Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 105
Filtrar
Mais filtros

Base de dados
País/Região como assunto
Tipo de documento
Intervalo de ano de publicação
1.
Environ Sci Technol ; 58(16): 7228-7236, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38551367

RESUMO

The development of electrocatalysts that can efficiently reduce nitrate (NO3-) to ammonia (NH3) has garnered increasing attention due to their potential to reduce carbon emissions and promote environmental protection. Intensive efforts have focused on catalyst development, but a thorough understanding of the effect of the microenvironment around the reactive sites of the catalyst is also crucial to maximize the performance of the electrocatalysts. This study explored an electrocatalytic system that utilized quaternary ammonium surfactants with a range of alkyl chain lengths to modify an electrode made of carbon nanotubes (CNT), with the goal of regulating interfacial wettability toward NO3- reduction. Trimethyltetradecylammonium bromide with a moderate alkyl chain length created a very hydrophobic interface, which led to a high selectivity in the production of NH3 (∼87%). Detailed mechanistic investigations that used operando Fourier-transform infrared (FTIR) spectroscopy and online differential electrochemical mass spectrometry (DEMS) revealed that the construction of a hydrophobic modified CNT played a synergistic role in suppressing a side reaction involving the generation of hydrogen, which would compete with the reduction of NO3-. This electrocatalytic system led to a favorable process for the reduction of NO3- to NH3 through a direct electron transfer pathway. Our findings underscore the significance of controlling the hydrophobic surface of electrocatalysts as an effective means to enhance electrochemical performance in aqueous media.


Assuntos
Amônia , Eletrodos , Nanotubos de Carbono , Nitratos , Molhabilidade , Amônia/química , Nanotubos de Carbono/química , Nitratos/química , Oxirredução , Catálise
2.
Environ Sci Technol ; 58(4): 2144-2152, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38234209

RESUMO

The electrocatalytic nitrate reduction reaction (NO3RR) has recently emerged as a promising technique for readily converting aqueous nitrate (NO3-) pollutants into valuable ammonia (NH3). It is vital to thoroughly understand the mechanism of the reaction to rationally design and construct advanced electrocatalytic systems that can effectively and selectively drive the NO3RR. There are several natural enzymes that incorporate molybdenum (Mo) and that can activate NO3-. Based on this, a cadmium (Cd) single-atom anchored Mo2TiC2Tx electrocatalyst (referred to as CdSA-Mo2TiC2Tx) through the NO3RR to generate NH3 was rationally designed and demonstrated. In an H-type electrolysis cell and at a current density of 42.5 mA cm-2, the electrocatalyst had a Faradaic efficiency of >95% and an impressive NH3 yield rate of 48.5 mg h-1 cm-2. Moreover, the conversion of NO3- to NH3 on the CdSA-Mo2TiC2Tx surface was further revealed by operando attenuated total reflection Fourier-transform infrared spectroscopy and an electrochemical differential mass spectrometer. The electrocatalyst significantly outperformed Mo2TiC2Tx as well as reported state-of-the-art catalysts. Density functional theory calculations revealed that CdSA-Mo2TiC2Tx decreased the ability of the d-p orbital to hybridize with NH3* intermediates, thereby decreasing the activation energy of the potential-determining step. This work not only highlights the application prospects of heavy metal single-atom catalysts in the NO3RR but also provides examples of bio-inspired electrocatalysts for the synthesis of NH3.


Assuntos
Amônia , Nitratos , Cádmio , Molibdênio , Eletrodos
3.
Environ Sci Technol ; 57(8): 3434-3444, 2023 02 28.
Artigo em Inglês | MEDLINE | ID: mdl-36537350

RESUMO

Machine learning (ML) provides an efficient manner for rapid prediction of the life-cycle environmental impacts of chemicals, but challenges remain due to low prediction accuracy and poor interpretability of the models. To address these issues, we focused on data processing by using a mutual information-permutation importance (MI-PI) feature selection method to filter out irrelevant molecular descriptors from the input data, which improved the model interpretability by preserving the physicochemical meanings of original molecular descriptors without generation of new variables. We also applied a weighted Euclidean distance method to mine the data most relevant to the predicted targets by quantifying the contribution of each feature, thereby the prediction accuracy was improved. On the basis of above data processing, we developed artificial neural network (ANN) models for predicting the life-cycle environmental impacts of chemicals with R2 values of 0.81, 0.81, 0.84, 0.75, 0.73, and 0.86 for global warming, human health, metal depletion, freshwater ecotoxicity, particulate matter formation, and terrestrial acidification, respectively. The ML models were interpreted using the Shapley additive explanation method by quantifying the contribution of each input molecular descriptor to environmental impact categories. This work suggests that the combination of feature selection by MI-PI and source data selection based on weighted Euclidean distance has a promising potential to improve the accuracy and interpretability of the models for predicting the life-cycle environmental impacts of chemicals.


