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1.
Artigo em Inglês | MEDLINE | ID: mdl-39331297

RESUMO

In this study, the KOH-modified Fe-ZIF-derived carbon materials (Fe@NC-KOH-x) were designed for Fenton-like systems to enhance bisphenol A (BPA) removal from wastewater. Compared with the Fe@NC without KOH activation, the pore structure, BET (Brunner-Emmet-Teller) surface area, and oxygen-containing functional group of KOH-activated Fe@NC-KOH-x are dramatically improved, which increases the adsorption and catalytic performance. The Fe@NC-KOH-900/PMS system showed significant BPA removal reactivity across wide pH ranges and low doses of Fe@NC-KOH-900. Interestingly, our findings indicated that the removal effectiveness of BPA improved when PMS was introduced following the saturation adsorption of Fe@NC-KOH-x, as compared to the simultaneous introduction of Fe@NC-KOH-x and PMS. More particularly, through regression analysis, we found that the proportion of reactive species in the Fe@NC-KOH-x/PMS system changes with the increase of pyrolysis temperature, and there was a certain relationship between structure-function and active species in the Fe@NC-KOH-x/PMS system. O-C = O, Fe-N4, C-O, and pyrrolic N in Fe@NC-KOH-x lead to the generation of •OH, and SO4-•, C = O, Fe-N4, and defect are closely related to FeIV = O, and the formation of 1O2 is affected by Fe-N4, graphite N, C = O, and defect. Also, the density functional theory (DFT) calculation and the potential correlation between catalyst active centers and reactive oxygen species indicate that Fe-N4 is the main active site of Fe@NC-KOH-x. These outcomes of the study offer an innovation for enhanced elimination of BPA in wastewater treatment and provide a dynamic understanding of the mechanism of BPA degradation.

2.
Chemosphere ; 307(Pt 3): 135961, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35963378

RESUMO

The high-performance and free secondary pollution of the catalysts are the most critical issues in the peroxymonosulfate-based advanced oxidation processes (PMS-AOPs). In this research, the KOH was used to activate ZIF-8 derived carbon materials to synthesize the NC-KOH-x (x = 700, 800, 900 °C), which was an effective metal-free PMS activator. As-prepared NC-KOH-x showed significant improvement not only pore structure and BET surface area but also CO groups, and graphite N content, which were beneficial for the adsorptive and oxidative reaction. The NC-KOH-900 as an excellent metal-free carbon-catalyst exhibited considerable reactivity for bisphenol A (BPA) removal in broad pH ranges. Almost 100% of BPA was eliminated using 9 mg NC-KOH-900, 0.5 mM PMS within 60 min. Interestingly, It was found that the BPA removal efficiency by adding PMS after saturated adsorption of NC-KOH-x was better than that by adding NC-KOH-x and PMS simultaneously. Electronic paramagnetic resonance (EPR) and quenching experiments results demonstrated that the BPA degradation relied mainly on the nonradical (1O2) pathways and the defects (ID/IG), graphitic nitrogen, pyridinic nitrogen, and CO were verified as leading catalytic sites for BPA degradation via PMS activation. Finally, degradation pathways of BPA were proposed and the Toxicity Estimation Software Tool (T.E.S.T.) result implicated that the intermediates of BPA were environmentally friendly to the microorganism and recycled in the ecosystem. The outcomes of this study illustrated the NC-KOH-x owned many merits of state-of-the-art, eco-friendly, and high-performance for great potential practical application value.


Assuntos
Carbono , Grafite , Compostos Benzidrílicos , Carbono/química , Ecossistema , Metais , Nitrogênio/química , Peróxidos/química , Fenóis , Porosidade
3.
Chemosphere ; 293: 133455, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-34974041

RESUMO

Bisphenol A (BPA) is a typical kind of endocrine disruption chemical, which has a negative effect on human health, and thus it is necessary to remove BPA from water. Herein, activation of peroxymonosulfate (PMS) by Fe, Cu-Coordinated ZIF-Derived Carbon Framework bifunctional catalyst (Fe/Cu@NC-x) fabricated via hydrothermal-calcination method for BPA removal. The physicochemical properties of Fe/Cu@NC-x were studied by X-ray diffraction, Transmission electron microscopy, Scanning electron microscopy, Raman Spectroscopy, Brunauer-Emmett Teller, and X-ray photoelectron spectroscopy. The effects of the Fe/Cu@NC-900 dosage and PMS concentration, initial pH, and co-existing anions on BPA degradation were evaluated. Under optimized factors (pH unadjusted, Fe/Cu@NC-900 = 0.2 g/L, and PMS = 0.75 g/L), the degradation efficiency of BPA can reach 98% after 30 min. In addition, the BPA degradation efficiency was different extents restrain by inorganic anions (SO42- > Cl- > HCO3- > NO3-). Furthermore, the free radicals (SO4-·, ·OH, and O2-·) and non-radical (1O2) contribute to rapid BPA degradation in Fe/Cu@NC-900/PMS system. This study presents a novel material with significant performance for the removal of organic pollutants.


Assuntos
Carbono , Peróxidos , Compostos Benzidrílicos , Carbono/química , Humanos , Peróxidos/química , Fenóis
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