Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 49
Filtrar
1.
Langmuir ; 39(47): 16863-16872, 2023 Nov 28.
Artículo en Inglés | MEDLINE | ID: mdl-37963178

RESUMEN

A suitable adsorbent is essential in the process of removing hazardous vanadium(V) from actual groundwater. In this work, MIL-88A(Fe)/cotton (MC) was employed to eliminate V(V) from simulated vanadium-contaminated groundwater. The findings demonstrated that MC exhibited an exceptional performance in removing V(V), displaying a maximum adsorption capacity of 218.71 mg g-1. MC exhibits great promise as an adsorbent for V(V) elimination in an extensive pH range spanning 3 to 11. Even in the presence of high levels of competing ions such as Cl-, NO3-, and SO42-, MC demonstrated remarkable specificity in adsorbing V(V). The results of column experiments and co-occurring ions influence tests indicate that MC is a potential candidate for effectively treating actual vanadium-contaminated groundwater. The effluent could meet the vanadium content restriction of 50 µg L-1 required in China's drinking water sources. Regeneration of MC can be performed easily without experiencing significant capacity loss. The results obtained from this research indicate the promising potential of MC in mitigating vanadium pollution.

2.
Environ Sci Technol ; 56(8): 5200-5212, 2022 04 19.
Artículo en Inglés | MEDLINE | ID: mdl-35394751

RESUMEN

Material-enhanced heterogonous peroxymonosulfate (PMS) activation on emerging organic pollutant degradation has attracted intensive attention, and a challenge is the electron transfer efficiency from material to PMS for radical production. Herein, an interface architecture of Co(OH)2 nanosheets growing on the KNbO3 perovskite [Co(OH)2/KNbO3] was developed, which showed high catalytic activity in PMS activation. A high reaction rate constant (k1) of 0.631 min-1 and complete removal of pazufloxacin within 5 min were achieved. X-ray photoelectron spectroscopy, X-ray absorption near edge structure spectra, and density functional theory (DFT) calculations revealed the successful construction of the material interface and modulated electronic structure for Co(OH)2/KNbO3, resulting in the hole accumulation on Co(OH)2 and electron accumulation on KNbO3. Bader topological analysis on charge density distribution further indicates that the occupations of Co-3d and O-2p orbitals in Co(OH)2/KNbO3 are pushed above the Fermi level to form antibonding states (σ*), leading to high chemisorption affinity to PMS. In addition, more reactive Co(II) with the closer d-band center to the Fermi level results in higher electron transfer efficiency and lower decomposition energy of PMS to SO4•-. Moreover, the reactive sites of pazufloxacin for SO4•- attack were precisely identified based on DFT calculation on the Fukui index. The pazufloxacin pathways proceeded as decarboxylation, nitroheterocyclic ring opening reaction, defluorination, and hydroxylation. This work can provide a potential route in developing advanced catalysts based on manipulation of the interface and electronic structure for enhanced Fenton-like reaction such as PMS activation.


Asunto(s)
Compuestos de Calcio , Peróxidos , Electrónica , Óxidos , Peróxidos/química , Titanio
3.
Environ Res ; 210: 112937, 2022 07.
Artículo en Inglés | MEDLINE | ID: mdl-35157918

RESUMEN

The high-throughput production of the eco-friendly MIL-88A(Fe) was achieved under mild reaction conditions with normal pressure and temperature. The as-prepared MIL-88A(Fe) exhibited efficient photo-Fenton catalytic ofloxacin (OFL) degradation upon visible light irradiation with good stability and reusability. The OFL (20.0 mg/L) was completely degraded within 50 min under visible light with the aid of MIL-88A(Fe) (0.25 g/L) and H2O2 (1.0 mL/L) in aqueous solution (pH = 7.0). The hydroxyl radicals (·OH) are the main active species during the photo-Fenton oxidation process. Meanwhile, the degradation intermediates and the corresponding degradation pathways were identified and proposed with the aid of both ultra-high performance liquid chromatography tandem quadrupole time-of-flight mass spectrometry (UHPLC-Q-TOF-MS) and density functional theory (DFT) calculations. Finally, the degradation product library was firstly established to identify intermediate transformation products (TPs) with their variation of concentration, and their corresponding toxicologic activities were assessed via Toxtree and T.E.S.T software as well. Finally, the MIL-88A is efficient and stable with four cycles' catalysis operations, demonstrating good potential for water treatment.