Assuntos
Meio Ambiente , Aquecimento Global , Humanos , Redes Neurais de Computação , Água Doce , Aprendizado de Máquina
4.
Environ Sci Technol ; 57(45): 17404-17414, 2023 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-37920955

RESUMO

Electrochemical advanced oxidation process (EAOP) is a promising technology for decentralized water decontamination but is subject to parasitic anodic oxygen evolution and formation of toxic chlorinated byproducts in the presence of Cl-. To address this issue, we developed a novel electrolytic process by water flow-driven coupling of anodic oxygen evolution reaction (OER) and cathodic molecular oxygen activation (MOA). When water flows from anode to cathode, O2 produced from OER is carried by water through convection, followed by being activated by atomic hydrogen (H*) on Pd cathode to produce •OH. The water flow-driven OER/MOA process enables the anode to be polarized at low potential (1.7 V vs SHE) that is lower than that of conventional EAOP whose •OH is produced from direct water oxidation (>2.3 V vs SHE). At a flow rate of 30 mL min-1, the process could achieve 94.8% removal of 2,4-dichlorophenol (2,4-DCP) and 71.5% removal of chemical oxygen demand (COD) within 45 min at an anode potential of 1.7 V vs SHE and cathode potential of -0.5 V vs SHE. To achieve the comparable 2,4-DCP removal performance, 4.3-fold higher energy consumption was needed for the conventional EAOP with titanium suboxide anode (anode potential of 2.9 V vs SHE), but current efficiency declined by 3.5 folds. Unlike conventional EAOP, chlorate and perchlorate were not detected in the OER/MOA process, because low anode potential <2.0 V vs SHE was thermodynamically unfavorable for the formation of chlorinated byproducts by anodic oxidation, indicated by theoretical calculations and experimental data. This study provides a proof-in-concept demonstration of water flow-driven OER/MOA process, representing a paradigm shift of electrochemical technology for water decontamination and prevention of chlorinated byproducts, making electrochemical water decontamination more efficient, more economic, and more sustainable.


Assuntos
Poluentes Químicos da Água , Água , Oxigênio , Descontaminação , Eletrólise , Oxirredução , Eletrodos , Poluentes Químicos da Água/química
5.
Environ Sci Technol ; 57(28): 10458-10466, 2023 07 18.
Artigo em Inglês | MEDLINE | ID: mdl-37387677

RESUMO

The growth of renewable energy industries and the ongoing need for fertilizer in agriculture have created a need for sustainable production of ammonia (NH3) using low-cost, environment-friendly techniques. The electrocatalytic nitrate (NO3-) reduction reaction (NO3RR) has the potential to improve both the management of environmental nitrogen and the recycling of synthetic nutrients. However, NO3RR is frequently hindered by the incomplete NO3- conversion, sluggish reaction kinetics, and suppression of the hydrogen evolution reaction (HER). Inspired by specific local electronic structures that are adjustable for single-atom catalysts, this work presents a nanohybrid electrocatalytic filter with iron single atoms (FeSA) immobilized on MXene. The fabricated FeSA/MXene filter exhibited maximum NH3 Faradaic efficiency and selectivity (82.9 and 99.2%, respectively) that were higher than those for filters made of Fe nanoparticles anchored on MXene (FeNP/MXene) (69.2 and 81.3%, respectively) and MXene alone (32.8 and 52.4%, respectively), measured at an initial pH of 7 and an applied potential of -1.4 V vs Ag/AgCl. Density functional theory calculations revealed that, compared to the FeNP/MXene filter, the FeSA/MXene filter prevented the competition from the HER and reduced the activation energy of the potential-limiting step (*NO to *NHO) that made the NH3 synthesis thermodynamically favorable . This work highlights an alternative strategy for achieving a synergistic NO3- removal and nutrient recovery with durable catalytic activity and stability.


