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1.
Environ Sci Technol ; 58(12): 5589-5597, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38485130

RESUMO

Heavy metal pollution treatment in industrial wastewater is crucial for protecting biological and environmental safety. However, the highly efficient and selective removal of heavy metal ions from multiple cations in wastewater is a significant challenge. This work proposed a pulse electrochemical method with a low-/high-voltage periodic appearance to selectively recover heavy metal ions from complex wastewater. It exhibited a higher recovery efficiency for heavy metal ions (100% for Pb2+ and Cd2+, >98% for Mn2+) than other alkali and alkaline earth metal ions (Na+, Ca2+, and Mg2+ were kept below 3.6, 1.3, and 2.6%, respectively) in the multicomponent solution. The energy consumption was only 34-77% of that of the direct current electrodeposition method. The results of characterization and experiment unveil the mechanism that the low-/high-voltage periodic appearance can significantly suppress the water-splitting reaction and break the mass-transfer limitation between heavy metal ions and electrodes. In addition, the plant study demonstrates the feasibility of treated wastewater for agricultural use, further proving the high sustainability of the method. Therefore, it provides new insights into the selective recovery of heavy metals from industrial wastewater.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Águas Residuárias , Metais Pesados/química , Eletricidade , Água , Íons , Adsorção , Poluentes Químicos da Água/química
2.
Small ; : e2311401, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38348946

RESUMO

Biochar materials have shown great potential for broad catalytic application. However, using these materials in the capacitive deionization technology (CDI) system for heavy metal removal still faces a significant challenge due to their low specific capacity and removal capability. Here, a comprehensive regulation on the interfacial/bulk electrochemistry of biochar by Zn doping is reported, which suggests a high renewable capacity (20 mg g-1 ) and outstanding selective capacitive removal ability (SCR) of Pb2+ from leachate. The SCR efficiency of Pb2+ is as high as 99% compared to K+ (8%), Na+ (13%), and Cd2+ (37%). This work proves that the doped Zn on the biochar can combine with OH- generated by water splitting to form M─OH bonds, which is beneficial for improving the specific capacity. Significantly, the relationship between double-layer capacitance and pseudo-capacitance can also be optimized by regulating the content of Zn, leading to different removal abilities of heavy metals. Therefore, this work offers insights into charge-storage kinetics, which provide valuable guidelines for designing and optimizing the biochar electrode for broader environmental applications.

3.
Small ; 20(5): e2305807, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37731008

RESUMO

Surfactant-like contaminants (SLCs) with distinctive amphiphilic structures have become a global concern in wastewater due to their toxicity and persistency. Despite extensive efforts, achieving efficient and selective SLCs removal remains challenging because of their wide range of molecular weights and complex functional group compositions. Superhydrophobic nanoparticles can potentially tackle this challenge by targeting the long oleophilic chains of SLCs. However, conventional contact angle measurements hinder hydrophobicity characterization and corresponding selectivity research because of the powder morphology of nanoparticles. Herein, the authors offered information regarding the distribution of water molecular probes in surfaces and proposed a quantitative characterization approach based on low-field nuclear magnetic resonance. Through synthesizing superhydrophobic and hydrophilic polydopamine nanospheres with similar morphologies, the selective adsorption potential of superhydrophobic nanoparticles for SLCs is systematically demonstrated. As revealed by the interaction mechanisms, the superhydrophobic surface of nanospheres increased its affinity and selectivity for SLCs adsorption by enhancing hydrophobic interactions. Superhydrophobic modification achieved ten times the adsorption capacity of sodium dodecyl benzene sulfonate, an exemplified surfactant, compared with pristine nanoparticles. By regulated self-polymerization, the superhydrophobic nanospheres are coated onto the surface of a 3D sponge and enable efficient selective SLCs adsorption from highly polluted leachate matrices with long-term stability and reusability.