Asunto(s)
Ofloxacino , Purificación del Agua , Catálisis , Peróxido de Hidrógeno/química , Ofloxacino/toxicidad , Purificación del Agua/métodos
4.
Environ Sci Technol ; 55(12): 8341-8350, 2021 06 15.
Artículo en Inglés | MEDLINE | ID: mdl-34076409

RESUMEN

Defective MIL-88B(Fe) nanorods are exploited as exemplary iron-bearing metal-organic framework (MOF) catalyst for molecular oxygen (O2) activation at ambient temperature, triggering effective catalytic oxidation of formaldehyde (HCHO), one of the major indoor air pollutants. Defective MIL-88B(Fe) nanorods, growing along the [001] direction, expose abundant coordinatively unsaturated Fe-sites (Fe-CUSs) along extended hexagonal channels with a diameter of ca. 5 Å, larger enough for the diffusion of O2 (3.46 Å) and HCHO (2.7 Å). The Lewis acid-base interaction between Fe-CUSs and accessible HCHO accelerates the FeIII/FeII cycle, catalyzing Fenton-like O2 activation to produce reactive oxidative species (ROSs), including superoxide radicals (•O2-), hydroxyl radicals (•OH), and singlet oxygen (1O2). Consequently, adsorbed HCHO can be oxidized into CO2 with a considerable mineralization efficiency (over 80%) and exceptional recyclability (4 runs, 48 h). Dioxymethylene (CH2OO), formate (HCOO-) species, and formyl radicals (•CHO) are recorded as the main reaction intermediates during HCHO oxidation. HCHO, H2O, and O2 are captured and activated by abundant FeIII/FeII-CUSs as acid/base and redox sites, triggering synergetic ROS generation and HCHO oxidation, involving cooperative acid-base and redox catalysis processes. This study will bring new insights into exploiting novel MOF catalysts for efficient O2 activation and reliable indoor air purification at ambient temperature.


Asunto(s)
Compuestos Férricos , Nanotubos , Catálisis , Formaldehído , Oxidación-Reducción , Oxígeno , Temperatura
5.
Environ Sci Technol ; 55(19): 13209-13218, 2021 10 05.
Artículo en Inglés | MEDLINE | ID: mdl-34553909

RESUMEN

The introduction of defects into hierarchical porous metal-organic frameworks (HP-MOFs) is of vital significance to boost their adsorption performance. Herein, an advanced template-assisted strategy has been developed to fine-tune the phosphate adsorption performance of HP-MOFs by dictating the type and number of defects in HP-UiO-66(Zr). To achieve this, monocarboxylic acids of varying chain lengths have been employed as template molecules to fabricate an array of defect-rich HP-UiO-66(Zr) derivatives following removal of the template. The as-prepared HP-UiO-66(Zr) exhibits a higher sorption capacity and faster sorption rate compared to the pristine UiO-66(Zr). Particularly, the octanoic acid-modulated UiO-66(Zr) exhibits a high adsorption capacity of 186.6 mg P/g and an intraparticle diffusion rate of 6.19 mg/g·min0.5, which are 4.8 times and 1.9 times higher than those of pristine UiO-66(Zr), respectively. The results reveal that defect sites play a critical role in boosting the phosphate uptake performance, which is further confirmed by various advanced characterizations. Density functional theory (DFT) calculations reveal the important role of defects in not only providing additional sorption sites but also reducing the sorption energy between HP-UiO-66(Zr) and phosphate. In addition, the hierarchical pores in HP-UiO-66(Zr) can accelerate the phosphate diffusion toward the active sorption sites. This work presents a promising route to tailor the adsorption performance of MOF-based adsorbents via defect engineering.