Assuntos
Amônia , Nitratos , Eletrodos , Hidrogênio , Ferro
6.
Environ Sci Technol ; 57(46): 17990-18000, 2023 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-37189261

RESUMO

In this study, a machine learning (ML) framework is developed toward target-oriented inverse design of the electrochemical oxidation (EO) process for water purification. The XGBoost model exhibited the best performances for prediction of reaction rate (k) based on training the data set relevant to pollutant characteristics and reaction conditions, indicated by Rext2 of 0.84 and RMSEext of 0.79. Based on 315 data points collected from the literature, the current density, pollutant concentration, and gap energy (Egap) were identified to be the most impactful parameters available for the inverse design of the EO process. In particular, adding reaction conditions as model input features allowed provision of more available information and an increase in the sample size of the data set to improve the model accuracy. The feature importance analysis was performed for revealing the data pattern and feature interpretation by using Shapley additive explanations (SHAP). The ML-based inverse design for the EO process was generalized to a random case for tailoring the optimum conditions with phenol and 2,4-dichlorophenol (2,4-DCP) serving as model pollutants. The resulting predicted k values were close to the experimental k values by experimental verification, accounting for the relative error lower than 5%. This study provides a paradigm shift from conventional trial-and-error mode to data-driven mode for advancing research and development of the EO process by a time-saving, labor-effective, and environmentally friendly target-oriented strategy, which makes electrochemical water purification more efficient, more economic, and more sustainable in the context of global carbon peaking and carbon neutrality.


Assuntos
Poluentes Ambientais , Purificação da Água , Carbono , Aprendizado de Máquina , Oxirredução , Fenóis
7.
Environ Sci Technol ; 57(27): 10127-10134, 2023 07 11.
Artigo em Inglês | MEDLINE | ID: mdl-37315045

RESUMO

Herein, we developed an electrochemical filtration system for effective and selective abatement of nitrogenous organic pollutants via peroxymonosulfate (PMS) activation. Highly conductive and porous copper nanowire (CuNW) networks were constructed to serve simultaneously as catalyst, electrode, and filtration media. In one demonstration of the CuNW network's capability, a single pass through a CuNW filter (τ < 2 s) degraded 94.8% of sulfamethoxazole (SMX) at an applied potential of -0.4 V vs SHE. The exposed {111} crystal plane of CuNW triggered atomic hydrogen (H*) generation on sites, which contributed to effective PMS reduction. Meanwhile, with the involvement of SMX, a Cu-N bond was formed by the interactions between the -NH2 group of SMX and the Cu sites of CuNW, accompanied by the redox cycling of Cu2+/Cu+, which was facilitated by the applied potential. The different charges of the active Cu sites made it easier to withdraw electrons and promote PMS oxidation. Theoretical calculations and experimental results were combined to suggest a mechanism for pollution abatement with CuNW networks. The results showed that system efficacy for the degradation of a wide array of nitrogenous pollutants was robust across a broad range of solution pH and complex aqueous matrices. The flow-through operation of the CuNW filter outperformed conventional batch electrochemistry due to convection-enhanced mass transport. This study provides a new strategy for environmental remediation by integrating state-of-the-art material science, advanced oxidation processes, and microfiltration technology.


Assuntos
Poluentes Ambientais , Nanofios , Poluentes Químicos da Água , Cobre , Nitrogênio , Poluentes Químicos da Água/análise , Peróxidos/química , Sulfametoxazol/química
8.
Environ Res ; 236(Pt 2): 116867, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37573819