4.
J Hazard Mater ; 465: 133178, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38064951

RESUMO

Mycotoxin contaminations in food and environment seriously harms human health. Constructing sensitive and point-of-test early-warning tools for mycotoxin determination is in high demand. In this study, a CuCo@PDA nanozyme-based aptamer-mediated lateral flow assay (Apt-LFA) has been elaborately designed for on-site and sensitive determination of mycotoxin Aflatoxin B1 (AFB1). Benefiting from the rich functional groups and excellent peroxidase-like activity, the CuCo@PDA with original dark color can be conjugated with the specific recognition probe (i.e., aptamer), generating colorimetric signal on the test lines of Apt-LFA via a competitive sensing strategy. The signal can further be amplified in-situ by catalytic chromogenic reaction. Therefore, a visual and dual-readout detection of AFB1 has been realized. The developed Apt-LFA provides a flexible detection mode for qualitative and quantitative analysis of AFB1 by naked-eyes observation or smartphone readout. The smartphone-based LFA platform shows a reliable and ultrasensitive determination of AFB1 with the limit of detection (LOD) of 2.2 pg/mL. The recoveries in the real samples are in the range of 95.11-113.77% with coefficients of variations less than 9.84%. This study provides a new approach to realize point-of-test and sensitive detection of mycotoxins in food and environment using nanozyme-based Apt-LFAs.


Assuntos
Aptâmeros de Nucleotídeos , Técnicas Biossensoriais , Humanos , Aflatoxina B1/análise , Contaminação de Alimentos/análise , Alimentos , Limite de Detecção
5.
Environ Res ; 238(Pt 1): 117138, 2023 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-37716395

RESUMO

Exploring the vegetation carbon cycle and the factors influencing vegetation carbon sequestration in areas with complex plateau-basin topography and fragile ecosystems is crucial. In this study, spatial and temporal characteristics of carbon sequestration by vegetation in Sichuan and Chongqing from 2010 to 2020 and the influencing factors were investigated through simulations of net primary productivity (NPP) using the modified Carnegie-Ames-Stanford approach (CASA) and the Thornthwaite Memorial (TM) model and using chemical equations of photochemical reactions. The results indicated that: The spatial distribution of carbon sequestration capacity (CSC) trends showed an increase in the east (the most prominent increased trend along the mountainous areas of the basin) and a decrease in the west (western Sichuan plateau). Differences exist in the impact factors of CSC in different regions. In the basin margins and mountainous areas, where the proportion of forests was high, a combination of climate change and human activities contributed to the increase in CSC. The relatively warm and humid meteorological conditions in the hinterland of the basin were more conducive to the increase in CSC, and climate change also affected the region more significantly. In contrast, in the relatively high altitude of western Sichuan, controlled human activities were the key to improving CSC. The results of the study contribute to the understanding of the basic theory of vegetation carbon cycle in areas with complex plateau-basin topography and fragile ecosystems, as well as to provide suggestions for ecological shelter construction and ecological restoration in the upper Yangtze River.


Assuntos
Sequestro de Carbono , Ecossistema , Humanos , Mudança Climática , Florestas , Atividades Humanas , China , Carbono
6.
Artigo em Inglês | MEDLINE | ID: mdl-36900837

RESUMO

Thallium is widely used in industrial and agricultural development. However, there is still a lack of systematic understanding of its environmental hazards and related treatment methods or technologies. Here, we critically assess the environmental behavior of thallium in aqueous systems. In addition, we first discuss the benefits and limitations of the synthetic methods of metal oxide materials that may affect the practicality and scalability of TI removal from water. We then assess the feasibility of different metal oxide materials for TI removal from water by estimating the material properties and contaminant removal mechanisms of four metal oxides (Mn, Fe, Al, and Ti). Next, we discuss the environmental factors that may inhibit the practicality and scalability of Tl removal from water. We conclude by highlighting the materials and processes that could serve as more sustainable alternatives to TI removal with further research and development.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Tálio , Poluentes Químicos da Água/análise , Óxidos , Água , Adsorção
7.
J Hazard Mater ; 445: 130481, 2023 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-36493653

