Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 60
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Water Sci Technol ; 89(3): 811-822, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38358504

RESUMO

Advanced oxidation technologies based on hydroxyl radical (•OH) and sulfate radical (SO4-•) are two common types of advanced oxidation technologies, but there are not many reports on the application of advanced oxidation methods in actual wastewater pretreatment. This article compares the pre-treatment performance of Fe2+/H2O2 and Fe2+/Persulfate systems in actual pharmaceutical wastewater, and combines EEM, GC-MS, and toxicity testing results to explore the differences in TOC, COD, and NH3-N removal rates, optimal catalyst dosage, applicable pH range, toxicity of effluent after reaction, and pollutant structure between the two systems. The results indicate that the Fe2+/H2O2 system has a higher pollutant removal rate (TOC: 71.9%, COD: 66.9%, NH3-N: 34.1%), but also requires a higher catalyst (Fe2+) concentration (6.0 g/L), and its effluent exhibits characteristic peaks of aromatic proteins. The Fe2+/Persulfate system has a wider pH range (pH ≈ 3-7) and is more advantageous in treating wastewater containing more cyclic organic compounds, but the effluent contains some sulfur-containing compounds. In addition, toxicity tests have shown that the toxicity reduction effect of the Fe2+/Persulfate system is stronger than that of the Fe2+/H2O2 system.


Assuntos
Poluentes Ambientais , Peróxido de Hidrogênio , Águas Residuárias , Cromatografia Gasosa-Espectrometria de Massas , Compostos de Enxofre , Preparações Farmacêuticas
2.
Water Res ; 249: 120950, 2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38056201

RESUMO

The efficient removal of emerging pollutant from water is the ultimate frontiers of advanced oxidation processes (AOPs), yet it is challenging to obtain higher catalytic activity and oxidation rate. Herein, a sustainable solution was proposed by optimizing the curvature of confined structure to modulate the electronic state of the active sites in nanochannels for improving the catalytic activity. In addition, the confined effect can enhance the oxidation rate by shorting the mass transfer of active species and pollutants. A void-nanoconfined nanoreactor was prepared by loading Fe2O3 into the nanochannels (<5 nm) of the hollow carbon sphere. An enhancement of 3 orders of magnitude was obtained in the degradation rate constant of void-nanoconfined catalytic system toward sulfamethoxazole (SMX) (6.25 min-1) compared with the non-confined system. The kinetics enhancement was attributed to the larger electron potential difference between the outer and inner nanochannel caused by the curvature increase of carbon sphere, accelerating the electron transfer, so that the energy barrier of SMX degradation reaction was reduced by 31 kcal/mol with the assistance of confinement energy. Importantly, the NC-IN/PDS system exhibited outstanding removal efficiency for the actual river water using a continuous flow reactor. This work provides a new insight into designing an efficient and stable catalytic nanoreactor, enriching the domain of advanced wastewater treatment strategies.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Domínio Catalítico , Oxirredução , Sulfametoxazol/química , Carbono , Água , Eletrônica , Poluentes Químicos da Água/química
3.
Small ; 20(7): e2307102, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37806750

RESUMO

The proton-coupled electron transfer(PCET) reaction plays a crucial role in the chemical transformation process andhas become one of the most concerned elementary reactions. However, the complex kinetics of PCET reaction, which requires the simultaneous transfer of protons and electrons, leads to the dilemma that thermodynamics and kinetics cannot bebalanced and restricts its further development. In this, an interface micro-electric field (IMEF) basedon Fe─N4 in FeMOFs (Fe-Based Metal-Organic Frameworks) glass is designed tosynchronize proton/electron interface behavior for the first time to realizeefficient PCET reaction and optimize reaction thermodynamics and kinetics. The IMEF facilitates the separation of photogenerated electrons and holes, and accelerates Fe(III)/Fe(II) cycle. Driven by near-surface electric field force, the protons near surfacemigrate to Fe sites and participate in Fe(IV)═O formation and reaction, lowering the reaction energy barrier. Based on the interface regulation ofIMEF, a high-efficiency PCET reaction is realized, and kinetic reactionrate constant of photocatalytic oxidation of emerging contaminants is increasedby 3.7 times. This study highlights a strategy for IMEFs to modulate PEC Treactions for a wide range of potential applications, including environmental and ecological applications.