RESUMO

Phosphorus scarcity and the deleterious ecological impact of the release of organophosphorus pesticides have emerged as critical global issues. Previous research has shown the ability of electrochemistry to induce the precipitation of calcium phosphate from phosphorus-laden wastewater to recover the phosphorus. The current study presents a flow-through electrochemical system consisting of a column-shaped electrochemical reactor, a tubular stainless-steel (SS) cathode, and a titanium suboxides (TiSO) anode. This system simultaneously oxidizes tetrakis (hydroxymethyl) phosphonium sulfate (THPS) and recycles phosphates. The influence of current density, flow rate, and initial calcium ions concentration were examined under continuous flow operation. To enhance the electrochemical reactor's performance, we elevated the current density from 5 to 30 mA cm-2, which caused the phosphorus recovery efficiency to increase from 37% to 72% within 120 min, accompanied by an enhancement of the THPS mineralization efficiency from 57% to 90%. These improvements were likely due to the higher yield of reactive species chloride species (Cl•) formed at the TiSO anode and the higher local pH at the cathode. By investigating the formation of Cl• at the TiSO anode, we found that THPS mineralization exceeded 75% in the presence of NaCl at a current density of 20 mA cm-2. The demonstrated performance of the flow-through electrochemical system should enable the utilization of anodic oxidation-cathodic precipitation for the recovery of phosphorus from organophosphorus-contaminated wastewater.

9.
Environ Sci Technol ; 56(16): 11750-11759, 2022 08 16.
Artigo em Inglês | MEDLINE | ID: mdl-35905440

RESUMO

Developing advanced heterogeneous catalysts with atomically dispersed active sites is an efficient strategy to boost the kinetics of peroxymonosulfate (PMS) activation for micropollutant removal. Here, we report a binary Mo2TiC2Tx MXene-based electroactive filter system with abundant surface Mo vacancies for effective activation of PMS. The Mo vacancies assumed two essential roles: (i) as anchoring sites for Fe single atoms (Fe-SA) and (ii) as cocatalytic sites for the Fenton-like reaction. Fe-SA formed strong metal-oxygen bonds with the Mo2TiC2Tx support, stabilizing at the sites previously occupied by Mo. The resulting Fe-SA/Mo2TiC2Tx nanohybrid filter achieved 100% degradation of sulfamethoxazole (SMX) in the single-pass mode (hydraulic retention time <2 s) when assisted by an electric field (2.0 V). The rate constant (k = 2.89 min-1) for SMX removal was 24 and 67 times greater than that of Fe nanoparticles immobilized on Mo2TiC2Tx and the pristine Mo2TiC2Tx filter, respectively. Operation in the flow-through configuration outperformed the conventional batch reactor model (k = 0.17 min-1) due to convection-enhanced mass transport. The results obtained from experimental investigations and theoretical calculations suggested that atomically dispersed Fe-SA, anchored on Mo vacancies, was responsible for the adsorption and activation of PMS to produce sulfate radicals (SO4•-) in the presence of an electric field. This study provides a proof-of-concept demonstration of an electroactive Fe-SA/Mo2TiC2Tx filter for broader application in the treatment of water contaminated by emerging micropollutants.


Assuntos
Ferro , Peróxidos , Catálise , Ferro/química , Peróxidos/química , Sulfametoxazol
10.
Environ Res ; 204(Pt B): 112117, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-34571037

RESUMO

Herein, an electrochemical carbon nanotubes (CNT) filter modified with MIL-101(Fe) has been designed for the electro-Fenton applications by serving as a functional flow-through electrode. Under an electric field, the hybrid filter enabled the in situ generation of H2O2via the two-electron oxygen reduction reaction, which promoted the production of HO by the accelerated Fe2+/Fe3+ cycling of MIL-101(Fe). It was observed that 93.2 ± 1.2% tetracycline and 69.0 ± 0.8% total organic carbon (TOC) were removed in 2 h under the optimized conditions. The electron paramagnetic resonance (EPR) analysis and radical scavenging experiments revealed that HO predominated the tetracycline degradation. As compared to the batch reactor, the performance of the proposed system was improved by 5.6 times owing to the convection-enhanced mass transport. The plausible working mechanism and degradation pathway were also subsequently proposed. The findings reported in this study provide a promising insight for the environmental remediation by integrating nanotechnology and Fenton chemistry.