RESUMO

Highly efficient charge transfer is a critical factor to modulate the photocatalytic activity. However, the conscious modulation of charge transfer efficiency is still a great challenge. Herein, a novel interfacial Mo-N bond and appropriate oxygen vacancies (OVs) modulated S-scheme MoO3-x/S-CN heterojunction was rationally fabricated for efficient photocatalytic disinfection. The results of characterizations and density functional theory (DFT) calculations suggested that the enhanced charge transfer dynamics is ascribed to the optimizing oxygen vacancies density and forming interfacial Mo-N bond. It can improve charge transfer efficiency from 36.4% (MoO3-x) to 52.5% (MoO3-x/S-CN) and produce more reactive oxygen species (ROS), achieving entirely inactivate of 7.60-log E. coli and S. aureus within 50 min and 75 min. Besides, MoO3-x/S-CN can well resist the disturbance from the coexisting substances, and can be applied in a wide pH range, and even authentic water bodies. Monitoring of bacterial antioxidant systems and membrane integrity revealed that bacterial inactivation begins with the oxidation of cell membrane and dies from leakage of intracellular substances and destruction of cell structure. This work provides an inspiration on consciously modulating S-scheme charge transfer efficiency by optimizing oxygen vacancies density and atomic-level interface control for promoting the photocatalytic antibacterial activity.


Assuntos
Desinfecção , Oxigênio , Escherichia coli , Staphylococcus aureus , Espécies Reativas de Oxigênio
8.
Anal Chem ; 94(48): 16768-16777, 2022 12 06.
Artigo em Inglês | MEDLINE | ID: mdl-36419373

RESUMO

Antibiotic residues in the environment and in foods pose a serious threat to ecosystems and human health. Developing sensitive and on-site detection methods is therefore in high demand. In this work, a portable paper-based colorimetric sensor with a smartphone platform with an ultrahigh sensitivity has been designed for on-site and quantitative analysis of antibiotic residues based on aptamer-regulated nanozyme activity. The developed excellent peroxidase-like nanozymes, carbon-protected NiCo bimetal oxides with a unique hollow nanocage structure (NiCo@C HCs), could effectively catalyze the oxidation of chromogenic substrates by H2O2. Once bound to a specific aptamer, the enzyme-mimicking activity of NiCo@C HCs is obviously inhibited as a result of the masking of active sites but could be restored via the target-aptamer recognition. Herein, the aptamer-modified NiCo@C HCs are embedded on paper pieces to construct paper-based biochips for visual detection. Meanwhile, a smartphone platform is integrated for the signal readout. Using enrofloxacin (ENR) as an analyte model, the proposed paper-based analysis platform shows a reliable and sensitive detection of ENR with an ultralow detection limit of 0.029 ng/mL. The platform also works well in various real samples. This analysis method is facile in design, showing a great application potential for on-site and mass screening of antibiotic residues in the environment and in foods.


Assuntos
Técnicas Biossensoriais , Colorimetria , Humanos , Colorimetria/métodos , Antibacterianos/análise , Smartphone , Limite de Detecção , Peróxido de Hidrogênio/análise , Ecossistema , Técnicas Biossensoriais/métodos
9.
Water Res ; 227: 119324, 2022 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-36368084

RESUMO

In this study, a novel and efficient heterogeneous electro-Fenton (EF) process with a potassium ferrate (K2FeO4) modified carbon felt (Fe-CF) cathode was developed for chloramphenicol (CAP) removal. The catalytic activity was assessed by the comparison of different systems and the effects of multiple operating parameters (K2FeO4 dosage, initial solution pH, applied current) and co-existing constituents. Results indicated that the Fe-CF cathode exhibited excellent performance for CAP degradation (almost 100% removal efficiency within 60 min) over a wide range of pH (pH 3-9) during heterogeneous EF ascribed to the synergistic effect of embedded iron species and porous graphitic carbon structure and effective utilization of the in-situ generated H2O2. Moreover, the Fe-CF cathode possessed good recyclability with low metal leaching (98.2% CAP removal efficiency after reused for 5 times) and outstanding real water application performance. The ∙OH and O2∙- were responsible for CAP degradation, while ∙OH played a main role. Moreover, the toxicity evaluation by E. coli growth experiments demonstrated an efficient toxicity reduction in this system. Overall, a novel heterogeneous EF functional cathode with superior performance was fabricated via a green, low-cost one-step method, which shows promising application potential for actual wastewater treatment.