Asunto(s)
Estructuras Metalorgánicas , Fosfatos , Adsorción , Porosidad
6.
Environ Sci Technol ; 55(6): 4045-4053, 2021 03 16.
Artículo en Inglés | MEDLINE | ID: mdl-33625227

RESUMEN

Herein, a silicate-enhanced flow-through electro-Fenton system with a nanoconfined catalyst was rationally designed and demonstrated for the highly efficient, rapid, and selective degradation of antibiotic tetracycline. The key active component of this system is the Fe2O3 nanoparticle filled carbon nanotube (Fe2O3-in-CNT) filter. Under an electric field, this composite filter enabled in situ H2O2 generation, which was converted to reactive oxygen species accompanied by the redox cycling of Fe3+/Fe2+. The presence of the silicate electrolyte significantly boosted the H2O2 yield by preventing the O-O bond dissociation of the adsorbed OOH*. Compared with the surface coated Fe2O3 on the CNT (Fe2O3-out-CNT) filter, the Fe2O3-in-CNT filter demonstrated 1.65 times higher kL value toward the degradation of the antibiotic tetracycline. Electron paramagnetic resonance and radical quenching tests synergistically verified that the dominant radical species was the 1O2 or HO· in the confined Fe2O3-in-CNT or unconfined Fe2O3-out-CNT system, respectively. The flow-through configuration offered improved tetracycline degradation kinetics, which was 5.1 times higher (at flow rate of 1.5 mL min-1) than that of a conventional batch reactor. Liquid chromatography-mass spectrometry measurements and theoretical calculations suggested reduced toxicity of fragments of tetracycline formed. This study provides a novel strategy by integrating state-of-the-art material science, Fenton chemistry, and microfiltration technology for environmental remediation.


Asunto(s)
Peróxido de Hidrógeno , Hierro , Catálisis , Oxidación-Reducción , Silicatos
7.
Environ Res ; 201: 111596, 2021 10.
Artículo en Inglés | MEDLINE | ID: mdl-34224713

RESUMEN

Hydroxyl modified UiO-66 ((OH)2-UiO-66-X%, X represents the mass content ratio of introduced 2,5-dihydroxyterephthalic acid) was prepared via a solvothermal reaction between zirconium tetrachloride, benzene-1,4-dicarboxylic acid (H2BDC), as well as 2,5-dihydroxyterephthalic acid (H2BDC-(OH)2). It was found that hydroxyl groups can act as the intramolecular hole scavenger to boost the photo-induced charge carrier separation to enhance Cr(VI) reduction. The photocatalytic Cr(VI) reduction activities of (OH)2-UiO-66-X% were investigated upon the irradiation of low-power ultraviolet LED light. The findings demonstrated that (OH)2-UiO-66-20% with good cyclicity and stability exhibited superior photocatalytic performances to both UiO-66 and (OH)2-UiO-66. The introduction of hydroxyl groups can also extend the light absorption region to longer wavelength in visible range, which provides possibility for displaying photocatalytic activities under sunlight. The effect of small molecule organic acid (SOAs), pH value, and co-existing inorganic ions on photocatalytic performances of (OH)2-UiO-66-20% were investigated. Tartaric acid (TA) as typical SOAs was introduced to the reaction system to further boost the photocatalytic Cr(VI) reduction via acting as hole scavenger, constructing charge-transfer-complex for quick electron transportation, and producing COO·- radicals. This work opened a new opportunity for modified MOFs for boosted elimination activities for environmental pollutants.