Assuntos
Estruturas Metalorgânicas , Nanotubos de Carbono , Eletrodos , Peróxido de Hidrogênio , Oxirredução
11.
BMC Surg ; 22(1): 113, 2022 Mar 24.
Artigo em Inglês | MEDLINE | ID: mdl-35331206

RESUMO

BACKGROUND: Primary adenoid cystic carcinoma (ACC) of breast is rarely seen clinically. It is a special subtype of triple-negative breast cancer characterized by low expression of Ki-67, low malignant potential, slow progression and favorable prognosis. To date, treatment for this disease is controversial and no consensus is reached. We analyzed clinical manifestations and pathological characteristics of seven primary breast ACC cases and reported in combination with literature review to promote understanding, diagnosis and treatment of this disease. CASE PRESENTATION: We collected seven breast ACC cases pathologically diagnosed and treated in Department of breast surgery of the First Affiliated Hospital of China Medical University from January 2015 to December 2018. We organized and summarized the clinical, imaging, pathological and prognostic information and performed statistical analysis. The median age was 60 years (ranging from 54 to 64 years). Tumors of all patients were detected by immunohistochemistry. Molecular types were mostly triple negative (4/7), and Ki-67 expression was low (5/7). Lymph node metastases were absent in all patients received axillary lymph node surgery. Median follow-up time was 39 months (ranging from 25 to 68 months). There was no occurrence of relapse, distant metastasis or death. CONCLUSION: Breast ACC is accompanied with favorable diagnosis, which is different from typical triple-negative breast cancer. Accurate diagnosis of ACC is particularly important.


Assuntos
Neoplasias da Mama , Carcinoma Adenoide Cístico , Neoplasias da Mama/cirurgia , Carcinoma Adenoide Cístico/diagnóstico , Carcinoma Adenoide Cístico/patologia , Carcinoma Adenoide Cístico/cirurgia , Feminino , Humanos , Metástase Linfática , Mastectomia , Pessoa de Meia-Idade , Recidiva Local de Neoplasia/cirurgia
12.
Acc Chem Res ; 53(12): 2892-2902, 2020 12 15.
Artigo em Inglês | MEDLINE | ID: mdl-33170634

RESUMO

Rapid population growth and industrialization have driven the emergence of advanced electrochemical and membrane technologies for environmental and energy applications. Electrochemical processes have potential for chemical transformations, chloralkali disinfection, and energy storage. Membrane separations have potential for gas, fluid, and chemical purification. Electrochemical and membrane technologies are often used additively in the same unit process, e.g., the chloroalkali process where a membrane is used to separate cathodic and anodic products from scavenging each other. However, to access the maximal potential requires intimate hybridization of the two technologies into an electroactive membrane. The combination of the two discrete technologies results in a range of synergisms such as reduced footprint, increased processing kinetics, reduced fouling, and increased energy efficiency.Due to their high specific surface area, excellent electric conductivity, and desirable robustness, 1D carbon nanotubes (CNTs) hold promise for many applications over a range of industry sectors such as a base material for electrodes and membranes. Importantly, CNT morphology and surface chemistry can be rationally modified and fine-tuning of these CNT physicochemical properties can enhance their functionality toward practical applications. The CNT 1D form allows assembly of a stable thin-film fibrous network by a variety of facile techniques. These CNT networks have pore sizes in the range of 10-500 nm (dpore ∼ 6-8dCNT) and thicknesses of 10-200 µm, both similar to those of classical polymer membranes, thus allowing for straightforward incorporation into commercial membrane devices modified for electroactivity inclusion.In this Account, CNTs and their composites are used as model electroactive porous materials to exemplify the design strategies and environmental applications of emerging electroactive membrane technology. The Account begins with a brief summary of the electroactive membrane design principles and flow processes developed by our groups. After the methodology section, a detailed discussion is provided on the underlying physical-chemical mechanisms that govern the electroactive membrane technology. Then we summarize our findings on the rational design of several flow-through electrochemical CNT filtration systems focused on either anodic oxidation reactions or cathodic reduction reactions. Subsequently, we discuss a recently discovered electrochemical valence-state-regulation strategy that is capable to detoxify and sequester heavy metal ions. Finally, we conclude the Account with our perspectives toward future development of the electroactive membrane technology.

13.
Environ Sci Technol ; 55(6): 4045-4053, 2021 03 16.
Artigo em Inglês | MEDLINE | ID: mdl-33625227

RESUMO

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.


Assuntos
Peróxido de Hidrogênio , Ferro , Catálise , Oxirredução , Silicatos
14.
Environ Sci Technol ; 55(19): 13209-13218, 2021 10 05.
Artigo em Inglês | MEDLINE | ID: mdl-34553909

RESUMO

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.