Assuntos
Peróxido de Hidrogênio , Poluentes Químicos da Água , Fibra de Carbono , Peróxido de Hidrogênio/química , Carbono , Cloranfenicol , Escherichia coli , Poluentes Químicos da Água/química , Oxirredução , Ferro/química , Eletrodos
10.
Biosens Bioelectron ; 216: 114652, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36095977

RESUMO

Accurate on-site analysis of food quality, environmental pollutants, and disease biomarkers is of great significance for safeguarding public health. In this work, based on the novel nanozymes, MnCo oxides@carbon yolk-shell nanocages (MnCo@C NCs), a portable colorimetric sensor with smartphone platform has been developed for rapid, on-site and quantitative analysis of total antioxidant capacity (TAC) and phenolic compounds. The MnCo@C NCs are synthesized via one-step calcination of polydopamine-coated MnCo Prussian blue analogs (MnCo-PBA@PDA). The PDA-derived carbon shell is found to be able to protect the nanocages from collapsing, thus increasing their specific surface areas and porosity. Benefiting from the unique structure and multivalent MnCo bimetallic oxides, the MnCo@C NCs perform outstanding catalytic performance and multiple enzyme-mimicking activities including oxidase, laccase and catalase. Hence, a multifunctional application platform integrated smartphone has been constructed for rapid and sensitive colorimetric detection of three model analytes (i.e., ascorbic acid (AA), 2,4-dichlorophenol (2,4-DP), and epinephrine) with extremely low detection limits of 0.29 µM, 0.76 µM, and 0.70 µM, respectively. This sensor device is successfully applied in TAC analysis in vegetables, fruits, and beverages, as well as epinephrine determination in human serum samples. This work provides new insights into designing multifunctional nanozymes to advance the instant detection technology in the field of food supervision, environment monitoring, and human health.


Assuntos
Técnicas Biossensoriais , Poluentes Ambientais , Antioxidantes , Ácido Ascórbico , Biomarcadores , Carbono/química , Catalase , Colorimetria , Epinefrina , Humanos , Lacase , Óxidos , Smartphone
11.
J Hazard Mater ; 440: 129720, 2022 10 15.
Artigo em Inglês | MEDLINE | ID: mdl-35952429

RESUMO

The Fenton-like processes are considered to be one of the most promising strategies for inactivating bacteria due to their capacity to produce reactive oxygen species (ROS). Herein, a catalytic system for efficient inactivation of Escherichia coli (E. coli) was developed by anchoring single-atom Ru on layered double hydroxides (LDH). The Ru/NiFe-LDH catalyst showed excellent performance in activating peroxymonosulfate (PMS) to inactivate E. coli. Under the combined action of the ultra-low concentrations of Ru/NiFe-LDH (40 mg/L) and PMS (5 mg/L), 7 log E. coli can be totally inactivated within 90 s. This was attributed to the combined effect of single-atom Ru adsorption to E. coli and the ROS produced in situ. Mechanism studies indicated that the 1O2 with electrophilic properties was the key active species responsible for the rapid inactivation of E. coli. The E. coli inactivation process suggested that the ROS produced first attacked the outer membrane of the cell, then the antioxidant enzymes in the cell were induced, the macromolecule substances were released and mineralized, eventually leading to irreversible cell death. This work firstly loads monoatomic Ru on LDH for bacterial inactivation, providing a feasible method for rapid inactivation of E. coli.


Assuntos
Antioxidantes , Escherichia coli , Hidróxidos , Peróxidos , Espécies Reativas de Oxigênio
12.
J Colloid Interface Sci ; 623: 445-455, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35597014

RESUMO

The design of a photocatalyst for efficient algal inactivation under visible light is essential for the application of photocatalysis to the control of harmful algal blooms. In this study, a novel Z-scheme heterojunction tubular photocatalyst, Ag2O@PG, was synthesized by chemically depositing silver oxide compounded with P-doped hollow tubular graphitic carbon nitride for the photocatalytic inactivation of Microcystis aeruginosa (M. aeruginosa). The photocatalytic algal inactivation experiments showed that the photocatalytic activity of Ag2O@PG was influenced by the ratio of the composition of the obtained materials. The optimal algal inactivation efficiency was observed when using Ag2O@PG-0.4 at a dosage of 0.2 g/L. It was able to achieve a 99.1 % M. aeruginosa inactivation at an initial concentration of 4.5 × 106 cells/mL following 5 h' visible light irradiation. During the process, the cell membrane permeability and cell morphology changed. Furthermore, under the constant attack of superoxide radicals and holes caused by Ag2O@PG, the superoxide dismutase, glutathione and malondialdehyde of algae cells increased during the experiments to alleviate oxidative damage. Eventually, the antioxidant system of algae cells was destroyed. To further validate the potential application of Ag2O@PG-0.4 in real algal bloom environment, an experiment in real water samples was carried out. Overall, the Ag2O@PG-0.4 as an efficient photocatalyst has a promising potential for emergency treatment measures to alleviate algal blooms.