4.
Environ Res ; 221: 115315, 2023 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-36657591

RESUMO

In this study, the denitrification efficacy of corn cob hydrolysate (CCH) was compared and analyzed with that of glucose and acetate to determine its feasibility as an additional carbon source, and its metabolic mechanism as a denitrification carbon source was investigated in depth. By constructing a denitrification reactor, it was found that the TN removal rate exceeded 97% and the effluent COD remained below 70 mg/L during the stable operation with CCH as the carbon source, and the denitrification effect was comparable to that of the glucose stage (GS) and the acetate stage (AS). The analysis of the microbial community showed that the dominant phylum was Proteobacteria and Bacteroidota, where the abundance of Bacteroidota in the hydrolysate stage (HS) (24.37%) was significantly higher than that of GS (4.89%) and AS (11.93%). And the analysis at the genus level showed the presence of a large number of genera of organic matter hydrolysis and acid production in HS that were almost absent in other stages, such as Paludibacter (12.83%), Gracilibacteria (4.27%), f__Prolixibacteraceae_Unclassified (2.94%). In addition, the higher fatty acid metabolism and lower sugar metabolism of HS during carbon metabolism were similar to the ratio of AS, suggesting that CCH was mainly fermented to acids and then involved in the tricarboxylic acid (TCA) cycle. During nitrogen metabolism, the high relative abundance of narG, nirS, and nosZ ensured the denitrification process. The results of this study were expected to provide a theoretical basis and data support for promoting denitrification from novel carbon sources.


Assuntos
Microbiota , Zea mays , Carbono , Desnitrificação , Bactérias , Nitrogênio , Reatores Biológicos/microbiologia
5.
Chemosphere ; 297: 134100, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35219710

RESUMO

In this study, a novel polydopamine (PDA)-modified metal organic frameworks (MOFs) catalyst (MIL/PDA) was successfully fabricated to activate persulfate (PS) for the degradation of sulfamethoxazole (SMX) in wastewater. The experimental results indicated that PDA-modified catalyst exhibited superior catalytic performance and enhanced the degradation of SMX (91.5%) compared to pure MOFs. The physical-chemical properties of the MIL/PDA catalyst were comprehensively characterized, and the applications in the catalytic degradation of SMX were evaluated. It was found that the modification of PDA enhanced the electron transfer, while promoting the redox cycle of Fe(III)/Fe(II), which in turn boosted the production of active oxygen species. Furthermore, MIL/PDA showed high stability and reusable performance over multiple cycles. Both radical and non-radical pathways were jointly involved in the activation process of PS were confirmed by quenching experiments combined with electron paramagnetic resonance (EPR). Based on this, the possible mechanism of the catalytic reaction was investigated. Finally, five degradation pathways of SMX degradation were proposed according to the results of liquid chromatography-mass spectrometry (LC-MS). This work provided a new insight into the design of novel and efficient heterogeneous catalysts for advanced wastewater treatment.


Assuntos
Estruturas Metalorgânicas , Poluentes Químicos da Água , Compostos Férricos , Indóis , Polímeros , Sulfametoxazol/química , Águas Residuárias/análise , Poluentes Químicos da Água/análise
6.
J Hazard Mater ; 429: 128299, 2022 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-35077971

RESUMO

Metal-organic frameworks (MOFs) have attracted more attention because of their excellent environmental catalytic capabilities. Modulation approach as an advanced assistant strategy is vital essential to enhancing the performance of MOFs. In this study, the modulated method was used to successfully synthesize a group of Fe-based MOFs, with formic acid as the modulator on the synthesis mixture. The most modulated sample Fe-MOFs-2 exhibit high specific surface areas and higher catalytic activity, which could effectively degrade SMX via PS activation, with almost 95% removal efficiency within 120 min. The results revealed that the % RSE of modulated Fe-MOFs-2 increased from 2.31 to 3.27 when compared with the origin Fe-MOFs. This may be due to the addition of formic acid induces the formation of more coordinatively unsaturated metal sites in the catalyst, resulting in structural defects. In addition, the quenching experiment and EPR analysis verified SO4-·and·OH as the major active free radicals in the degradation process. Modulated Fe-MOFs-2 demonstrated good reusability and stability under fifth cycles. Finally, four possible degradation pathways and catalytic mechanism of Fe-MOFs-2 was tentatively proposed. Our work provides insights into the rational design of modulated Fe-MOFs as promising heterogeneous catalysts for advanced wastewater treatment.


