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1.
J Environ Sci (China) ; 148: 243-262, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095161

RESUMO

Because of the recent widespread usage of antibiotics, the acquisition and dissemination of antibiotic-resistance genes (ARGs) were prevalent in the majority of habitats. Generally, the biological wastewater treatment processes used in wastewater treatment plants have a limited efficiencies of antibiotics resistant bacteria (ARB) disinfection and ARGs degradation and even promote the proliferation of ARGs. Problematically, ARB and ARGs in effluent pose potential risks if they are not further treated. Photocatalytic oxidation is considered a promising disinfection technology, where the photocatalytic process generates many free radicals that enhance the interaction between light and deoxyribonucleic acid (DNA) for ARB elimination and subsequent degradation of ARGs. This review aims to illustrate the progress of photocatalytic oxidation technology for removing antibiotics resistant (AR) from wastewater in recent years. We discuss the sources and transfer of ARGs in wastewater. The overall removal efficiencies of ultraviolet radiation (UV)/chlorination, UV/ozone, UV/H2O2, and UV/sulfate-radical based system for ARB and ARGs, as well as the experimental parameters and removal mechanisms, are systematically discussed. The contribution of photocatalytic materials based on TiO2 and g-C3N4 to the inactivation of ARB and degradation of ARGs is highlighted, producing many free radicals to attack ARB and ARGs while effectively limiting the horizontal gene transfer (HGT) in wastewater. Finally, based on the reviewed studies, future research directions are proposed to realize specific photocatalytic oxidation technology applications and overcome current challenges.


Assuntos
Eliminação de Resíduos Líquidos , Águas Residuárias , Águas Residuárias/química , Eliminação de Resíduos Líquidos/métodos , Bactérias , Desinfecção/métodos , Farmacorresistência Bacteriana/genética , Raios Ultravioleta , Purificação da Água/métodos
2.
ACS Appl Mater Interfaces ; 16(39): 52550-52558, 2024 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-39300808

RESUMO

Regulating the selective generation of reactive oxygen species (ROS) is a significant challenge in the field of photocatalytic oxidation, with successful approaches still being limited. Herein, we present a strategy to selectively generate singlet oxygen (1O2) and superoxide radicals (O2•-) by tuning the dimensionality of porphyrin-based covalent organic frameworks (COFs). The transformation of COFs from three-dimensional (3D) solids to two-dimensional (2D) sheets was achieved through the reversible protonation of the imine bond. Upon irradiation, both bulk and thin-layer COF-367 can transfer energy to O2 to generate 1O2. However, thin-layer COF-367 exhibited a superior performance compared to its bulk counterpart in activating O2 to form the O2•- radicals via electron transfer. After excluding the influences of the band structure, O2 adsorption energy, and frontier orbital composition attributed to the dimensionality of the COFs, it is reasonably speculated that the variance in ROS generation arises from the differential exposure ratios of the active surfaces, leading to distinct reaction pathways between the carrier and O2. This study is the first to explore the modulation mechanism of COF dimensionality on the activation of the O2 pathway, underscoring the importance of considering COF dimensionality in photocatalytic reactions.

3.
Chemosphere ; 366: 143409, 2024 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-39326714

RESUMO

An effective approach for the elimination of indoor gaseous toluene through photocatalytic oxidation involves the engineering of surface defects on catalysts. In this study, the concentrations of surface oxygen defects in PdTi-xN (x = 10, 30) catalysts were controlled using the sodium borohydride solid-phase reduction method, and their performances in the photocatalytic oxidation of indoor gaseous toluene were evaluated. PdTi-10 N demonstrated high photocatalytic efficiency for toluene oxidation, achieving 84% toluene conversion and approximately 75% CO2 mineralization. Characterization results indicated that surface oxygen defects can enhance the separation of photo-generated electrons and holes, facilitating their interaction with Pd0 species to form Ti3+ species. More reactive oxygen species (·OH-and ·O2-) were generated on PdTi-10 N due to the synergistic effect of surface oxygen defect and Ti3+ species, which played a significant role as the toluene oxidation. This work provides a new insight for the design and development of high-performance Pd/TiO2 catalysts in the field of indoor VOCs treatment.

4.
Environ Sci Pollut Res Int ; 31(40): 52707-52723, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39190251

RESUMO

The widespread use of organophosphorus flame retardants (OPFRs) in industrial and household products increases the risk of their environmental exposure, posing a serious threat to ecosystems and human health. Photocatalytic technology has been widely used in wastewater treatment due to its high efficiency, mild reaction conditions, and robustness. This review summarizes the current status of research on photocatalytic degradation of OPFRs, focusing on the effect of different types of catalysts on the degradation efficiency, the effects of pH, and co-existing inorganic and organic ions. And pH and co-existing inorganic mainly affect the active oxygen and the active surface sites of the catalyst. In addition, toxicological calculations of the intermediates of the degradation pathway using T.E.S.T. and ECOSAR showed that photocatalysis could effectively reduce the toxicity of OPFRs. Development of new photocatalytic materials, in-depth study of the degradation mechanism of different catalysts and flame retardants, and attention to practical applications and toxicity issues can be the development direction of future research.


Assuntos
Retardadores de Chama , Compostos Organofosforados , Compostos Organofosforados/química , Catálise , Poluentes Químicos da Água/química , Fotólise
5.
ACS Appl Mater Interfaces ; 16(28): 37275-37287, 2024 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-38959130

RESUMO

Titanium dioxide (TiO2) shows significant potential as a self-cleaning material to inactivate severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) and prevent virus transmission. This study provides insights into the impact of UV-A light on the photocatalytic inactivation of adsorbed SARS-CoV-2 virus-like particles (VLPs) on a TiO2 surface at the molecular and atomic levels. X-ray photoelectron spectroscopy, combined with density functional theory calculations, reveals that spike proteins can adsorb on TiO2 predominantly via their amine and amide functional groups in their amino acids blocks. We employ atomic force microscopy and grazing-incidence small-angle X-ray scattering (GISAXS) to investigate the molecular-scale morphological changes during the inactivation of VLPs on TiO2 under light irradiation. Notably, in situ measurements reveal photoinduced morphological changes of VLPs, resulting in increased particle diameters. These results suggest that the denaturation of structural proteins induced by UV irradiation and oxidation of the virus structure through photocatalytic reactions can take place on the TiO2 surface. The in situ GISAXS measurements under an N2 atmosphere reveal that the virus morphology remains intact under UV light. This provides evidence that the presence of both oxygen and UV light is necessary to initiate photocatalytic reactions on the surface and subsequently inactivate the adsorbed viruses. The chemical insights into the virus inactivation process obtained in this study contribute significantly to the development of solid materials for the inactivation of enveloped viruses.


Assuntos
SARS-CoV-2 , Titânio , Raios Ultravioleta , Titânio/química , Titânio/efeitos da radiação , SARS-CoV-2/efeitos da radiação , SARS-CoV-2/química , Inativação de Vírus/efeitos da radiação , Inativação de Vírus/efeitos dos fármacos , Humanos , Glicoproteína da Espícula de Coronavírus/química , Glicoproteína da Espícula de Coronavírus/metabolismo , COVID-19/virologia , COVID-19/prevenção & controle , Adsorção , Propriedades de Superfície
6.
Water Environ Res ; 96(5): e11057, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38797515

RESUMO

Photocatalytic oxidation-adsorption synergistic treatment of organic arsenic pollutants is a promising wastewater treatment technology, which not only degrades organic arsenic pollutants by photocatalytic degradation but also removes the generated inorganic arsenic by adsorption. This paper compares the results of photocatalytic oxidation-adsorption co-treatment of organic arsenic pollutants such as monomethylarsonic acid, dimethylarsinic acid, phenylarsonic acid, p-arsanilic acid, and 3-nitro-4-hydroxyphenylarsonic acid on titanium dioxide, goethite, zinc oxide, and copper oxide. It examines the influence of the morphology of organic arsenic molecules, pH, coexisting ions, and the role of natural organic matter. The photocatalytic oxidation-adsorption co-treatment mechanism is investigated, comparing the hydroxyl radical oxidation mechanism, the hydroxyl radical and superoxide anion radical cooxidation mechanism, and the hydroxyl radical and hole cooxidation mechanism. Finally, the future prospects of metal oxide photocatalytic materials and the development of robust and efficient technologies for removing organic arsenic are envisioned.


Assuntos
Oxirredução , Poluentes Químicos da Água , Purificação da Água , Poluentes Químicos da Água/química , Adsorção , Catálise , Purificação da Água/métodos , Arsênio/química , Processos Fotoquímicos
7.
ACS Appl Mater Interfaces ; 16(23): 30020-30030, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38814279

RESUMO

Titanium-oxo clusters, with their robust structure and suitable optical and electronic properties, have been widely investigated as photocatalysts. Heterometallic Ti/M-oxo clusters provide additional tunability and functionality, which enable systematic structure-activity investigations to elucidate the reaction mechanisms and improve the catalyst design. Incorporating cerium into Ti-oxo clusters can provide additional redox (CeIV/CeIII) and oxygen harvesting ability, but to date, only a limited number of structurally defined titanium-cerium (Ti/Ce) clusters have been reported due to their synthetic challenges. Herein, we report the synthesis and photocatalytic properties of two structurally defined Ti/Ce-oxo clusters, Ti8Ce2(BA)16 and Ti9Ce4(BA)20, as well as a TiCe-BA cluster with a calculated formula of Ti20Ce9O36(BA)42. Photocatalytic study of these clusters demonstrates that the amount of Ce3+ species greatly impacts its photocatalytic oxidation performance, and their superior photocatalytic reactivity toward aerobic alcohol oxidation can be contributed to the synergistic effects of the multiple radical species generated upon light absorption. This work represents a significant milestone in the construction of stable Ti/Ce-oxo clusters, enriching the current library of known heterometallic Ti/M-oxo clusters, and providing a series of crystalline materials with great promise of photoluminescence and photovoltaic chemistry.

8.
Adv Mater ; 36(28): e2309205, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38733334

RESUMO

Visible-light-driven photocatalytic oxidation by photogenerated holes has immense potential for environmental remediation applications. While the electron-mediated photoreduction reactions are often at the spotlight, active holes possess a remarkable oxidation capacity that can degrade recalcitrant organic pollutants, resulting in nontoxic byproducts. However, the random charge transfer and rapid recombination of electron-hole pairs hinder the accumulation of long-lived holes at the reaction center. Herein, a novel method employing defect-engineered indium (In) single-atom photocatalysts with nitrogen vacancy (Nv) defects, dispersed in carbon nitride foam (In-Nv-CNF), is reported to overcome these challenges and make further advances in photocatalysis. This Nv defect-engineered strategy produces a remarkable extension in the lifetime and an increase in the concentration of photogenerated holes in In-Nv-CNF. Consequently, the optimized In-Nv-CNF demonstrates a remarkable 50-fold increase in photo-oxidative degradation rate compared to pristine CN, effectively breaking down two widely used antibiotics (tetracycline and ciprofloxacin) under visible light. The contaminated water treated by In-Nv-CNF is completely nontoxic based on the growth of Escherichia coli. Structural-performance correlations between defect engineering and long-lived hole accumulation in In-Nv-CNF are established and validated through experimental and theoretical agreement. This work has the potential to elevate the efficiency of overall photocatalytic reactions from a hole-centric standpoint.

9.
Environ Sci Pollut Res Int ; 31(20): 30085-30098, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38598155

RESUMO

Formaldehyde (HCHO) is one of the primary indoor air pollutants, and efficiently eliminating it, especially at low concentrations, remains challenging. In this study, BiVO4-TiO2 catalyst was developed using ultrasonic blending technology for the photocatalytic oxidation of low-level indoor HCHO. The crystal structure, surface morphology, element distribution, and active oxidation species of the catalyst were examined using XRD, SEM, TEM, UV-Vis, EDS, and ESR techniques. Our results demonstrated that the BiVO4-TiO2 catalyst, prepared by ultrasonic blending, exhibited good oxidation performance and stability. The HCHO concentration reduced from 1.050 to 0.030 mg/m3 within 48 h, achieving a removal rate of 97.1%. The synergy between BiVO4 and TiO2 enhanced the efficiency of separating photogenerated carriers and minimized the likelihood of recombination between photogenerated electrons and holes. Additionally, this synergy significantly enhanced the presence of hydroxyl radicals (·OH) on the catalyst, resulting in an oxidation performance superior to that of either BiVO4 or TiO2. Our research offers valuable insights for the development of new photocatalysts to address HCHO pollution.


Assuntos
Bismuto , Formaldeído , Oxirredução , Titânio , Vanadatos , Formaldeído/química , Titânio/química , Vanadatos/química , Bismuto/química , Catálise , Luz , Ultrassom
10.
Angew Chem Int Ed Engl ; 63(20): e202402760, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38483296

RESUMO

The phenomenon of polymorphism is ubiquitous in nature, the controlled manipulation of which not only increases our ontological understanding of nature but also facilitates the conceptualization and realization of novel functional materials. However, achieving targeted polymorphism in supramolecular assemblies (SAs) remains a formidable challenge, largely because of the constraints inherent in controlling the specific binding motifs of noncovalent interactions. Herein, we propose self-adaptive aromatic cation-π binding motifs to construct polymorphic SAs in both the solid and solution states. Using distinct discrete cation-π-cation and long-range cation-π binding motifs enables control of the self-assembly directionality of a C2h-symmetric bifunctional monomer, resulting in the successful formation of both two-dimensional and three-dimensional crystalline SAs (2D-CSA and 3D-CSA). The differences in the molecular packing of 3D-CSA compared with that of 2D-CSA significantly improve the charge separation and carrier mobility, leading to enhanced photocatalytic activity for the aerobic oxidation of thioanisole to methyl phenyl sulfoxide (yield of 99 % vs 57 %). 2D-CSA, which has a vertical extended structure with favorable stronger interaction with toluene though face-to-face cation-π interactions than methylcyclohexane, shows higher toluene/methylcyclohexane separation efficiency than 3D-CSA (96.9 % for 2D-CSA vs 56.3 % for 3D-CSA).

11.
J Colloid Interface Sci ; 664: 63-73, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38460385

RESUMO

Photocatalytic oxidative coupling of amines is considered a mild, efficient, and sustainable strategy for the synthesis of imines. As a versatile organic semiconductor, conjugated microporous polymers (CMPs) are attractive in photocatalysis areas due to the diversity of their polymeric monomers. Herein, we report that in addition to the design of monomers, size-confined polymerization is also a feasible strategy to modulate the structure and photocatalysis properties of CMPs. We adopted dibromopyrazine as polymeric units to prepare pyrazine-involved hollow spherical CMPs (H-PyB) using a template method and successfully performed size-confined polymerization of hollow samples by resizing the templates. Interestingly, the small confinement space induced the formation of CMPs with better conjugate extensibility, resulting in enhanced conductivity, narrowed bandgaps, improved photoelectric performance, etc. As a result, small-sized H-PyB CMPs had superior activity for the photocatalytic oxidation of amines. Particularly, the smallest H-PyB CMPs that we designed in the present work exhibited excellent performance for the photocatalytic coupling oxidation of amines. When using benzylamine as a model substrate, the yield of the corresponding imine reached âˆ¼ 113 mmol·g-1·h-1, accompanied by almost 100 % selectivity. Furthermore, the as-designed confined samples exhibited stable photocatalytic activity as well as good applicability for oxidative coupling of different amines. This work not merely reports a kind of CMP photocatalysts with excellent performance for the imine coupling oxidation but also proposes an alternative strategy for constructing high-performance organic photocatalysts by size-confined synthesis.

12.
Chemosphere ; 353: 141525, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38395369

RESUMO

Air pollution causes extreme toxicological repercussions for human health and ecology. The management of airborne bacteria and viruses has become an essential goal of air quality control. Existing pathogens in the air, including bacteria, archaea, viruses, and fungi, can have severe effects on human health. The photocatalysis process is one of the favorable approaches for eliminating them. The oxidative nature of semiconductor-based photocatalysts can be used to fight viral activation as a green, sustainable, and promising approach with significant promise for environmental clean-up. The photocatalysts show wonderful performance under moderate conditions while generating negligible by-products. Airborne viruses can be inactivated by various photocatalytic processes, such as chemical oxidation, toxicity due to the metal ions released from photocatalysts composed of metals, and morphological damage to viruses. This review paper provides a thorough and evaluative analysis of current information on using photocatalytic oxidation to deactivate viruses.


Assuntos
Poluição do Ar , Infecções por Coronavirus , Coronavirus , Humanos , Poluição do Ar/prevenção & controle , Infecções por Coronavirus/prevenção & controle , Oxirredução , Metais
13.
Environ Sci Technol ; 58(9): 4404-4414, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38310571

RESUMO

Photocatalytic oxidation has gained great interest in environmental remediation, but it is still limited by its low efficiency and catalytic deactivation in the degradation of aromatic VOCs. In this study, we concurrently regulated the surface hydroxyl and oxygen vacancies by introducing Al into ZnSn layered double hydroxide (LDH). The presence of distorted Al species induced local charge redistribution, leading to the remarkable formation of oxygen vacancies. These oxygen vacancies subsequently increased the amount of surface hydroxyl and elongated its bond length. The synergistic effects of surface hydroxyl and oxygen vacancies greatly enhanced reactant adsorption-activation and facilitated charge transfer to generate •OH, •O2-, and 1O2, resulting in highly efficient oxidation and ring-opening of various aromatic VOCs. Compared with commercial TiO2, the optimized ZnSnAl-50 catalyst exhibited about 2-fold activity for the toluene and styrene degradation and 10-fold activity for the chlorobenzene degradation. Moreover, ZnSnAl-50 demonstrated exceptional stability in the photocatalytic oxidation of toluene under a wide humidity range of 0-75%. This work marvelously improves the photocatalytic efficiency, stability, and adaptability through a novel strategy of surface hydroxyl and oxygen vacancies engineering.


Assuntos
Radical Hidroxila , Oxigênio , Adsorção , Oxirredução , Tolueno
14.
Anal Chim Acta ; 1293: 342284, 2024 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-38331552

RESUMO

In the present work, we developed a photoelectrochemical aptasensor to determine omethoate (OMT) based on the dual signal amplification of CeO2@MnO2 photocatalysis for glucose oxidation and exonuclease I-assisted cyclic catalytic hydrolysis. CeO2@MnO2 heterojunction material prepared by hydrothermal method was linked with captured DNA (cDNA) and then assembled on the ITO conductive glass to form ITO/CeO2@MnO2-cDNA, which exhibited significant photocurrent response and good photocatalytic performance for glucose oxidation under visible light irradiation, providing the feasibility for sensitive determining OMT. After binding with the aptamer of OMT (apt), the formation of rigid double stranded cDNA/apt kept CeO2@MnO2 away from ITO surface, which ensured a low photocurrent background for the constructed ITO/CeO2@MnO2-cDNA/apt aptasensor. In the presence of target OMT, the restoration of the cDNA hairpin structure and the exonuclease I-assisted cyclic catalytic hydrolysis led to the generation and amplification of measurement photocurrent signals, and allowed the aptasensor to have an ideal quantitative range of 0.01-10.0 nM and low detection limit of 0.0027 nM. Moreover, the aptasensor has been applied for selective determination of OMT in real samples with good precision of the relative standard deviation less than 6.2 % and good accuracy of the recoveries from 93 % to 108 %. What's more, the aptasensor can be used for other target determination only by replacing the captured DNA and corresponding aptamer.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Dimetoato/análogos & derivados , Glucose , DNA Complementar , Compostos de Manganês , Óxidos , DNA/química , Técnicas Biossensoriais/métodos , Aptâmeros de Nucleotídeos/química , Técnicas Eletroquímicas/métodos , Limite de Detecção
15.
Adv Mater ; 36(3): e2306758, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37865887

RESUMO

Ring-opening of phenol in wastewater is the pivotal step in photocatalytic degradation. The highly selective generation of catalytical active species (•OH) to facilitate this process presents a significant scientific challenge. Therefore, a novel approach for designing photocatalysts with single-atom containment in metal-covalent organic frameworks (M-COFs) is proposed. The selection of imine-linked COFs containing abundant N and O-chelate sites provides a solid foundation for anchoring metal atom. These dispersed metal atom possess rapid accumulation and transfer capabilities for photogenerated electrons, while the periodic π-conjugated structure in 2D-COFs establishes an effective platform. Additionally, the Lewis acid properties of imine bonds in COFs can enhance the adsorption capacity toward gases with Lewis base properties, such as O2 and N2 . It is demonstrated that the Pd2+ @Tp-TAPT, designed based on this concept, exhibits efficient oxygen adsorption and follows the reaction pathway of O2 →•O2 - →H2 O2 →•OH with high selectivity, thereby achieving completely degradation of refractory phenol through photocatalysis within 10 min. It is anticipated that the selective generation of catalytic active species via advanced material design concepts will serve as a significant reference for achieving precise material catalysis in the future.

16.
Molecules ; 28(24)2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-38138607

RESUMO

This study demonstrates rapid photocatalytic oxidation of a benzene, toluene, ethylbenzene, and xylene (BTEX) mixture over TiO2/volcanic glass. The assessment of the photocatalytic oxidation of BTEX was conducted under conditions simulating those found in indoor environments affected by aromatic hydrocarbon release. We show, under UV-A intensities of 15 mW/cm2 and an air flow rate of 55 m3/h, that low ppmv levels of BTEX concentrations can be reduced to below detectable levels. Solid-phase microextraction technique was employed to monitor the levels of BTEX in the test chamber throughout the photocatalytic oxidation, lasting approximately 21 h. Destruction of BTEX from the gas phase was observed in the following sequence: o-xylene, ethylbenzene, toluene, and benzene. This study identified sequential degradation of BTEX, in combination with the stringent regulatory level set for benzene, resulted in the air quality hazard indexes (Total Hazard Index and Hazard Quotient) remaining relatively high during the process of photocatalytic oxidation. In the practical application of photocatalytic purification, it is crucial to account for the slower oxidation kinetics of benzene. This is of particular importance due to not only its extremely low exposure limits, but also due to the classification of benzene as a Group 1 carcinogenic compound by the International Agency for Research on Cancer (IARC). Our study underscores the importance of taking regulatory considerations into account when using photocatalytic purification technology.


Assuntos
Benzeno , Tolueno , Humanos , Xilenos/análise , Derivados de Benzeno/metabolismo , Medição de Risco , Monitoramento Ambiental/métodos
17.
Heliyon ; 9(11): e21738, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38034683

RESUMO

Poly-halogenated phenols generated from a range of industrial processes can find their way into rivers and ground water. Here we report on a potential treatment for reducing the toxicity of these aqueous pollutants using two highly toxic penta-halogenated phenols (pentachlorophenol (PCP) and pentabromophenol (PBP)) as surrogates. Solutions were passed through a glass column packed with a silica support fused with titanium dioxide (TiO2) and horseradish peroxidase (HRP) immobilized on its TiO2/glass surface (HRP-Tglass). TiO2 photocatalysis was activated through irradiation with UVB (320 nm) which in turn activated the HRP. Two operational flow rates (0.5 and 1.25 mL min-1; hydraulic retention times (HRTs) of 20 and 8 min, respectively), tested the effect of retention time on the extent of degradation and reduction in toxicity of the treated effluent. Microtox® was used to measure the toxicity of the substrate and its by-products at both flow rates. At the highest flow rate, dehalogenation was limited (removal of 37 % chlorine and 22 % bromine) and the toxicity of the reaction products increased. At the lowest flow rate, the longer exposure time resulted in approximately 97 % and 96 % transformation of PCP and PBP, respectively, a greater degree of dehalogenation (removal of 65 % chlorine and 70 % bromine) and a substantial decrease in toxicity of the treated solutions. The higher toxicity of effluent from the higher flow rate was attributed to the initial degradation products being more toxic than the substrates. With a longer HRT, these were then further broken down to less toxic products. Additional toxicity tests (Hydra hexactinella (Hydra) and Chinese Hamster Ovary (CHO) cell toxicity were conducted on the effluent from the lowest flow rate. Both were less sensitive than the Microtox test, with Hydra proving more sensitive than CHO. The novelty of this work is the toxicity risk assessment of the products resulting from the use of a spatially separated immobilized enzyme and photooxidation system. The system was robust and showed no decrease in treatment efficacy over 10 h.

19.
Molecules ; 28(18)2023 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-37764227

RESUMO

A review of the current literature shows there is no clear consensus regarding the reaction mechanisms of air-borne aromatic compounds such as toluene by photocatalytic oxidation. Potential oxidation reactions over TiO2 or TiO2-based catalysts under ultraviolet and visible (UV/VIS) illumination are most commonly considered for removal of these pollutants. Along the pathways from a model pollutant, toluene, to final mineralization products (CO2 and H2O), the formation of several intermediates via specific reactions include parallel oxidation reactions and formation of less-reactive intermediates on the TiO2 surface. The latter may occupy active adsorption sites and causes drastic catalyst deactivation in some cases. Major hazardous gas-phase intermediates are benzene and formaldehyde, classified by the International Agency for Research on Cancer (IARC) as Group 1 carcinogenic compounds. Adsorbed intermediates leading to catalyst deactivation are benzaldehyde, benzoic acid, and cresols. The three most typical pathways of toluene photocatalytic oxidation are reviewed: methyl group oxidation, aromatic ring oxidation, and aromatic ring opening.

20.
Environ Sci Pollut Res Int ; 30(43): 96782-96794, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37581737

RESUMO

In this study, the visible light-responsive catalysts Fe3O4/Bi2WO6 were prepared and characterized by BET, SEM, EDS, XRD, XPS, and MPMS. The performances of five catalysts (0.05 Fe/Bi, 0.13 Fe/Bi, 0.17 Fe/Bi, 0.21 Fe/Bi, and 0.30 Fe/Bi) for photocatalytic degradation of bisphenol A under visible light (300-W Xe lamp) were compared. Among five catalysts, 0.17 Fe/Bi (the molar ratio of Fe3O4 to Bi2WO6 was 0.17) acquired the highest BPA photocatalytic removal of 90.2% at 120 min. With the synergistic effect between Vis/0.17 Fe/Bi and peroxymonosulfate (PMS), the BPA removal obtained was as high as 100% at 90 min ([BPA] = 100 mg/L, [0.17 Fe/Bi] = 1.25 g/L, [PMS] = 2.0 g/L, and T = 25 °C). After five times reused of 0.17 Fe/Bi, its removal of BPA dropped by 13.4% in presence of PMS, which demonstrated 0.17 Fe/Bi possessed relatively stable performance. High BPA degradation was attributed to the attacking effects of various oxide species (SO4•-, •OH, h+, O2•-) generated in the Fe3O4/Bi2WO6/PMS system under the cooperation of photocatalyst Fe3O4/Bi2WO6 and oxidizing agent PMS.


Assuntos
Luz , Peróxidos , Fenóis
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