Assuntos
Microcystis , Luz , Microcystis/química
13.
Chemosphere ; 300: 134449, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35364089

RESUMO

The problems of high salinity and coexistence of antibiotics in mariculture wastewater pose a great challenge to the traditional wastewater treatment technology. Herein, an electrocatalytic system based on cathodes to sustain reactive chlorine species (RCS) in a high chlorine environment was proposed. The results show that the content of RCS is affected by cathodes. The electrocatalytic system with FeNi/NF as cathode has the largest RCS retention capacity when compared with other cathode systems (carbon felt, nickel foam, copper foam, stainless steel, and nickel-iron foam). This is related to FeNi/NF's higher hydrogen production activity, which inhibits the reduction reaction of RCS. Furthermore, the degradation of tetracycline by the proposed FeNi/NF system maintained long-term effective performance across 20 cycles. Thus, the application of high chlorine resistance electrocatalysis system provides a possibility for practical electrocatalysis treatment of mariculture wastewater.


Assuntos
Cloro , Águas Residuárias , Antibacterianos , Aquicultura , Eletrodos , Níquel , Tetraciclina
14.
J Hazard Mater ; 430: 128464, 2022 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-35176697

RESUMO

Iron-cobalt layered double hydroxides (FeCoLDH) showed superior oxygen evolution reaction (OER) performance, but the sluggish water adsorption and dissociation dynamics restrict its capacity to degrade organic pollutants by electro-oxidation. Herein, enhanced electro-oxidation performance of FeCoLDH with hydrophilic structure was designed and exhibited efficient removal efficiency of tetracycline. Theoretical calculation and characterization results consistently elucidated that the electronic structure of FeCoLDH is optimized by doping phosphorus and depositing copper nanodots (NDs). In addition, the obtained Cu NDs/P-FeCoLDH shows higher degradation ability of tetracycline in all-pH conditions than pristine FeCoLDH. That's because it owns smaller barrier with 0.6 eV to generate hydroxyl radicals (•OH) than pristine FeCoLDH. Furthermore, it can effectively degrade organic pollutants in seawater, river water and pharmaceutical wastewater samples. This work provides novel and rational electrode materials for electro-oxidation system with practical application potential, which could offer new insights into the fundamental understanding of electrochemistry.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Eletrodos , Peróxido de Hidrogênio , Ferro , Oxirredução , Águas Residuárias/química , Poluentes Químicos da Água/química
15.
Chemosphere ; 291(Pt 3): 133001, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34808205

RESUMO

The photo-Fenton-like catalytic process has shown great application potential in environmental remediation. Herein, a novel photo-Fenton-like catalyst of Bi2WO6 nanosheets decorated hortensia-like CoAl-layered double hydroxides (Bi2WO6/CoAl-LDHs) was synthesized via hydrothermal process. The optimized Bi2WO6/CoAl-LDHs composite performed the high-efficiency photo-Fenton-like catalytic performance for oxytetracycline (OTC) removal (98.47%) in the mediation of visible-light and H2O2. The comparative experiment, technical characterization and density functional theory calculation results indicated that the efficient photo-Fenton-like catalytic performance of Bi2WO6/CoAl-LDHs was attributed to the synergistic action of the Fenton-like process of cobalt ions in CoAl-LDHs, an internal electric field and the S-scheme heterojunction form between Bi2WO6 and CoAl-LDHs, which could significantly promote the active substance formation and the photocatalytic process in the catalytic system. This study will stimulate the new inspiration of designing the efficient catalytic system for environmental remediation and other fields.


Assuntos
Carvão Mineral , Peróxido de Hidrogênio , Catálise , Hidróxidos , Modelos Teóricos
16.
Water Res ; 201: 117360, 2021 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-34174730

RESUMO

Finding a low cost and effective alternative to noble metal based catalyst has long been concerned in wastewater treatment and organic transformation. This work developed a highly efficient sewage sludge-based catalyst via a simple one-step pyrolysis method, and for the first time, applied it in the catalytic reduction of nitrophenols. Due to the higher content of graphitic nitrogen, abundant defect sites and low electron transfer resistance, sewage sludge derived biochar obtained at 800 °C (SSBC-800) exhibits the best catalytic performance, with the reaction rate of 0.48 min-1 and turnover frequency for 4-nitrophenol calculated to be 1.25 × 10-4 mmol•mg-1 min-1, which is comparable to or even superior than some reported noble metal-based catalyst. Moreover, SSBC-800 showed good recyclability of 90% 4-nitrophenol removal within 8 min after 4 runs, and maintained high catalytic activity in reduction of other substituent nitrophenols, such as 2-nitrophenol (0.54 min-1), 3-nitrophenol (0.61 min-1) and 2,4-dinitrophenol (0.18 min-1), and in real water samples, indicating its practical applicability. The electron paramagnetic resonance spectra and electrochemical characterization demonstrate that SSBC-800 accelerates the dissociation of BH4- to form active hydrogen, which is the main species responsible for 4-nitrophenol reduction, while electron transfer reaction involving the surface bound hydride derived from the intimate contact between BH4- and SSBC-800 plays an important role in this process. This research not only provides a novel valorization pathway for sewage sludge, but also sheds new light on further designing of carbon-based catalyst for nitrophenol reduction.


Assuntos
Carvão Vegetal , Esgotos , Hidrogenação , Nitrofenóis
17.
J Hazard Mater ; 403: 123610, 2021 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-32829226

RESUMO

Low-cost biochar adsorbent owning great potential for environmental remediation faces a bottleneck in application for its unsatisfied adsorption performance. Compared to the efforts on increasing adsorption capacity, improving adsorption speed which is important for treatment efficiency is often neglected. Herein, a hierarchical porous biochar (HPB) derived from shrimp shell was prepared and exhibited good adsorption capacity (Qm>300 mg/g) and fast adsorptive equilibrium (≤10 min) towards three typical aromatic organics, whose adsorption universality was further proved by two-way ANOVA analysis. Whereafter, model analysis demonstrated that, the adsorptive forms (mono- and multi-layers) on HPB depended on whether the contaminant is charged. Compared to the benzene-ring site of organics, the charged site contributed 5.13 times to adsorption promotion in monolayer but -0.49 times in inhibition for multilayers forms. Simultaneously, functional group sites contributed relatively weak (0.023 to 0.342 times only). Following structural control revealed that, hierarchical pore structure of HPB was the key for the fast adsorption speed, and highly graphitic structure was important for the high adsorption capacity. This study aims to provide an advanced biochar adsorbent, not only in adsorption capacity but also in adsorptive speed, and reveal the relationship between the structure and adsorption performance of biochar.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Adsorção , Carvão Vegetal , Cinética , Porosidade , Poluentes Químicos da Água/análise
18.
Anal Chem ; 92(19): 13073-13083, 2020 10 06.
Artigo em Inglês | MEDLINE | ID: mdl-32872771