Assuntos
Estruturas Metalorgânicas , Purificação da Água , Catálise , Formiatos , Sulfametoxazol
7.
J Hazard Mater ; 424(Pt A): 127380, 2022 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-34879571

RESUMO

Developing high-efficient catalysts is crucial for activating peroxymonosulfate (PMS). Fe-N-C catalysts exhibit excellent performance for PMS activation because of the contribution of doped N, Fe-Nx and Fe3C sites. In our work, a series of Fe-N-C catalysts with high-performance was obtained by pyrolyzing Fe-Zn-MOFs precursors. During pyrolysis process, the change of chemical bonds and formation of active sites in the precursor were elucidated by characterization analysis and related catalytic experiments. Graphitic N, Fe-Nx and Fe3C were confirmed to activate PMS synergistically for ciprofloxacin (CIP) degradation. Besides, the catalytic performance was proportional to the amount of doped iron and calcination temperature. Moreover, the Fe-N-C-3-800/PMS system not only displayed good recycling performance, but also had high anti-interference ability. Integrated with quenching and electron paramagnetic resonance (EPR) experiments, a non-radical pathway dominated by 1O2 was proposed. Furthermore, PMS could bond to Fe-N-C-3-800 to form intermediate for charge transfer, thus accelerate electron transfer between CIP and PMS to realize degradation of CIP. Six main pathways of CIP degradation were proposed, which include bond fission of N-C on piperazine ring and direct oxidation of CIP. This study provided a new idea for the design of heterogeneous carbon catalysts in advanced oxidation field.


Assuntos
Ciprofloxacina , Peróxidos , Catálise , Zinco
8.
Front Microbiol ; 12: 755398, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34621262

RESUMO

The deinking pulp (DIP) is a main resource for paper making, and the wastewater from DIP process needs to be treated. Anaerobic biochemical technique has been widely applied in DIP wastewater treatment, due to the remarkable capability in reducing high chemical oxygen demand (COD). In this study, a mathematical simulation model was established to investigate the performance of a full-scale anaerobic biochemical system for treating DIP wastewater. The model was based on Anaerobic Digestion Model No. 1 (ADM1), which was modified according to the specific anaerobic digestion process for DIP wastewater treatment. The hydrodynamic behavior of a full-scale anaerobic biochemical system was considered in this model. The characteristics of the influent DIP wastewater were assessed, and then, the substrate COD proportion was divided successfully for the necessity of ADM1 applying. The Monte Carlo technique was implemented to distinguish the most sensitive parameters that influenced the model output indicators comprising effluent COD and biogas production. The sensitive parameters were estimated and optimized. The optimized value of k _m_pro is 12.02, K _S_pro is 0.35, k _m_ac is 4.26, K _S_ac is 0.26, k _m_h2 is 16.62, and K _S_h2 is 3.21 × 10-5. The model was calibrated with 150 days operation values measured in the field. The subsequent 100 days on-site values were used to validate the model, and the results obtained by the simulations were in good agreement. This study provides a meaningful and theoretical model guidance for full-scale wastewater anaerobic biochemical treatment simulation.

9.
Huan Jing Ke Xue ; 42(7): 3392-3399, 2021 Jul 08.
Artigo em Chinês | MEDLINE | ID: mdl-34212665

RESUMO

During wastewater treatment using a traditional biological denitrification process, the excessive concentration of nitrate nitrogen (NO3--N) in the effluent is the primary cause of excessive total nitrogen (TN) generation. By using an external carbon source to increase the carbon to nitrogen ratio (C/N), the denitrification process can be strengthened, which effectively addresses this problem. Using an integrated denitrification reactor developed based on the two-stage denitrification process principle with the addition of polybutylene succinate (PBS) in the second stage, the denitrification process was analyzed using a scanning electron microscope before and after characterization of PBS materials. Moreover, amplicon sequencing was used for in-depth exploration of changes in the microbial community structure in the second denitrification pool before and after the addition of PBS. The data of a continuous 120-day experiment showed that the COD removal rate dropped from 95.7% to 90.8%, the TN removal rate increased from 51.8% to 80%, the relative abundance of Proteobacteria phylum rose from 36.1% to 46.1%, and the relative abundance of Thermomonas rose from 6.47% to 13.48%. The results show that after the addition of PBS, PBS can not only provide carbon source for denitrification, but its surface can also serve as a carrier for microbial growth and attachment, play a good role in filming, and increase the abundance of denitrifying bacteria and strengthen denitrification. During the nitrification process, denitrification performance was significantly enhanced, effectively improving the TN removal rate of the system.


Assuntos
Carbono , Desnitrificação , Reatores Biológicos , Nitrificação , Nitrogênio , Águas Residuárias
10.
J Hazard Mater ; 411: 125194, 2021 06 05.
Artigo em Inglês | MEDLINE | ID: mdl-33858121

RESUMO

The poor water stability of metal-organic frameworks (MOFs) significantly hindered their catalytic application in advanced oxidation system. A protective outer layer was an effective strategy to solve this problem. However, the commonly used coating techniques are too complicated or too difficult to accurately control, thus, the applicability was relatively low. In this study, a water stable MOF core-SiO2 shell nanomaterial (Fe-MOF-74@SiO2) was synthesized by a facile hydrothermal method, and applied to activate persulfate (PS) for dimethyl phthalate (DMP) degradation. The catalyst water stability and DMP degradation in the system were investigated, suggesting that the SiO2-coated catalyst was more stable and exhibited higher DMP degradation efficiency over the pure MOF. It was found that pH had negligible effects on Fe-MOF-74@SiO2 + PS system, while, higher temperature facilitated the degradation of DMP. The activation mechanism was studied by quenching experiments combined with electron paramagnetic resonance, indicating that SO4⋅- played a major role in the activation of PS with Fe-MOF-74@SiO2 for DMP removal, while ⋅OH also involved in the catalytic process. Finally, possible DMP degradation pathways were proposed. These findings indicated that the core-shell structured Fe-MOF-74@SiO2 showed promise for DMP degradation by PS advanced oxidation system.

11.
Environ Sci Pollut Res Int ; 28(32): 43815-43830, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-33840030

RESUMO

In this work, Co-Ce-Zr/γ-Al2O33 particle electrodes were prepared for the efficient degradation of ciprofloxacin (CIP). Co-Ce-Zr/γ-Al2O3 particle electrodes were analyzed with a scanning electron microscope (SEM), X-Ray Diffraction (XRD), X-Ray Fluorescence Spectrometer (XRF), X-ray photoelectron spectroscopy (XPS), and energy-dispersive X-ray spectroscopy (EDS). According to the results, significant amounts of Co3O4, CeO2, and ZrO2 were formed on the Co-Ce-Zr/γ-Al2O3 particle electrodes. It was shown that when the conditions of the reaction system were at pH=6, conductivity of 4 ms/cm, current of 0.2 A, initial pollutant concentration of 100 mg/L, and material dosage of 15 g, CIP could be completely degraded within 40 min, and the energy consumed in the reaction was 41.3 kWh/kg CIP. The rate of total organic carbon (TOC) removal by Co-Ce-Zr/γ-Al2O3 particle electrodes was recorded to be approximately 52.6%. Using a response surface methodology, we explored the optimal operating conditions. At the same time, we also explored the influence of inorganic anions in water and actual water medium on the rate of CIP removal. In addition, the ESR data proved that the main active substance in the reaction system was ·OH. The degradation intermediates were investigated, and the possible mechanism was proposed. Thus, this research provided a new solution for the treatment of antibiotic-containing wastewater.


Assuntos
Ciprofloxacina , Poluentes Químicos da Água , Ciprofloxacina/análise , Eletrodos , Oxirredução , Águas Residuárias , Poluentes Químicos da Água/análise
12.
Chemosphere ; 273: 130269, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33773811

RESUMO

Heterogeneous electro-Fenton (E-F) is considered as an attractive technique for efficient removal of refractory organic pollutants in wastewater. The regeneration of FeII and catalyst reusability are key issues for effective and sustainable degradation. Developing binder-free iron phase/carbon composite cathode is a feasible strategy. In this work, the stable Ce/Fe-nanoporous carbon modified graphite felt electrode (Ce/Fe@NPC-GF) was fabricated using in situ solvothermal method and subsequent carbonization treatment, which worked as the cathode in a heterogeneous electro-Fenton system to degrade sulfamethoxazole. The electrocatalytic activity was significantly improved with doping of Ce. It was found that mesoporous Ce/Fe@NPC-GF cathode demonstrated high oxygen reduction activity and low resistance. The co-existence of FeⅡ/FeⅢ and CeⅢ/CeⅣ redox couples enhanced remarkably interfacial electron transfer, promoting in-situ H2O2 generation and decomposition, sequentially boosting the production of reactive radicals (·OH and ·O2-). Under 20 mA and pH 3, Sulfamethoxazole (SMX) was basically degraded in 120 min, and the removal rate was satisfactory in wide pH (2-6). After 8 cycles, the electrode could still maintain high stability and outstanding catalytic capacity. This work displayed a novel in-situ preparation method of composite cathode with excellent catalytic performance in E-F system, which offered inspiration for developing efficient heterogeneous electro-Fenton cathode material.


Assuntos
Peróxido de Hidrogênio , Poluentes Químicos da Água , Catálise , Eletrodos , Compostos Férricos , Oxirredução , Águas Residuárias
13.
Chemosphere ; 273: 129747, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33540330

RESUMO

The traditional Electro-Fenton (EF) is an efficient technology for wastewater treatment but suffers from the acidic condition requirement and external catalyst addition. To overcome these challenges, a GF@MoS2@FeOCl cathode was fabricated using a facile method. The as-prepared GF@MoS2@FeOCl cathode showed excellent performance for ciprofloxacin (CIP) degradation in EF process with RuO2/Ti electrode as the anode. H2O2 was electro-generated and activated on-site at the cathode at mild pH without adding Fe2+. CIP was 100% removed with 74.4% of mineralization in 90 min at pH 6. The GF@MoS2@FeOCl cathode exhibited good reusability after consecutive runs of degradation. The degradation intermediates were investigated, and the possible mechanism was proposed. This work demonstrated that the prepared GF@MoS2@FeOCl cathode is a promising candidate for contaminants treatment in an EF system.


Assuntos
Grafite , Poluentes Químicos da Água , Antibacterianos , Ciprofloxacina , Eletrodos , Peróxido de Hidrogênio , Concentração de Íons de Hidrogênio , Ferro , Molibdênio , Oxirredução
14.
Chemosphere ; 270: 128620, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33109356

RESUMO

Adsorptive removal of dimethyl phthalate (DMP) in water combined with advanced oxidation processes (AOPs) has attracted interest. In this work, the adsorptive and catalytic properties of an Fe-based metal-organic framework (Fe-MOF-74) have been improved by molecular imprinting technique. The adsorption behaviors have been evaluated by the Freundlich and pseudo-second-order model. The results have shown that selective adsorption ability of the material for DMP was highly enhanced and chemisorption was dominating. A 1.5-fold increase in catalytic rate after being modified by molecular imprinting indicated that the selective adsorption is crucial. In the synergy of adsorption and catalysis, DMP was first specifically adsorbed on the surface of the material by hydrogen bonds and electrostatic interactions. Then, hydroxyl radicals and sulfate radicals, which were both generated via activation of persulfate (PS), catalytically oxidized DMP. The degradation rate can rapidly reach around 90% in 30 min and three possible degradation pathways were proposed. The molecular imprinting modified catalyst can be used for DMP effective degradation in water.


Assuntos
Impressão Molecular , Ácidos Ftálicos , Poluentes Químicos da Água , Adsorção , Catálise , Oxirredução
15.
J Hazard Mater ; 398: 123024, 2020 11 05.
Artigo em Inglês | MEDLINE | ID: mdl-32768834

RESUMO

In this work, ZSM-5-(C@Fe), as a peroxymonosulfate (PMS) heterogeneous activator, was synthesized, characterized, and evaluated for activating PMS to degrade ciprofloxacin (CIP) in wastewater. Zeolite Socony Mobil-5 (ZSM-5) was utilized to enhance structural stability and provided a scaffold to graft Fe doping C nanocomposites activator. Pyrolytic metal-organic frameworks (MOFs) can use crystal structure to construct stable carbon-encapsulated Fe nanocomposites. The formation of C-O-Si, C-O-Al and C-Fe was the key to the stability of catalysts. Fe doping in ZSM-5-(C@Fe) formed non-radical degradation pathway was the key to improve the degradation efficiency. The experimental data indicated ZSM-5-(C@Fe) could completely remove 20 mg L-1 CIP within 15 min and achieve good results in the experiments of treating actual wastewater, which could reduce 40% COD of the paper mill aerobic pond effluent. The Fukui function calculation and UHPL C-H RMS/MS analysis elucidated that the 1O2-dominated electrophilic reaction and the ZSM-5-(C@Fe) complex PMS-dominated nucleophilic reaction were the main pathways for CIP degradation and the radical degradation pathway (·OH and SO4-˙) plays auxiliary role. In addition, two new degradation pathways of the N29 and C27 in quinolone ring and the N22 in piperazine ring were discovered. This finding had important implications for the removal of N from organic pollutants.


Assuntos
Ciprofloxacina , Zeolitas , Peróxidos , Águas Residuárias
16.
Bioprocess Biosyst Eng ; 43(6): 1093-1104, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32166399

RESUMO

A comprehensive model for nitrous oxide (N2O) emissions in an anaerobic/oxygen-limited aerobic (A/OLA) process is proposed here. This paper includes the following main innovations: (i) adding the phosphorus-accumulating organism (XPAO) denitrification pathway to the contribution of N2O emissions; (ii) considering the biological removal of organic matter and phosphorus and predicting the effect of influent phosphorus concentration on N2O emissions via an increase in the influent phosphorus concentration; and (iii) determining the effect of XPAO on N2O production in a simultaneous nitrification, denitrification and phosphorus removal (SNDPR) system by sensitivity analysis. The results suggested that the simulated data matched the measured data well. The predominant pathways of N2O emissions in the process of A/OLA were the ammonium-oxidizing bacterium (XAOB) denitrification pathway and the heterotrophic bacterium (XH) denitrification pathway, while the incomplete hydroxylamine (NH2OH) oxidation pathway and the XPAO denitrification pathway contributed less to N2O emissions. The metabolic activity of XPAO had a significant effect on N2O emissions, and increasing the influent phosphorus concentration was beneficial for reducing the release of N2O. This study is expected to provide a meaningful reference for reducing N2O emissions in wastewater treatment engineering.


Assuntos
Bactérias/crescimento & desenvolvimento , Reatores Biológicos , Modelos Biológicos , Óxido Nitroso/metabolismo , Oxigênio/metabolismo , Aerobiose , Anaerobiose
17.
Environ Sci Pollut Res Int ; 27(9): 9152-9166, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31916156

RESUMO

A novel adsorbent derived from banyan aerial roots was prepared via modification and employed to aqueous gentian violet (GV) and rhodamine B (RhB) removal. The surface morphology and physicochemical properties of modified banyan aerial roots (MBARs) were investigated by SEM, EDS, N2 adsorption/desorption, zeta potential, XRD, and FT-IR characterization experiments. Adsorption factors were tested, and the optimal conditions for GV and RhB removal were pH of 6 and 3, doses of 0.02 g and 0.03 g, and reaction time of 540 min. Adsorption isotherm simulation illustrated that theoretical monolayer adsorption capacities of GV and RhB were 456.64 mg/g and 115.23 mg/g, respectively. Kinetics data was assessed with pseudo-first-order and pseudo-second-order models, and the latter described GV and RhB adsorption better at 288 K, 298 K, 308 K, and 318 K. Thermodynamic analysis indicated that GV and RhB adsorption processes were endothermic and spontaneous. From the research results, it could be inferred that GV adsorption was mainly dominated by electrostatic interaction, while RhB adsorption might be primarily attributed to electrostatic interaction and hydrogen bonding. The study based on full utilization of waste plant fibers facilitates recycling of biomass resources, and due to simplicity, safety, and eco-friendliness of the preparation, as well as low cost and high efficiency of the application, MBARs may be potential absorbents for the treatment of dyestuff wastewater.


Assuntos
Rodaminas/química , Poluentes Químicos da Água , Purificação da Água , Adsorção , Violeta Genciana , Cinética , Espectroscopia de Infravermelho com Transformada de Fourier , Termodinâmica
18.
Chemosphere ; 240: 124849, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31561166

RESUMO

In this work, reduced graphene oxide/metal organic framework composites (RGO/MOF) have been fabricated for the purpose of activating persulfate (PS) successfully first time. Benefiting from the abundant active sites of composites and the excellent electron conductivity arising from repaired large π conjugate plane structure, RGO/MIL-101(Fe) performed better than RGO and MIL-101(Fe) for PS activation and organic compounds degradation from aqueous. The physical-chemical properties of composite catalysts were fully characterized and the applications to the catalytic degradation of trichlorophenol (TCP) were evaluated. The results showed that RGO/MIL-101(Fe) could effectively degrade TCP, under the reaction conditions of pH 3.0, 20 mg/L TCP, 20 mM PS, 0.5 g/L catalyst, and the removal efficiency is 92% in 180 min. Furthermore, chemical reduction and thermal process played key role in regulating defect levels and electron transfer channels. The obtained adsorptive and conductive graphene allow rapid electron transport between free radicals and enriched contaminants. These advancements of the structure and chemical properties were beneficial to improve the catalytic activity in the activation of PS. Finally, a possible activation mechanism was also investigated, which involved the prevailing free radical pathway and recessive non-radical pathway.


Assuntos
Clorofenóis/química , Grafite/química , Catálise
19.
Sci Total Environ ; 708: 134630, 2020 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-31806343

RESUMO

The study investigated ciprofloxacin (CIP) adsorption capacity of the novel biomaterials prepared from banyan aerial roots by simple thermochemical modification. Pretreated banyan aerial root fibers were modified with a green reagent citric acid (1 M) at 90, 120 and 150 °C, which enhanced the fiber adsorption capacity revealed by characterization and adsorption tests. Several characterization methods were applied to exploring the surface morphologies and physicochemical properties of unmodified banyan aerial roots (UBARs) and modified banyan aerial roots (T-MBARs, T stands for the modification temperature). Based on SEM images and N2 adsorption/desorption isotherms, the modification resulted in decrease of the specific surface area owing to cellulose molecular linking. In that case, the improved CIP adsorption of MBARs might be attributed to the larger carboxyl quantity and stronger electronegativity manifested via FTIR spectra and zeta potential analysis. Through the adsorption experiments, the optimal pH value of 8 and the suitable absorbent dosage of 0.03 g were obtained. The simulation results showed that the Freundlich model can fit the adsorption thermodynamic data quite well, while the kinetic data was simulated preferably by the pseudo-second-order kinetic equation signifying the chemical adsorption process, and the intra-particle diffusion was involved in the adsorption consisted of three stages. The findings of batch experiments under diverse operations represented that MBARs purified aqueous CIP better than UBARs, closely related to the superior electronegativity. Both characterization and adsorption studies illustrated the dominant role of electrostatic interaction during CIP removal, accompanied by hydrogen bonding and diffusion interaction besides. The present work suggested that MBAR fibers could possess a promising application to ciprofloxacin potent removal from aqueous solutions.


Assuntos
Ciprofloxacina/isolamento & purificação , Adsorção , Materiais Biocompatíveis , Concentração de Íons de Hidrogênio , Cinética , Poluentes Químicos da Água , Purificação da Água
20.
Environ Pollut ; 256: 113399, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31662253

RESUMO

Achieving large pore size, high catalytic performance with stable structure is critical for metal-organic frameworks (MOFs) to have more hopeful prospects in catalytic applications. Herein, we had reported a method to synthesize highly reactive yet stable defective iron-based Metal organic frameworks by using different monocarboxylic acids with varying lengths as a modulator. The physical-chemical characterization illustrating that modulators could improve the crystallinity, enlarge pore size and enhance catalytic performance and octanoic acid (OA) was screened to be the suitable choice. The catalytic performance of catalysts was detected through persulfate (PS) activation for degrading Tetrabromobisphenol A (TBBPA). The study demonstrated that the highest degradation efficiency for 0.018 mmol L-1 TBBPA was that 97.79% in the conditions of the 1.0 g L-1 Fe(BDC)(DMF,F)-OA-30 dosage and TBBPA:PS = 200:1. In addition, there was observed that no obvious change of the crystal structure, little the leachable iron concentration in the solutions and no significant loss of catalytic activities of Fe(BDC)(DMF,F)-OA-30 after 5th cycles. The iron valence state of Fe(BDC)(DMF,F)-OA-30 before and after degradation and electrochemical properties reveal that the partial substitution of organic ligands by octanoic acid, when removing OA and forming defects by heat and vacuum treatment to generate coordinatively unsaturated metal sites and accelerate the original transmission of electronic, leading to enhance the activity of persulfate activation for efficient removal TBBPA.


Assuntos
Modelos Químicos , Bifenil Polibromatos/química , Catálise , Ferro/química , Estruturas Metalorgânicas
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA
...