Asunto(s)
Ligandos , Cromo , Tartratos
8.
Chem Commun (Camb) ; 60(64): 8350-8359, 2024 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-39028126

RESUMEN

Metal-organic frameworks (MOFs) have become a hot spot in the area of functional materials and have undergone rapid development in a wide range of fields in the 21st century. However, the scalable application of MOFs is still constrained by high production cost at the front end. Additionally, systematic discussion of the reuse of spent MOFs is lacking. Encouragingly, an increasing number of studies have been focusing on the low-cost production and recycling of MOF-based materials, providing feasible solutions for resource recovery and reduction. To stimulate future enthusiasm and interest in realizing the blue economy of MOFs, ranging from front-end production to terminal disposal, we have presented and summarized the state-of-the-art progress in the sustainable synthesis, separation, and reuse of MOFs. Based on the existing challenges, we also propose fit-for-purpose future directions in the MOF field to move toward blue economy.

9.
Chem Commun (Camb) ; 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39145466

RESUMEN

A durable and efficient hydrophobic/superoleophilic MIL-88A(Fe)@sponge (MS) with high throughput was fabricated via the dip-coating technique. Its adsorption capacities for pump oil, peanut oil, and CCl4 were 32.13 g g-1, 34.85 g g-1, and 34.25 g g-1, respectively. The hydrophobic surface of MS has excellent chemical resistance and physical stability in harsh environments.

10.
Dalton Trans ; 53(11): 5266-5273, 2024 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-38407245

RESUMEN

In this work, a three-dimensional bimetallic metal-organic framework (BMOF), BUC-101 (Co/Mn-H6chhc, H6chhc = cis-1,2,3,4,5,6-cyclohexane-hexacarboxylic acid, BUC = Beijing University of Civil Engineering and Architecture) was synthesized by a one-pot solvothermal method and characterized in detail by single crystal X-ray diffraction (SCXRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) element mapping analysis. BUC-101 showed excellent catalytic peroxymonosulfate (PMS) activation performance to degrade rhodamine B (RhB) without energy input. In addition, BUC-101 can maintain good stability and recyclability during the PMS activation processes, in which 99.9% RhB degradation efficiencies could be accomplished in 5 operational runs. The possible PMS activation and RhB degradation mechanisms of the BUC-101/PMS system were proposed and affirmed.

11.
Chem Commun (Camb) ; 60(27): 3713-3716, 2024 Mar 28.
Artículo en Inglés | MEDLINE | ID: mdl-38477555

RESUMEN

Co2P/tetrasodium diphosphate (TD) derived from ZIF-67/sodium phytate was newly developed and synthesized, and exhibited excellent degradation ability toward various refractory organics via peroxymonosulfate activation. A corresponding reaction mechanism was proposed. In addition, a continuous-flow operation of phenol degradation was realized.

12.
J Hazard Mater ; 472: 134420, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38691997

RESUMEN

In this work, MIL-88A(Fe) was immobilized onto the expanded perlites to fabricate the floating MIL-88A(Fe)@expanded perlites (M@EP) catalyst via high throughput batch synthesis method under room temperature. The as-prepared M@EP could efficiently activate H2O2 to achieve 100% tetracycline antibiotics (TCs) removal under both artificial low power UV light (UVL) and real sunlight (SL) irradiation. The toxicological evaluation, growth experiment of mung beans and antimicrobial estimation revealed the decreasing aquatic toxicity of the TCs intermediates compared to those of the pristine TCs. A self-designed continuous bed reactor was employed to investigate the long-term operation of the M@EP. The findings demonstrated that the antibiotics mixture can be continuously degraded up to 7 days under UVL and 5 daytimes under SL irradiation, respectively. More importantly, ca. 76.9% and 81.6% of total organic carbon (TOC) removal efficiencies were accomplished in continuous bed reactor under UVL and SL irradiation, respectively. This work advances the immobilized MOFs on floating supports for their practical application in large-scale wastewater purification through advanced oxidation processes. ENVIRONMENTAL IMPLICATION: This work presented the high throughput production and photo-Fenton degradation application of floating MIL-88A(Fe)@expanded perlites (M@EP). Three tetracycline antibiotics (TCs) were selected as model pollutants to test the degradation ability of M@EP in batch experiment and continuous operation under artificial light and solar light. The complete TCs degradation could be accomplished in self-designed device up to 7 d under UV light and 5 d under real solar light. This work tapped a new door to push MOFs-based functional materials in the real water purification.

13.
Nat Commun ; 15(1): 7208, 2024 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-39174565

RESUMEN

Catalytic peroxymonosulfate (PMS) activation processes don't solely rely on electron transfer from dominant metal centers due to the complicated composition and interface environment of catalysts. Herein the synthesis of a cobalt based metal-organic framework containing polyvanadate [V4O12]4- cluster, Co2(V4O12)(bpy)2 (bpy = 4,4'-bipyridine), is presented. The catalyst demonstrates superior degradation activity toward various micropollutants, with higher highest occupied molecular orbital (HOMO), via nonradical attack. The X-ray absorption spectroscopy and density functional theory (DFT) calculations demonstrate that Co sites act as both PMS trapper and electron donor. In situ spectral characterizations and DFT calculations reveal that the terminal oxygen atoms in the [V4O12]4- electron sponge could interact with the terminal hydrogen atoms in PMS to form hydrogen bonds, promoting the generation of SO5* intermediate via both dynamic pull and direct electron transfer process. Further, Co2(V4O12)(bpy)2 exhibits long-term water purification ability, up to 40 h, towards actual wastewater discharged from an ofloxacin production factory. This work not only presents an efficient catalyst with an electron sponge for water environmental remediation via nonradical pathway, but also provides fundamental insights into the Fenton-like reaction mechanism.

14.
Chemosphere ; 322: 138221, 2023 May.
Artículo en Inglés | MEDLINE | ID: mdl-36828116

RESUMEN

FT-x composites with core-shell structure (FT = FeS2@TiO2, x represents the mass ratio of the used FeCl3·6H2O to MIL-125) were fabricated by a hydrothermal method using MIL-125(Ti) as a self-sacrificing template. Both the photo-Fenton activity and stability of the FT-1 were improved greatly in comparison with its counterparts due to the unique core-shell structure and synergistic effect between FeS2 and TiO2. Especially, the Fe leaching concentration of FT-1 was approximately 1/10 of the individual FeS2, benefiting from the protection effect of TiO2 shell. Under dark condition, the formed FeOOH occupied active sites and inhibited iron cycle as well as H2O2 decomposition, leading to the inactivation of FT-1. UV light irradiation not only boosted the catalytic activity but also prevented the FT-1 from reactivity decline owning to the regeneration of Fe2+ by photogenerated electrons and continuous generation of ·OH. Experimental and DFT calculation results indicated that a type-II heterojunction was formed, in which photogenerated electrons were transferred from FeS2 core to TiO2 shell, accelerating charge separation and further boosting sulfamethoxazole (SMX) degradation. FT-1 displayed outstanding photo-Fenton activity in wide pH ranged from 2 to 6 and good anti-interfering ability toward impurities in water matrix. Besides, the reusability of FT-1 was good, in which 90% SMX degradation was maintained even after 5 runs. Noteworthy, the photo-Fenton activity was recovered via a revulcanization process, in which FeOOH was completely transformed into FeS2. This founding provided insights for the design and construction of heterojunction with both excellent photo-Fenton activity and stability.


Asunto(s)
Peróxido de Hidrógeno , Sulfametoxazol , Peróxido de Hidrógeno/química , Hierro/química , Titanio/química
15.
J Hazard Mater ; 445: 130552, 2023 03 05.
Artículo en Inglés | MEDLINE | ID: mdl-36502718

RESUMEN

For broad-spectrum adsorption and capture toward cationic metal ions, a facile strategy was adopted to fabricate defective SO3H-MIL-101(Cr) (SS-SO3H-MIL-101(Cr)-X, X = 2, 3, 4) with enhanced vacancies using seignette salt (SS) as the modulating agent. The boosted adsorption performances of SS-SO3H-MIL-101(Cr)-X toward eight different ions, including Ag+, Cs+, Pb2+, Cd2+, Ba2+, Sr2+, Eu3+ and La3+ in both individual component and mixed component systems, could be ascribed to the effective mass transfer resulting from the exposure of defective sites. Especially, the optimal SS-SO3H-MIL-101(Cr)-3 could remove all the selected metal cations to below the permissible limits required by the World Health Organization (WHO) in the continuous-flow water treatment system. Furthermore, SS-SO3H-MIL-101(Cr)-3 exhibited good adsorption capacity (189.6 mg·g-1) toward Pb2+ under neutral condition and excellent desorption recirculation performance (removal efficiency > 95% after 5 cycles). Moreover, the adsorption mechanism involved the electrostatic adsorption and coordinative interactions resulting from complexation between the adsorption active sites and targeted cations (like Cr-O-M and S-O-M), which were explored systematically via both X-ray photoelectron spectroscopy (XPS) determination and density functional theory (DFT) calculations. Overall, this work provided guidance for modulating SS-SO3H-MIL-101(Cr)-X to promote its potential application in widespread metal cations removal from wastewater.


Asunto(s)
Estructuras Metalorgánicas , Contaminantes Químicos del Agua , Plomo , Contaminantes Químicos del Agua/química , Estructuras Metalorgánicas/química , Iones , Cationes , Adsorción
16.
Antioxidants (Basel) ; 12(7)2023 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-37507885

RESUMEN

Zeolitic imidazolate framework-8 nanoparticles (ZIF-8 NPs) are typical metal-organic framework (MOF) materials and have been intensively studied for their potential application in drug delivery and environmental remediation. However, knowledge of their potential risks to health and the environment is still limited. Therefore, this study exposed female and male zebrafish to ZIF-8 NPs (0, 9.0, and 90 mg L-1) for four days. Subsequently, variations in their behavioral traits and brain oxidative stress levels were investigated. The behavioral assay showed that ZIF-8 NPs at 90 mg/L could significantly decrease the locomotor activity (i.e., hypoactivity) of both genders. After a ball falling stimulation, zebrafish exposed to ZIF-8 NPs (9.0 and 90 mg L-1) exhibited more freezing states (i.e., temporary cessations of movement), and males were more sensitive than females. Regardless of gender, ZIF-8 NPs exposure significantly reduced the SOD, CAT, and GST activities in the brain of zebrafish. Correlation analysis revealed that the brain oxidative stress induced by ZIF-8 NPs exposure might play an important role in their behavioral toxicity to zebrafish. These findings highlight the necessity for further assessment of the potential risks of MOF nanoparticles to aquatic species and the environment.

17.
Chemosphere ; 338: 139495, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37451638

RESUMEN

Cobalt 2-methylimidazole (ZIF-67) have abundant nitrogen and cobalt elements, which can be used as an excellent precursor for catalyst synthesis. In this study, a new Co, N co-doped carbon-based catalyst (Co-N-BC) was synthesized from ZIF-67 and biochar, which can significantly improve the degradation of 4-nitrophenol (4-NP) in catalytic ozonation. The mineralization rate of 4-NP achieves 65.8% within 60 min. The catalyst showed high recycling stability in the four cycles of reuse experiment. Different operating parameters, such as solution pH, the concentration of O3 and 4-NP, have been studied in the Co-N-BC catalytic ozonation. O3, O2-· and ·OH are determined as the main reactive species for 4-NP degradation, and ·OH is especially responsibly for 4-NP mineralization. The existence of inorganic ions, such as Cl-, NO2-, CO32- and PO43-, all significantly inhibited the degradation of 4-NP to different extend, respectively. The effect of substituent on a series of organics with similar structure of 4-NP was also investigated in Co-N-BC catalytic ozonation. This study provides a new composite material for heterogeneous catalytic ozonation, which is very promising in 4-NP contained complex wastewater treatment.