RESUMO

Herein, we developed an unmodified hexagonal boron nitride (h-BN) photoelectrochemical (PEC) biosensing platform with a low background signal and high sensitivity based on CuS quantum dots (QDs)/Co3O4 polyhedra-driven multiple signal amplifications. The prepared porous h-BN nanosheets with large specific surface areas, as the photoelectric substrate material, can provide extensive active reaction sites. Meanwhile, the CuS QDs/Co3O4 polyhedra were synthesized by the zeolitic imidazolate framework (ZIF-67) and utilized as a multiple signal amplifier, which can not only drive the p-n semiconductor quenching effect to compete with the h-BN photoelectrode for the consumption of electron donors and exciting light but also trigger a mimetic enzymatic catalytic precipitation effect to inhibit electron transfer. The quenching ability and peroxidase-like activity of CuS QDs/Co3O4 polyhedra were evaluated to prove its superiority, and the possible mechanisms of electron transfer and enzymatic catalytic were further analyzed in detail. The developed PEC biosensing platform for the chlorpyrifos assay presented outstanding performance with a wide linear range from 1 × 10-1 to 1 × 107 ng mL-1 and a low detection limit of 0.34 pg mL-1 and exhibited excellent selectivity, reproducibility, and stability. In addition, the CuS QDs/Co3O4 polyhedra-activated h-BN PEC biosensing platform may exhibit universality for various analytes via replacing the corresponding target aptamer sequence. This work provides a remarkable inspiration and valuable reference for the development of the PEC biosensor, and the signal amplifier-enabled unmodified PEC biosensing platform strategy has a bright application in early safety warning, bioanalysis and clinical diagnosis.


Assuntos
Técnicas Biossensoriais , Compostos de Boro/química , Clorpirifos/análise , Inibidores da Colinesterase/análise , Técnicas Eletroquímicas , Pontos Quânticos/química , Cobalto/química , Cobre/química , Óxidos/química , Tamanho da Partícula , Processos Fotoquímicos , Porosidade , Propriedades de Superfície
19.
Sci Total Environ ; 736: 139629, 2020 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-32474279

RESUMO

Pollution of Sb(III) in water has caused great concern in recent years. Nanoscale zero-valent iron (nZVI) can detoxify Sb(III) polluted water, but the rapid passivation and low adsorption capacity limit its practical application. Hence, this study provides a new and efficient nanotechnology to remove Sb(III) using the sulfidated nanoscale zero-valent iron (S-nZVI). The S-nZVI exhibits higher Sb(III)-removal efficiency than pristine nZVI under both aerobic and anoxic conditions. The adsorption capacity of Sb(III) by optimized S-nZVI (465.1 mg/g) is 6 times as high as that of the pristine nZVI (83.3 mg/g) under aerobic conditions. The results indicate that Sb(III) and Sb(V) can be immobilized on the surface of S-nZVI by forming Fe-S-Sb precipitates. Moreover, characterization results demonstrate that the existence of S2- can not only activate H2O2 to produce hydroxyl radical, but also accelerate the cycle of Fe3+/Fe2+ to improve the efficiency of Fenton reaction. Therefore, S-nZVI can produce more hydroxyl radicals to oxidize Sb (III) to Sb (V) and results in 2.3-fold higher oxidation rate of Sb(III) compared to pristine nZVI. The formed FeS layer on the S-nZVI surface can also improve the release ability of Fe2+ and accelerate the formation of nZVI corrosion products. S-nZVI thus holds great potential to be applied in antimony removal.

20.
Chemosphere ; 256: 127141, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32470738

RESUMO

To explore a green, low-cost, and efficient strategy to synthesis reduced graphene oxide (RGO), the process and mechanism of the graphene oxide (GO) reduction by a model electrochemically active bacteria (EAB), Geobacter sulfurreducens PCA, were studied. In this work, up to 1.0 mg mL-1 of GO was reduced by G. sulfurreducens within 0.5-8 days. ID/IG ratio in reduced product was similar to chemically RGO. After microbial reduction, the peak which corresponded to the reflection of graphene oxide (001) disappeared, while another peak considered as graphite spacing (002) appeared. The peak intensity of typical oxygen function groups, such as carboxyl C-O and >O (epoxide) groups, diminished in bacterially induced RGO comparing to initial GO. Besides, we observed the doping of nitrogen and phosphorus elements in bacterially induced RGO. In a good agreement with that, better electrochemical performance was noticed after GO reduction. As confirmed with differential pulse voltammetry (DPV) and cyclic voltammetry (CV) analysis, the maximum value of peak currents of bacterially induced RGO were significantly higher than those of GO. Our results showed the electron transfer at microbial cell/GO interface promoted the GO reduction, suggesting a broader application of EAB in biological mediated production of RGO.


Assuntos
Geobacter/metabolismo , Grafite/química , Produtos Biológicos , Elétrons , Grafite/síntese química , Óxidos
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