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1.
Bioresour Technol ; : 131103, 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-39002884

RESUMO

A novel UV/oxalic acid functionalized corn straw biochar (OCBC)/peroxyacetic acid (PAA) system was built to degrade sulfadiazine from waters. 94.7 % of SDZ was removed within 30 min by UV/OCBC/PAA. The abundant surface functional groups and persistent free radicals (PFRs) on OCBC were responsible for these performances. Cyclic voltammetry (CV) and other characterization analysis revealed, under UV irradiation, the addition of OCBC served as electron donor, which might promote the reaction of electrons with PAA. The quenching and electron paramagnetic resonance (EPR) tests indicated that R-O•, 1O2 and •OH were generated. Theoretical calculations indicated sulfonamide bridge was vulnerable under the attacks of reactive species. In addition, high removal effect achieved by 5 reuse cycles and different real waters also suggested the sustainability of UV/OCBC/PAA. Overall, this study provided a feasible approach to remove SDZ with high mineralization efficiency, in addition to a potential strategy for resource utilization of corn straw.

2.
Chemosphere ; 327: 138516, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36972874

RESUMO

An amorphous porous iron material (FH) was firstly self-synthesized using a simple coprecipitation approach and then utilized to activate peroxymonosulfate (PMS) for the catalytic degradation of pyrene and remediation of PAHs contaminated soil on site. FH exhibited more excellent catalytic activity than traditional hydroxy ferric oxide and possessed stability at a pH range of 3.0-11.0. According to quenching studies and electron paramagnetic resonance (EPR) analyses, non-radicals (Fe(IV) = O and 1O2) were the major reactive oxygen species (ROS) in the FH/PMS system's degradation of pyrene. X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) of FH before and after the catalytic reaction, as well as active site substitution experiments and electrochemical analysis all verified that PMS adsorbed on FH could produce more abundant bonded hydroxyl groups (Fe-OH) which dominated the radical and non-radical oxidation reactions. Then, a possible pathway for pyrene degradation was presented according to gas chromatography-mass spectrometry (GC-MS). Furthermore, the FH/PMS system exhibited excellent catalytic degradation in the remediation of PAH-contaminated soil at real sites. This work provides a remarkable potential remediation technology of persistent organic pollutants (POPs) in environmental and will contribute to understanding the mechanism of Fe-based hydroxides in advanced oxidation processes.


Assuntos
Ferro , Peróxidos , Ferro/química , Porosidade , Espectroscopia de Infravermelho com Transformada de Fourier , Peróxidos/química , Pirenos
3.
Sci Total Environ ; 858(Pt 3): 160097, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36368392

RESUMO

Single atomic Cu catalysts (SACs Cu@C) anchored by carbon skeleton and chlorine atom was synthesized by hydrolyzing Cu-MOFs and then pickled by aqua-regia to remove Cu nanoparticles (NPs Cu). Comparative characterizations revealed that SACs Cu@C was a hierarchically porous nanostructure and Cu dispersed uniformly throughout the carbon skeletons. With less active components, SACs Cu@C behaved better in activating PMS over NPs Cu@C on ibuprofen removal (91.3 % versus 30.2 % in 30 min). Two Cu coordination environments were found by EXAF and DFT calculation, including four-coordinated Cu with 4C atoms and six-coordinated Cu with 4Cu and 2Cl atoms. The obvious interfacial electron delivery between PMS and SACs Cu@C was found, which was enhanced by Cl atom. Cu(I)/Cu(II) redox cycle would donate electron to peroxy bond of PMS for generating OH, SO4- and O2-. But electron transferred in opposite direction when PMS bonded to Cu atom through its terminal oxygen atom in sulfate, which formed 1O2. IBP degradation proceeded through both radical and non-radical route. IBP degradation was inhibited with the presence of TBA, methanol and furfuryl alcohol but accelerated by p-BQ, which could accelerate OH generation. Two degradation pathways were deducted. This study provided a new insight into catalysts designed for PMS activation.


Assuntos
Carbono , Cloro , Ibuprofeno , Teoria da Densidade Funcional
4.
Environ Int ; 154: 106572, 2021 09.
Artigo em Inglês | MEDLINE | ID: mdl-33895440

RESUMO

In this study, we constructed an innovative photo-electrocatalysis-assisted peroxymonosulfate (PEC/PMS) system to degrade pharmaceuticals and personal care products (PPCPs). A hollow-structured photoanode (i.e., Pt@CeO2@MoS2) was specifically synthesized as a photoanode to activate PMS in the PEC system. As proof of concept, the Pt@CeO2@MoS2 photoanode exhibited superior degradation performance toward carbamazepine (CBZ) with PMS assistance. Specifically, the kinetic constant of PEC/PMS (k = 0.13202 min-1) could be enhanced about 87.4 times compared to that of the PEC system (0.00151 min-1) alone. The PMS activation mechanism revealed that the synergistic effect between the hollow material and the change of surface valence states (Ce3+ to Ce4+) and (Mo4+ to Mo6+) contribute to enhancing the degradation efficiency of the visible-light-driven PEC/PMS process. The scavenger testing and EPR showed that 1O2, O2•-, SO4•- and •OH play dominant roles in the SR-AOPs. Furthermore, the applicability of Pt@CeO2@MoS2 used in SR-AOPs was systematically investigated regarding of the reaction parameters and identification of intermediates and dominant radicals as well as the mineralization rate and stability. The outcomes of this study can provide a new platform for environmental remediation.


Assuntos
Cosméticos , Preparações Farmacêuticas , Molibdênio , Peróxidos
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