Asunto(s)
Ozono , Contaminantes Químicos del Agua , Ozono/química , Contaminantes Químicos del Agua/análisis , Catálisis , Cobalto/química
18.
J Colloid Interface Sci ; 649: 384-393, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37354795

RESUMEN

Constructing Fe-Cu bimetal catalysts is an efficient strategy to promote Fe(III)/Fe(II) cycle, whereas there is still a long way to go before fully understanding the role of the Cu in the catalysts. Herein, a new Fe-MOF namely BUC-96(Fe) was fabricated from FeSO4·7H2O, 4,4'-bipyridine (bpy) and 2,5-dihydroxyterephthalic acid (H4dhtp) by both hydrothermal reaction and microwave-assisted method. Also, bimetal BUC-96(FeCu-x) were obtained when the CuSO4 was added into the system identical to the synthesis process of BUC-96(Fe). Series BUC-96 MOFs showed good organics elimination performance via Fenton-like process, where 88.1% (k = 0.0672 min-1) of chloroquine phosphate (CQ, 20 mg/L) was decomposed over pristine BUC-96(Fe) within 30 min. Interestingly, nearly 100% CQ was degraded over BUC-96(FeCu-5) as catalyst under the identical conditions within 5 min, whose reaction rate (1.3527 min-1) was 20.1-fold higher than that of BUC-96. Additionally, BUC-96(FeCu-5) exhibited excellent Fenton-like oxidation degradation performance for 10 selected emerging organic pollutants. The reaction mechanism was studied in detail by experiments, and density functional theory (DFT) calculation. The results revealed that the introduced Cu not only accelerated Fe(III)/Fe(II) cycles, hydroxyl radical (·OH) generation, electron transfer, but also lowered H2O2 dissociated energy barrier. This work advanced the bimetal MOFs construction and application in wastewater treatment via Fenton-like process.

19.
Chemosphere ; 303(Pt 1): 134949, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35577127

RESUMEN

This state of the art review presented the photocatalytic reduction from highly toxic Cr(VI) to lowly toxic Cr(III) with metal-organic frameworks (MOFs) and their composites. The construction of composites facilitated the transportation of the photo-induced charges to enhance the Cr(VI) reduction, in which the corresponding mechanisms were clarified by both experimental tests and DFT calculations. The immobilized MOFs onto some substrates accomplished continuous operations toward Cr(VI) reduction even under real solar light. As well, the environmental applications of the Cr(VI) reduction were analyzed, in which the influence factors toward the Cr(VI) reduction were clarified. This review reported that a big breakthrough was achieved from the batch experiment to the continuous operation for Cr(VI) reduction, in which MOFs demonstrated a bright prospective in the field of photocatalytic Cr(VI) reduction.

20.
J Hazard Mater ; 426: 128134, 2022 03 15.
Artículo en Inglés | MEDLINE | ID: mdl-34959213

RESUMEN

The CoSx-CuSx was firmly immobilized on copper foam (CF) substrate to fabricate supported CoSx-CuSx/CF using ZIF-L(Co)/CF as a self-sacrificing template, in which CF substrate played an important role in improving the adhesion between CF and target catalyst as well as the interfacial interaction between CoSx and CuSx. The CoSx-CuSx/CF performed well in catalytic peroxymonosulfate (PMS) activation, which can accomplish 97.0% sulfamethoxazole (SMX) degradation within 10 min due to the special structure and Co2+ regeneration promoted by S2- and Cu+. The influences of pH, PMS dosage, catalyst dosage, co-existing anions and natural organic matter (NOM) on SMX removal were studied in detail. CoSx-CuSx/CF presented excellent catalytic activity and reusability, which might be fascinating candidate for real wastewater treatment. The possible pathway of SMX degradation was proposed, and the toxicity of the intermediates during the degradation process were evaluated. It is noteworthy that long-term continuous degradation of sulfonamide antibiotics was achieved using a self-developed continuous-flow fixed-bed reactor. This work demonstrated that CF as a substrate to fabricate supported catalysts derived from MOF had great potential in actual wastewater remediation.


Asunto(s)
Cobre , Contaminantes Químicos del Agua , Antibacterianos , Peróxidos , Sulfonamidas , Contaminantes Químicos del Agua/análisis
SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA