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1.
Angew Chem Int Ed Engl ; 56(34): 10170-10173, 2017 08 14.
Artículo en Inglés | MEDLINE | ID: mdl-28544164

RESUMEN

Hydrogen as an energy carrier promises a sustainable energy revolution. However, one of the greatest challenges for any future hydrogen economy is the necessity for large scale hydrogen production not involving concurrent CO2 production. The high intrinsic hydrogen content of liquid-range alkane hydrocarbons (including diesel) offers a potential route to CO2 -free hydrogen production through their catalytic deep dehydrogenation. We report here a means of rapidly liberating high-purity hydrogen by microwave-promoted catalytic dehydrogenation of liquid alkanes using Fe and Ni particles supported on silicon carbide. A H2 production selectivity from all evolved gases of some 98 %, is achieved with less than a fraction of a percent of adventitious CO and CO2 . The major co-product is solid, elemental carbon.

2.
J Hazard Mater ; 458: 131966, 2023 09 15.
Artículo en Inglés | MEDLINE | ID: mdl-37399721

RESUMEN

Pathogenic viruses (e.g., Enteroviruses, Noroviruses, Rotaviruses, and Adenovirus) present in wastewater, even at low concentrations, can cause serious waterborne diseases. Improving water treatment to enhance viral removal is of paramount significance, especially given the COVID-19 pandemic. This study incorporated microwave-enabled catalysis into membrane filtration and evaluated viral removal using a model bacteriophage (MS2) as a surrogate. Microwave irradiation effectively penetrated the PTFE membrane module and enabled surface oxidation reactions on the membrane-coated catalysts (i.e., BiFeO3), which thus elicited strong germicidal effects via local heating and radical formation as reported previously. A log removal of 2.6 was achieved for MS2 within a contact time as low as 20 s using 125-W microwave irradiation with the initial MS2 concentration of 105 PFU∙mL-1. By contrast, almost no inactivation could be achieved without microwave irradiation. COMSOL simulation indicates that the catalyst surface could be heated up to 305 oC with 125-W microwave irradiation for 20 s and also analyzed microwave penetration into catalyst or water film layers. This research provides new insights to the antiviral mechanisms of this microwave-enabled catalytic membrane filtration.


Asunto(s)
COVID-19 , Virus , Purificación del Agua , Humanos , Inactivación de Virus/efectos de la radiación , Microondas , Pandemias , Desinfección , Levivirus , Filtración
3.
J Hazard Mater ; 443(Pt A): 130211, 2023 Feb 05.
Artículo en Inglés | MEDLINE | ID: mdl-36367469

RESUMEN

Aqueous Cr(VI) pollution is an emerging environmental issue. Herein, a sphere-like ZnFe2O4 catalyst with a size of ∼430 nm was prepared by a solvothermal method, by which the aqueous Cr(VI) in a 50 mL solution with concentration of 50 mg/L was completely removed after 10 min-microwave (MW) irradiation. "Surface temperature visualization" tests and COMSOL simulations showed that the surface temperature of the as-prepared ZnFe2O4 catalysts could be as high as > 1000 °C only after 300 s MW irradiation, and the work function calculations and scavenging experiments demonstrated that the excited electrons derived by the "hot spots" effect of the ZnFe2O4 catalysts reduced the Cr(VI) to Cr(III). Kinetic reaction process of the reduction of *Cr2O72- to *CrO3H3 over the ZnFe2O4 catalysts was clarified by using DFT calculation, and the results indicated that *Cr2O72- adsorbed on the Fe atoms was more easily to be reduced, and that Fe atoms played more significant roles than the Zn and O atoms in ZnFe2O4 catalysts. The present study not only proves that the MW induced ZnFe2O4 catalytic reduction was promising for ultrafast remediation of toxic Cr(VI), but also provides a new insight into the corresponding mechanism.

4.
Sci Total Environ ; 790: 147853, 2021 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-34087737

RESUMEN

Microwave catalysis is extremely lucrative due to prompt mineralization and superior efficiency. Ideal microwave catalysts should possess crystalline nature, large surface area, room temperature ferromagnetic, high dielectric properties apart from structural stability at elevated temperature. In the present article, the candidature of microwave synthesized strontium hexaferrite 2D sheets (2D SFO) has been explored as microwave catalysts for the degradation of a host of organic dyes and antibiotics. Malachite green (MG) and nile blue A (NB) in particular exhibited 99.8% and 97.6% degradation, respectively. Degradation reaction is established to follow pseudo-second-order kinetics. Total organic carbon (TOC) measurements hint at 52% and 60% mineralization for MG and NB, respectively. Liquid chromatography-mass spectroscopy (LCMS) measurements indicate the reaction pathways via intermediates and eventual mineralization to CO2 and H2O. Mott-Schottky measurements along with scavenger tests hint that both hydroxyl and superoxide radicals participate in the reaction. Having superior efficiency apart from the versatile nature of the 2D SFO microwave catalyst, the present research will guide to the emergence of microwave catalysis as a new technology.


Asunto(s)
Antibacterianos , Microondas , Catálisis , Colorantes , Estroncio
5.
Environ Int ; 143: 105969, 2020 10.
Artículo en Inglés | MEDLINE | ID: mdl-32702597

RESUMEN

Perfluorooctanoic Acid (PFOA), one of the common per- and poly fluorinated alkylated substances (PFASs), is increasingly detected in the environment due to the diverse industrial applications and high resistance to degradation processes. This study evaluated degradation of PFOA in microwave-assistant catalytic membrane filtration, a process that integrates microwave catalytic reactions into a ceramic membrane filtration. First, water permeation of the pristine and catalyst-coated membranes were examined under the influence of microwave irradiation to analyse the impacts of the coating layer and water temperature increase on permeate flux, which were well interpreted by the Carman-Kozeny and Hagen-Posieulle (non-slipping and slit-like) models. Then, the PFOA removal was first assessed in a continuous filtration mode with and without microwave irradiation. Our results show that PFOA first adsorbed on membrane and catalyst materials, and then fully penetrated the membrane filter after reaching adsorption equilibrium. Under microwave irradiation (7.2 W·cm-2), approximate 65.9% of PFOA (25 µg·L-1) in the feed solution was degraded within a hydraulic time of 2 min (at the permeate flow rate of 43 LMH) due to the microwave-Fenton like reactions. In addition, low flow rates and moderate catalyst coating densities are critical for optimizing PFOA removal. Finally, potential degradation mechanisms of PFOA were proposed through the analysis of degradation by-products (e.g., PFPeA). The findings may provide new insight into the development of reactive membrane-enabled systems for destruction of refractory PFAS.


Asunto(s)
Fluorocarburos , Caprilatos , Catálisis , Microondas
6.
Chemosphere ; 214: 319-329, 2019 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-30267905

RESUMEN

A novel treatment technology of microwave catalytic oxidation degradation (MCOD) for nitrophenols (NPs) wastewater over green catalysts of gC3N4Bi2O2CO3 and SiCBi2O2CO3 was developed. This process is eco-friendly because the only used Bi2O2CO3 is non-toxic (which can be used as stomach medicine), and no heavy metal pollution exists in g-C3N4 and SiC. The results show that these Bi2O2CO3 based composites exhibited superior catalytic activity for the degradation of para-NP, as well as ortho-NP, with optimal removal ratio of 98.96%. In addition, the proportion of Bi2O2CO3 and irradiation time were the key parameters that had greatly influenced the degradation performance. Moreover, O2- was confirmed to be primary contributor for the degradation, which was different from our previous work that OH was the main specie in carbon loaded metal oxide system. That is to say, the type of oxidative specie may be controlled by the type of catalyst system. Besides, separation and transfer efficiency of the charge carriers could be enhanced by the heterojunctions fabricated in the band structures of the composites. This work not only demonstrated that the Bi2O2CO3 based composites coupled with MW irradiation can generate reactive oxidative species(ROS) which can degrade NPs high-effectively, but also developed a new and green idea for treating refractory industrial wastewater.


Asunto(s)
Tecnología Química Verde/métodos , Microondas , Nitrofenoles/química , Catálisis , Oxidación-Reducción , Óxidos/química , Aguas Residuales/química , Contaminantes Químicos del Agua/química , Purificación del Agua/métodos
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