinetics. Especially, the underlying mechanisms are thoroughly reviewed, including investigation of oxygen reduction properties and identification of reactive oxygen species and key intermediates. This review in environmental photocatalysis may inspire exciting new directions and methods for designing, fabricating and evaluating photocatalytic degradation systems for better environmental remediation and possibly other relevant fields, such as photocatalytic disinfection, water oxidation, and selective organic transformations.
● Terminal carboxylate group activation is PFOA degradation’s rate-limiting step. ● Bi3O(OH)(PO4)2 with surface frustrated Lewis pairs (SFLPs) efficiently degrade PFOA. ● Photo-induced Lewis acidic sites and proximal surface hydroxyls constitute SFLPs. ● SFLPs act as collection centers to effectively adsorb PFOA. ● SFLPs endow accessible pathways for photogenerated holes rapid transfer to PFOA. Heterogeneous photocatalysis has gained substantial research interest in treating per- and polyfluoroalkyl substances (PFAS)-contaminated water. However, sluggish degradation kinetics and low defluorination efficiency compromise their practical applications. Here, we report a superior photocatalyst, defected Bi3O(OH)(PO4)2, which could effectively degrade typical PFAS, perfluorooctanoic acid (PFOA), with high defluorination efficiency. The UV light irradiation could in situ generate oxygen vacancies on Bi3O(OH)(PO4)2 through oxidation of the lattice hydroxyls, which further promotes the formation of Lewis acidic coordinately unsaturated bismuth sites. Then, the Lewis acidic sites couple with the proximal surface hydroxyls to constitute the surface frustrated Lewis pairs (SFLPs). With the in-depth spectroscopic analysis, we revealed that the photo-induced SFLPs act as collection centers to effectively adsorb PFOA and endow accessible pathways to transfer photogenerated holes to PFOA rapidly. Consequently, activation of the terminal carboxyl, a rate-limiting step for PFOA decomposition, could be easily achieved over the defected Bi3O(OH)(PO4)2 photocatalyst. These results suggest that SFLPs exhibit great potential in developing highly efficient photocatalysts to degrade persistent organic pollutants. 相似文献
As rapidly growing environmental pollution demands the development of efficient photocatalytic materials, tremendous attention has been drawn to TiO2, a widely used photocatalytic material with cost‐effectiveness, stability, and outstanding reactivity. To maximize its photocatalytic efficiency by enhancing the photogenerated charge separation, lowering the intrinsically large bandgap (3.2 eV) of TiO2 is a key problem to be overcome. Herein, a new design is reported for an efficient photocatalyst realized by heterostructuring a 3D nanostructured TiO2 monolith (3D TiO2) and graphene quantum dots (GQDs) through using 3‐aminopropyltriethoxysilane (APTES) as a linker. The incorporation of APTES between the TiO2/GQD interface enables the formation of a charge injection‐type heterostructure, as confirmed by transient absorption spectroscopy, providing improvement of both visible absorption and charge separation. As a result, the heterostructure exhibits a 242% enhanced photocatalytic performance compared to that of nonheterostructured 3D TiO2 under visible irradiation, demonstrating its promising potential for practical photocatalytic applications in environmental remediation. 相似文献
A solution of atrazine in a TiO2 suspension, an endocrine disruptor in natural water, was tentatively treated by microwave-assisted photocatalytic technique. The effects of mannitol, oxygen, humic acid, and hydrogen dioxide on the photodegradation rate were explored. The results could be deduced as follows: the photocatalytic degradation of atrazine fits the pseudo-first-order kinetic well with k = 0.0328 s−1, and ·OH was identified as the dominant reactant. Photodegradation of atrazine was hindered in the presence of humic acid, and the retardation effect increased as the concentration of humic acid increased. H2O2 displayed a significant negative influence on atrazine photocatalysis efficiency. Based on intermediates identified with gas chromatography-mass spectrometry (GC-MS) and Liquid chromatography-mass spectrometry (LC-MS/MS) techniques, the main degradation routes of atrazine are proposed. 相似文献