Assuntos
Estruturas Metalorgânicas , Fosfatos , Adsorção , Porosidade
15.
Environ Sci Technol ; 54(9): 5913-5921, 2020 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-32271550

RESUMO

Gold (Au) has been considered catalytically inert for decades, but recent reports have described the ability of Au nanoparticles to catalyze H2O2 decomposition in the Haber-Weiss cycle. Herein, the design and demonstration of a flow-through electro-Fenton system based on an electrochemical carbon nanotube (CNT) filter functionalized with atomically precise Au nanoclusters (AuNCs) is described. The functionality of the device was then tested for its ability to catalyze antibiotic tetracycline degradation. In the functional filters, the Au core of AuNCs served as a high-performance Fenton catalyst; while the AuNCs ligand shells enabled CNT dispersion in aqueous solution for easy processing. The hybrid filter enabled in situ H2O2 production and catalyzed the subsequent H2O2 decomposition to HO·. The catalytic function of AuNCs lies in their ability to undergo redox cycling of Au+/Au0 under an electric field. The atomically precise AuNCs catalysts demonstrated superior catalytic activity to larger nanoparticles; while the flow-through design provided convection-enhanced mass transport, which yielded a superior performance compared to a conventional batch reactor. The adsorption behavior and decomposition pathway of H2O2 on the filter surfaces were simulated by density functional theory calculations. The research outcomes provided atomic-level mechanistic insights into the Au-mediated Fenton reaction.


Assuntos
Ouro , Nanopartículas Metálicas , Catálise , Peróxido de Hidrogênio , Oxirredução
16.
Environ Sci Technol ; 53(3): 1527-1535, 2019 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-30620181

RESUMO

Herein, we rationally designed a dual-functional electroactive filter system for simultaneous detoxification and sequestration of Sb(III). Binder-free and nanoscale TiO2-modified carbon nanotube (CNT) filters were fabricated. Upon application of an external electrical field, in situ transformation of Sb(III) to less toxic Sb(V) can be achieved, which is further sequestered by TiO2. Sb(III) removal kinetics and capacity increase with applied voltage and flow rate. This can be explained by the synergistic effects of the filter's flow-through design, electrochemical reactivity, small pore size, and increased number of exposed sorption sites. STEM characterization confirms that Sb were mainly sequestered by TiO2. XPS, AFS, and XAFS results verify that the Sb(III) conversion process was accelerated by the electrical field. The proposed electroactive filter technology works effectively across a wide pH range. The presence of sulfate, chloride, and carbonate ions negligibly inhibited Sb(III) removal. Exhausted TiO2-CNT filters can be effectively regenerated using NaOH solution. At 2 V, 100 µg/L Sb(III)-spiked tap water generated ∼1600 bed volumes of effluent with >90% efficiency. Density functional theory calculations suggest that the adsorption energy of Sb(III) onto TiO2 increases (from -3.81 eV to -4.18 eV) and Sb(III) becomes more positively charged upon application of an electrical field.


Assuntos
Nanotubos de Carbono , Poluentes Químicos da Água , Purificação da Água , Adsorção , Cinética
17.
Ecotoxicol Environ Saf ; 184: 109613, 2019 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-31491606

RESUMO

Four sugar sources were used as co-substrates to promote the degradation of a selected refractory dye reactive black 5 (RB5) by the natural bacterial flora DDMZ1. The boosting performance of the four sugar sources on RB5 decolorization ranked as: fructose > sucrose > glucose > glucose + fructose. Kinetic results of these four co-metabolism systems agreed well with a first-order kinetic model. Four sugar sources stimulated the extracellular azoreductase secretion causing enhanced enzyme activity. An increased formation of low molecular weight intermediates was caused by the addition of sugar sources. The toxicity of RB5 degradation products was significantly reduced in the presence of sugar sources. The bacterial community structure differed remarkably as a result of sugar sources addition. For a fructose addition, a considerably enriched population of the functional species Burkholderia-Paraburkholderia and Klebsiella was noted. The results enlarge our knowledge of the microkinetic and microbiological mechanisms of co-metabolic degradation of refractory pollutants.


Assuntos
Corantes/metabolismo , Naftalenossulfonatos/metabolismo , Açúcares/metabolismo , Bactérias/classificação , Bactérias/metabolismo , Biodegradação Ambiental , Corantes/química , Corantes/toxicidade , Cinética , NADH NADPH Oxirredutases/metabolismo , Naftalenossulfonatos/toxicidade , Nitrorredutases
18.
Artigo em Inglês | MEDLINE | ID: mdl-29083952

RESUMO

In order to manage water resources, a software sensor model was designed to estimate water quality using a hybrid fuzzy neural network (FNN) in Guangzhou section of Pearl River, China. The software sensor system was composed of data storage module, fuzzy decision-making module, neural network module and fuzzy reasoning generator module. Fuzzy subtractive clustering was employed to capture the character of model, and optimize network architecture for enhancing network performance. The results indicate that, on basis of available on-line measured variables, the software sensor model can accurately predict water quality according to the relationship between chemical oxygen demand (COD) and dissolved oxygen (DO), pH and NH4+-N. Owing to its ability in recognizing time series patterns and non-linear characteristics, the software sensor-based FNN is obviously superior to the traditional neural network model, and its R (correlation coefficient), MAPE (mean absolute percentage error) and RMSE (root mean square error) are 0.8931, 10.9051 and 0.4634, respectively.


Assuntos
Oxigênio/química , Rios/química , Qualidade da Água , Abastecimento de Água , Algoritmos , Análise da Demanda Biológica de Oxigênio , China , Simulação por Computador , Lógica Fuzzy , Humanos , Redes Neurais de Computação , Software
19.
World J Microbiol Biotechnol ; 34(11): 165, 2018 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-30374618

RESUMO

Textile printing and dyeing wastewater is usually characterized by high pH, high turbidity, poor bio-degradability, complex composition, and high chrominance, and is discharged in large amounts. It has been regarded as one of the hardest to treat forms of industrial wastewater. Conventional physicochemical technologies can remove these contaminants from water bodies, but at the expense of high energy consumption and high cost. Alternatively, biological processes with limited energy consumption, low cost and high efficiency are considered as promising technologies. Among them, the anaerobic biological processes have been proven to be effective for the treatment of high-concentration textile printing and dyeing wastewater. In this mini-review, recent advances on high-rate anaerobic technologies for such purposes are reviewed. Current limitations of these technologies are summarized, and future research directions are indicated.


Assuntos
Bactérias/metabolismo , Águas Residuárias/microbiologia , Poluentes Químicos da Água/metabolismo , Anaerobiose , Biodegradação Ambiental , Resíduos Industriais/análise , Indústria Têxtil , Águas Residuárias/química , Purificação da Água
20.
Environ Sci Technol ; 49(13): 7974-80, 2015 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-26056728

RESUMO

In this work, a carbon nanotube (CNT) electrochemical filter was investigated for treatment of aqueous antibiotics using tetracycline (TC) as a model compound. Electrochemical filtration of 0.2 mM TC at a total cell potential of 2.5 V and a flow rate of 1.5 mL min(-1) (hydraulic residence time <2 s) resulted in an oxidative flux of 0.025 ± 0.001 mol h(-1) m(-2). Replacement of the perforated Ti cathode with a CNT cathode increased the TC oxidative flux by 2.3-fold to 0.020 ± 0.001 mol h(-1) m(-2) at a total cell potential of 1.0 V. Effluent analysis by liquid chromatography-mass spectrometry and disk agar biocidal diffusion tests indicate that the electrochemical filtration process can degrade the TC molecular structure and significantly decrease its antimicrobial activity, respectively. Addition of dissolved natural organic matter (NOM) negatively affected the TC electrooxidation because of competition for CNT sorption and electrooxidation sites. At 2.0 V total cell potential, TC spiked (0.2 mM) into drinking water reservoir and wastewater treatment plant effluent samples had an oxidative flux of 0.015 ± 0.001 and 0.022 ± 0.001 mol h(-1) m(-2), respectively, and an energy requirement of 0.7 kWh kgCOD(-1) or 0.084 kWh m(-3). These results indicate a CNT electrochemical filter may have potential to effectively and efficiently treat antibiotics in water and wastewater effluent.


Assuntos
Antibacterianos/química , Eletroquímica/instrumentação , Filtração/instrumentação , Nanotubos de Carbono/química , Tetraciclina/química , Eletrodos , Elétrons , Meio Ambiente , Cinética , Testes de Sensibilidade Microbiana , Compostos Orgânicos/análise , Oxirredução , Termodinâmica , Fatores de Tempo , Eliminação de Resíduos Líquidos , Águas Residuárias/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA