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1.
Environ Sci Technol ; 58(18): 8053-8064, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38662987

RESUMO

The aggregation behavior of ubiquitous dissolved black carbon (DBC) largely affects the fate and transport of its own contaminants and the attached contaminants. However, the photoaging processes and resulting effects on its colloidal stability remain yet unknown. Herein, dissolved biochars (DBioCs) were extracted from common wheat straw biochar as a proxy for an anthropogenic DBC. The influences of UV radiation on their aggregation kinetics were systematically investigated under various water chemistries (pH, electrolytes, and protein). The environmental stability of the DBioCs before and after radiation was further verified in two natural water samples. Hamaker constants of pristine and photoaged DBioCs were derived according to Derjaguin-Landau-Verwey-Overbeek (DLVO) prediction, and its attenuation (3.19 ± 0.15 × 10-21 J to 1.55 ± 0.07 × 10-21 J after 7 days of radiation) was described with decay kinetic models. Pearson correlation analysis revealed that the surface properties and aggregation behaviors of DBioCs were significantly correlated with radiation time (p < 0.05), indicating its profound effects. Based on characterization and experimental results, we proposed a three-stage mechanism (contended by photodecarboxylation, photo-oxidation, and mineral exposure) that DBioCs might experience under UV radiation. These findings would provide an important reference for potential phototransformation processes and relevant behavioral changes that DBC may encounter.


Assuntos
Raios Ultravioleta , Água/química , Carvão Vegetal/química , Cinética , Poluentes Químicos da Água/química
2.
Environ Sci Technol ; 57(7): 2726-2738, 2023 02 21.
Artigo em Inglês | MEDLINE | ID: mdl-36746765

RESUMO

The characterization of variations in riverine microbiota that stem from contaminant sources and transport modes is important for understanding biogeochemical processes. However, the association between complex anthropogenic nitrogen pollution and bacteria has not been extensively investigated owing to the difficulties faced while determining the distribution of nitrogen contaminants in watersheds. Here, we employed the Soil and Water Assessment Tool alongside microbiological analysis to explore microbial characteristics and their responses to complex nitrogen pollution patterns. Significant variations in microbial communities were observed in sub-basins with distinct land-water pollution transport modes. Point source-dominated areas (PSDAs) exhibited reduced microbial diversity, high number of denitrification groups, and increased nitrogen cycling compared with others. The negative relative deviations (-3.38) between the measured and simulated nitrate concentrations in PSDAs indicated that nitrate removal was more effective in PSDAs. Pollution sources were also closely associated with microbiota. Effluents from concentrated animal feeding operations were the primary factors relating to the microbiota compositions in PSDAs and balanced areas. In nonpoint source-dominated areas, contaminants from septic tanks become the most relevant sources to microbial community structures. Overall, this study expands our knowledge regarding microbial biogeochemistry in catchments and beyond by linking specific nitrogen pollution scenarios to microorganisms.


Assuntos
Microbiota , Poluentes Químicos da Água , Animais , Nitrogênio/análise , Nitratos/análise , Monitoramento Ambiental , Poluentes Químicos da Água/análise , Água , Rios/química
3.
J Environ Manage ; 344: 118497, 2023 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-37413726

RESUMO

The heterogeneous Fenton-like systems induced by Fe-containing minerals have been largely applied for the degradation of organic pollutants. However, few studies have been conducted on biochar (BC) as an additive to Fenton-like systems mediated by iron-containing minerals. In this study, the addition of BC prepared at different temperatures was found to significantly enhance the degradation of contaminants in the tourmaline-mediated Fenton-like system (TM/H2O2) using Rhodamine B (RhB) as the target contaminant. Furthermore, the hydrochloric acid-modified BC prepared at 700 °C (BC700(HCl)) could achieve complete degradation of high concentrations of RhB in the BC700(HCl)/TM/H2O2 system. Free radical quenching experiments showed that TM/H2O2 system removed contaminants mainly mediated by the free radical pathway. After adding BC, the removal of contaminants is mainly mediated by the non-free radical pathway in BC700(HCl)/TM/H2O2 system which was confirmed by the Electron paramagnetic resonance (EPR) experiments and electrochemical impedance spectroscopy (EIS). In addition, BC700(HCl) had broad feasibility in the degradation of other organic pollutants (Methylene Blue (MB) 100%, Methyl Orange (MO) 100%, and tetracycline (TC) 91.47%) in the tourmaline-mediated Fenton-like system. Possible pathways for the degradation of RhB by the BC700(HCl)/TM/H2O2 system were also proposed.


Assuntos
Poluentes Ambientais , Peróxido de Hidrogênio , Peróxido de Hidrogênio/química , Minerais , Radicais Livres
4.
Angew Chem Int Ed Engl ; 62(36): e202309480, 2023 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-37462327

RESUMO

Artificial H2 O2 photosynthesis by covalent organic frameworks (COFs) photocatalysts is promising for wastewater treatment. The effect of linkage chemistry of COFs as functional basis to photoelectrochemical properties and photocatalysis remains a significant challenge. In this study, three kinds of azoles-linked COFs including thiazole-linked TZ-COF, oxazole-linked OZ-COF and imidazole-linked IZ-COF were successfully synthesized. More accessible channels of charge transfer were constructed in TZ-COF via the donor-π-acceptor structure between thiazole linkage and pyrene linker, leading to efficient suppression of photoexcited charge recombination. Density functional theory calculations support the experimental studies, demonstrating that the thiazole linkage is more favorable for the formation of *O2 intermediate in H2 O2 production than that of the oxazole and imidazole linkages. The real active sites in COFs located at the benzene ring fragment between pyrene unit and azole linkage.

5.
Ecotoxicol Environ Saf ; 192: 110326, 2020 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-32066004

RESUMO

Adsorption represents an attractive mean to remediate polluted water. Unfortunately, the surface positive charges, low surface area and complicated separation procedures inhibit the usability of poly (m-phenylenediamine) (PmPD) as an adsorbent for heavy metal removing. To overcome these drawbacks, a magnetic MnO2@Fe3O4/PmPD core-shell adsorbent was designed to remove heavy metals from water. The MnO2 shell, came from the redox reaction between KMnO4 and PmPD, increased the surface area and changed the surface electronegativity. MnO2@Fe3O4/PmPD could be easily separated from water. It showed a significant increase in heavy metals removal efficiency, with maximum capacities of 438.6 mg/g for Pb(II) and 121.5 mg/g for Cd(II), respectively. The affinity between heavy metals and MnO2@Fe3O4/PmPD were mainly due to electrostatic attraction, ion exchanges and coordinated interaction. Density functional theory (DFT) calculations further confirmed that Pb and Cd were bonded with O atoms. The calculated adsorption energy indicated that the (111) MnO2 facet presented stronger adsorption affinity toward Pb(II) than Cd(II). Additionally, FM150 (150 mg) could regenerate 22 L Pb(II) wastewater upon single passage through the filterable column with a flux of 20 mL/min. Thus, the present work demonstrates the promising potential of using MnO2@Fe3O4/PmPD for efficiently removing heavy metals from wastewater.


Assuntos
Óxido Ferroso-Férrico/química , Compostos de Manganês/química , Metais Pesados/química , Óxidos/química , Fenilenodiaminas/química , Águas Residuárias/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Troca Iônica , Fenômenos Magnéticos , Eletricidade Estática
6.
Small ; 15(2): e1803088, 2019 01.
Artigo em Inglês | MEDLINE | ID: mdl-30548176

RESUMO

Metal organic frameworks (MOFs), as an original kind of organic-inorganic porous material, are constructed with metal centers and organic linkers via a coordination complexation reaction. Among uncountable MOF materials, iron-containing metal organic frameworks (Fe-MOFs) have excellent potential in practical applications owing to their many fascinating properties, such as diverse structure types, low toxicity, preferable stability, and tailored functionality. Here, recent research progresses of Fe-MOFs in attractive features, synthesis, and multifunctional applications are described. Fe-MOFs with porosity and tailored functionality are discussed according to the design of building blocks. Four types of synthetic methods including solvothermal, hydrothermal, microwave, and dry gel conversion synthesis are illustrated. Finally, the applications of Fe-MOFs in Li-ion batteries, sensors, gas storage, separation in gas and liquid phases, and catalysis are elucidated, focusing on the mechanism. The aim is to provide prospects for extending Fe-MOFs in more practical applications.

7.
Small ; 15(23): e1901008, 2019 06.
Artigo em Inglês | MEDLINE | ID: mdl-30972930

RESUMO

Highly active photocatalysts driving chemical reactions are of paramount importance toward renewable energy substitutes and environmental protection. As a fascinating Aurivillius phase material, Bi2 MoO6 has been the hotspot in photocatalytic applications due to its visible light absorption, nontoxicity, low cost, and high chemical durability. However, pure Bi2 MoO6 suffers from low efficiency in separating photogenerated carriers, small surface area, and poor quantum yield, resulting in low photocatalytic activity. Various strategies, such as morphology control, doping/defect-introduction, metal deposition, semiconductor combination, and surface modification with conjugative π structures, have been systematically explored to improve the photocatalytic activity of Bi2 MoO6 . To accelerate further developments of Bi2 MoO6 in the field of photocatalysis, this comprehensive Review endeavors to summarize recent research progress for the construction of highly efficient Bi2 MoO6 -based photocatalysts. Furthermore, benefiting from the enhanced photocatalytic activity of Bi2 MoO6 -based materials, various photocatalytic applications including water splitting, pollutant removal, and disinfection of bacteria, were introduced and critically reviewed. Finally, the current challenges and prospects of Bi2 MoO6 are pointed out. This comprehensive Review is expected to consolidate the existing fundamental theories of photocatalysis and pave a novel avenue to rationally design highly efficient Bi2 MoO6 -based photocatalysts for environmental pollution control and green energy development.

8.
Ecotoxicol Environ Saf ; 184: 109597, 2019 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-31465956

RESUMO

Antibiotics can induce adverse effects on plants. Brassica crop seeds, for their advantages, are used widely in seed germination test to investigate phytotoxicity of substances. However, their performances on evaluating antibiotics remain to be studied to select sensitive species for control of potential risks. In this work, common species of Chinese cabbage (Brassica rapa L.), edible rape (Brassica napus L.), and cabbage (Brassica oleracea L.) with three cultivars each were selected to compare and analyze the sensitivity difference of their seeds to tetracycline (TC) stress. Results showed that the ratio of axis to cotyledon (RAC) by fresh weight was an alternative endpoint besides radicle length (RL) in the test. The species sensitivity distribution (SSD) based on the effective concentrations causing x% inhibition (ECx) in RL of seeds exposed to TC was applied to compare the sensitivity of seeds and estimate the hazardous concentration for x% species (HCx). From the species-dependent sensitivity and the sensitivity difference of cultivars in the same species of seeds to TC, the performance of Chinese cabbage was the best in the study. The sensitivity of seeds to TC could be evaluated by EC20 related to seed physical traits and germination indices, while the extent of seeds affected by TC could be evaluated by EC50 related to the composition of seed storage reserves. We recommended that it was a new idea to analyze responses of different seeds to TC at large scale according to seed innate characteristics.


Assuntos
Antibacterianos/toxicidade , Brassica/efeitos dos fármacos , Tetraciclina/toxicidade , Brassica/classificação , Brassica/crescimento & desenvolvimento , Germinação/efeitos dos fármacos , Sementes/classificação , Sementes/efeitos dos fármacos , Sementes/crescimento & desenvolvimento , Especificidade da Espécie
9.
J Environ Manage ; 217: 411-415, 2018 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-29627646

RESUMO

Oily scum, a hazardous by-product of petroleum industry, need to be deposed urgently to reduce environmental risks. This paper introduces catalytic wet persulfate oxidation (CWPO) process in the treatment of oily scum to realize risk relief. Under the activation of heat and Fe2+, persulfate (PS) was decomposed into sulfate radicals and hydroxyl radicals, which played a major role on the degradation of petroleum hydrocarbons. The effects of wet air oxidation (WAO) and CWPO process on the degradation of oily scum were compared. In CWPO process, the total petroleum hydrocarbons (TPHs) content of oily scum was decreased from 92.63% to 16.75%, which was still up to 70.19% in WAO process. The degradation rate of TPHs in CWPO process was about 3.38 times higher than that in WAO process. The great performance of CWPO process was also confirmed by elemental analysis, which indicated that the C and H contents of oily scum were reduced significantly by CWPO process. These results indicated that CWPO process has high potential on the degradation of oily scum for environmental protection.


Assuntos
Hidrocarbonetos/química , Petróleo , Catálise , Radical Hidroxila , Oxirredução
10.
J Environ Manage ; 205: 99-106, 2018 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-28968591

RESUMO

The application of graphene oxide (GO) has attracted increasing concerns in the past decade regarding its environmental impacts, except for the impact of GO on a metal-contaminated soil system, due to its special properties. In the present work, the effects of GO on the migration and transformation of heavy metals and soil bacterial communities in Cd-contaminant soil were systematically evaluated. Soil samples were exposed to different doses of GO (0, 1, and 2 g kg-1) over 60 days. The Community Bureau of Reference (BCR) sequential extraction procedure was used to reflect the interaction between GO and Cd. Several microbial parameters, including enzyme activities and bacterial community structure, were measured to determine the impacts of GO on polluted soil microbial communities. It was shown that Cd was immobilized by GO throughout the entire exposure period. Interestingly, the structure of the bacterial community changed. The relative abundance of the major bacterial phyla (e.g., Acidobacteria and Actinobacteria) increased, which was possibly attributed to the reduced toxicity of Cd in the presence of GO. However, GO exerted an adverse influence on the relative abundance of some phyla (e.g., WD272 and TM6). The diversity of bacterial communities was slightly restricted. The functional bacteria related to carbon and the nitrogen cycling were also affected, which, consequently, may influence the nutrient cycling in soil.


Assuntos
Bactérias , Grafite , Microbiologia do Solo , Óxidos , Solo
11.
Analyst ; 140(6): 1772-86, 2015 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-25529122

RESUMO

A comprehensive review of the development of H2S fluorescence-sensing strategies, including sensors based on chemical reactions and fluorescence resonance energy transfer (FRET), is presented. The advantages and disadvantages of fluorescence-sensing strategies are compared with those of traditional methods. Fluorescence chemosensors, especially those used in FRET sensing, are highly promising because of their low cost, technical simplicity, and their use in real-time sulfide imaging in living cells. Potential applications based on sulfate reduction to H2S, the relationship between sulfate-reducing bacteria activity and H2S yield, and real-time detection of sulfate-reducing bacteria activity using fluorescence sensors are described. The current challenges, such as low sensitivity and poor stability, are discussed.


Assuntos
Transferência Ressonante de Energia de Fluorescência/métodos , Corantes Fluorescentes/química , Sulfeto de Hidrogênio/análise , Microscopia de Fluorescência/métodos , Imagem Óptica/métodos , Animais , Compostos Aza/química , Complexos de Coordenação/química , Cobre/química , Humanos , Compostos Macrocíclicos/química , Modelos Moleculares , Nitrocompostos/química , Pontos Quânticos/química
12.
J Hazard Mater ; 469: 133806, 2024 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-38430599

RESUMO

Metal-free environmental-friendly and cost-effective catalysts for periodate (PI) activation are crucial to popularize their application for micropollutant removal in water. Herein, we report that carbon-doped boron nitride (C-BN) can efficiently activate PI to degrade acetaminophen under very low oxidant doses (40 µM) and over a relatively wide pH range (3-9). As expected, the significant reduction in periodate addition is likely to be due to the higher chemical utilization efficiency achieved by a non-radical oxidation pathway. This involved two main mechanisms, the electron transfer process mediated by the high-potential metastable C-BN-900-PI* complex and singlet oxygen. In this case, the CO groups and defects on the C-BN surface were identified as key active sites for PI activation. Notably, the prepared C-BN-900 had good cycling performance and the degradation efficiency is recovered after simple annealing. The existence of HCO3- and HA significantly inhibited the reaction, whereas Cl-, SO42-, and NO3- had little effect on the degradation of ACE. Overall, this study provides a new alternative method to regulate the non-radical pathway of boron nitride/periodate system.

13.
Water Res ; 253: 121255, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38341971

RESUMO

Tracking nitrogen pollution sources is crucial for the effective management of water quality; however, it is a challenging task due to the complex contaminative scenarios in the freshwater systems. The contaminative pattern variations can induce quick responses of aquatic microorganisms, making them sensitive indicators of pollution origins. In this study, the soil and water assessment tool, accompanied by a detailed pollution source database, was used to detect the main nitrogen pollution sources in each sub-basin of the Liuyang River watershed. Thus, each sub-basin was assigned to a known class according to SWAT outputs, including point source pollution-dominated area, crop cultivation pollution-dominated area, and the septic tank pollution-dominated area. Based on these outputs, the random forest (RF) model was developed to predict the main pollution sources from different river ecosystems using a series of input variable groups (e.g., natural macroscopic characteristics, river physicochemical properties, 16S rRNA microbial taxonomic composition, microbial metagenomic data containing taxonomic and functional information, and their combination). The accuracy and the Kappa coefficient were used as the performance metrics for the RF model. Compared with the prediction performance among all the input variable groups, the prediction performance of the RF model was significantly improved using metagenomic indices as inputs. Among the metagenomic data-based models, the combination of the taxonomic information with functional information of all the species achieved the highest accuracy (0.84) and increased median Kappa coefficient (0.70). Feature importance analysis was used to identify key features that could serve as indicators for sudden pollution accidents and contribute to the overall function of the river system. The bacteria Rhabdochromatium marinum, Frankia, Actinomycetia, and Competibacteraceae were the most important species, whose mean decrease Gini indices were 0.0023, 0.0021, 0.0019, and 0.0018, respectively, although their relative abundances ranged only from 0.0004 to 0.1 %. Among the top 30 important variables, functional variables constituted more than half, demonstrating the remarkable variation in the microbial functions among sites with distinct pollution sources and the key role of functionality in predicting pollution sources. Many functional indicators related to the metabolism of Mycobacterium tuberculosis, such as K24693, K25621, K16048, and K14952, emerged as significant important factors in distinguishing nitrogen pollution origins. With the shortage of pollution source data in developing regions, this suggested approach offers an economical, quick, and accurate solution to locate the origins of water nitrogen pollution using the metagenomic data of microbial communities.


Assuntos
Microbiota , Poluentes Químicos da Água , Nitrogênio/análise , Rios/química , RNA Ribossômico 16S , Poluição da Água/análise , Monitoramento Ambiental , China , Poluentes Químicos da Água/análise
14.
J Hazard Mater ; 460: 132316, 2023 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-37634377

RESUMO

Assisted wet deposition methods to localize the active phase metal on the carrier surface and prevent atomic aggregation during conventional heat treatment are strongly preferred. Herein, single-atom cobalt catalysts (SA-Co-PCN) with different metal-central content were target-prepared using a combination of impregnation and secondary annealing on polymerized carbon nitride (PCN) through reticular confinement. Fitting the coordination configuration of the Co-N pathway within the first coordination shell according to quantitative EXAFS indicated that the ligancy of Co-N was 4. The removal efficiency of representative micropollutants in the SA-Co-PCN/PMS system achieved 100% within 15 min. The outstanding degradation properties of micropollutants were ascribed to the SA-Co-PCN boosts PMS to a 1O2-dominated system. Moreover, the effects of substituents on the degradation behavior and ecotoxicology of sulfonamides (SAs) in PMS-activated systems were investigated in depth. The combination of DFT theoretical calculations and LC-MS further confirmed that the similar electron-rich sites on the SAs molecules allowed for commonality in the degradation pathway. Both S-N bond and C-S bond fragments became the initial attack and cleavage sites in the series of SAs. Ecotoxicity predictions indicated that most intermediates of SAs exhibited lower acute and chronic toxicity, especially acute toxicity, than the parent compounds. ENVIRONMENTAL IMPLICATION: Assisted wet deposition to localize the active phase metal on the carrier surface allows easy target formation of single-atom cobalt catalysts (SA-Co-PCN), which could boost PMS to a 1O2-dominated system for efficient oxidation of typical micropollutants. The degradation behavior and ecotoxicology of sulfonamides in the SA-Co-PCN/PMS system were investigated in depth, revealing that most intermediates of sulfonamides exhibited lower acute and chronic toxicity, especially acute toxicity, than the parent compounds. This work provides a strategy for the development of facilely prepared single-atom catalysts and contributes to the development and application potential of PMS advanced oxidation technology for water pollution control.

15.
Environ Sci Pollut Res Int ; 30(7): 19210-19223, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36227492

RESUMO

Fabrication of heterojunction photocatalysts is a promising strategy for enhancing photocatalytic activity. However, the study about traditional type-I heterojunction still remains to be developed. Herein, a PDIsa/BiOBr traditional type-I heterojunction was constructed by electrostatic self-assembly method, which owned improved light absorption capacity and photogenerated charge separation efficiency. The interfacial electric field and the polarization electric field of PDIsa impelled the separation of excitons. The degradation rate of ciprofloxacin (CIP) was improved by 3.2 times over the optimal PDIsa/BiOBr composite than pure BiOBr. In addition, the TOC removal efficiency reached 67.34% within 120 min. Trapping experiments and electron spin resonance (ESR) tests showed that superoxide radical (•O2-) was the most active species, and singlet oxygen (1O2) and hole (h+) played a secondary role. The work may furnish a new reference for designing BiOBr-based type-I heterojunction.


Assuntos
Bismuto , Ciprofloxacina , Catálise
16.
Bioresour Technol ; 386: 129447, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37399959

RESUMO

This paper examined the impacts of different pretreatments on the characteristics of biochar and its adsorption behavior for Pb2+. Biochar with combined pretreatment of water-washing and freeze-drying (W-FD-PB) performed a maximum adsorption capacity for Pb2+ of 406.99 mg/g, higher than that of 266.02 mg/g on water-washing pretreated biochar (W-PB) and 188.21 mg/g on directly pyrolyzed biochar (PB). This is because the water-washing process partially removed the K and Na, resulting in the relatively enriched Ca and Mg on W-FD-PB. And the freeze-drying pretreatment broke the fiber structure of pomelo peel, favoring the development of a fluffy surface and large specific surface area during pyrolysis. Quantitative mechanism analysis implied that cation ion exchange and precipitation were the driving forces in Pb2+ adsorption on biochar, and both mechanisms were enhanced during Pb2+ adsorption on W-FD-PB. Furthermore, adding W-FD-PB to Pb-contaminated soil increased the soil pH and significantly reduced the availability of Pb.


Assuntos
Poluentes do Solo , Água , Chumbo , Adsorção , Poluentes do Solo/química , Carvão Vegetal/química , Solo
17.
Chemosphere ; 310: 136805, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36223821

RESUMO

Natural inorganic colloids (NICs) are the most common and dominant existence in the ecosystem, with high concentration and wide variety. In spite of the low toxicity, they can alter activity and mobility of hazardous engineered nanoparticles (ENPs) through different interactions, which warrants the necessity to understand and predict the fate and transport of NICs in aquatic ecosystems. Here, this review summarized NICs properties and behaviors, interaction mechanisms and environmental factors at the first time. Various representative NICs and their physicochemical properties were introduced across the board. Then, the aggregation and sedimentation behaviors were discussed systematically, mainly concerning the heteroaggregation between NICs and ENPs. To speculate their fate and elucidate the corresponding mechanisms, the classical Derjaguin-Landau-Verwey-Overbeek (DLVO) and extended DLVO (X-DLVO) theories were focused. Furthermore, a range of intrinsic and extrinsic factors was presented in different perspective. Last but not the least, this paper pointed out theoretical and analytical gaps in current researches, and put forward suggestions for further research, aiming to provide a more comprehensive and original perspective in the fields of natural occurring colloids.


Assuntos
Ecossistema , Nanopartículas , Cinética , Nanopartículas/química , Coloides/química
18.
J Hazard Mater ; 430: 128375, 2022 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-35158240

RESUMO

With the accelerated industrialization, more and more sewage sludge (SS) needs to be treated properly. The conversion of sludge into harmless biochar material with dual utilization value of adsorption and catalysis by pyrolysis is in line with the concept of sustainable development. However, the reaction mechanisms of pristine sludge biochar (SDBC) and its composites (SDBCs) in adsorption, persulfate (PS), and Fenton-like advanced oxidation processes (AOPs) are very closely related to its adsorption performance and catalytic efficiency. In this paper, from the application mechanisms of SDBC in adsorption and AOPs, we review in detail the common methods for synthesizing SDBC and their characteristics. We discuss the synthesis techniques that affect the structural, chemical, and catalytic properties of SDBC, including gasification, pyrolysis, and hydrothermal carbonation (HTC). The pyrolysis temperature, environmental factors, and sludge characteristics have important effects on the properties of SDBC, leading to different mechanisms in adsorption and catalytic processes. Furthermore, this paper systematically generalizes the mechanisms of SDBCs in adsorption, where π-π interactions and electrostatic attractions are the main adsorption mechanisms. Then, activation mechanisms of SDBCs in PS and Fenton-like AOPs systems are discussed, including free radical pathways and non-free radical pathways. Finally, we present several challenges and perspectives for the application of SDBC and SDBCs in the field of adsorption, PS, and Fenton-like AOPs from the mechanistic point of views.


Assuntos
Poluentes Ambientais , Esgotos , Adsorção , Carvão Vegetal/química , Esgotos/química
19.
Chemosphere ; 309(Pt 1): 136419, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36152824

RESUMO

Transforming hazardous livestock manure into biochar as an advanced oxidation processes catalyst is a two-in-one strategy to treat waste by waste. In this work, a self-modified biochar catalyst obtained from chicken manure is developed for peroxymonosulfate activation to degrade levofloxacin hydrochloride. The deterioration rate of levofloxacin hydrochloride reached 89% in 40 min, after three cycles of the catalyst, the LFX still maintained 52% degradation rate. And under low levofloxacin hydrochloride concentration, the degradation rate can reach 99% within 40 min. Apart from catalyst characterization and optimization, the effects of catalyst, peroxymonosulfate, levofloxacin hydrochloride, co-existing anions, and natural organic matter concentrations during the reaction are investigated. Additionally, the quenching experiments and electron spin resonance spectroscopy both reveal the reaction mechanism. As the graphitic nitrogen combined with the sp2-hybridized carbon in biochar was highly electronegative, thus appealing electrons from neighboring carbon networks, making the adjoining carbon atoms to be positively charged, which facilitated the degradation process. The oxidative degradation of levofloxacin hydrochloride was ascribed to non-radical routes including surface-bound radicals, h+ and 1O2 mediated oxidation, the contribution rates were 91%, 93.5%, and 96.8%, respectively. Moreover, possible degradation pathways of levofloxacin hydrochloride are studied by Density Functional Theory (DFT) and LC-MS analysis. This work provides a novel method to produce chicken manure biochar by self-modified chicken manure during biochar pyrolysis for peroxymonosulfate activation in organic contaminations abatement and reveals the combined effect of graphitization and nitrogen functionalization while providing new ideas for the resource utilization of chicken manure.


Assuntos
Esterco , Nitrogênio , Animais , Galinhas , Levofloxacino , Carvão Vegetal/química , Peróxidos/química , Carbono
20.
Water Res ; 219: 118558, 2022 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-35569278

RESUMO

The widespread distribution of persistent organic pollutants (POPs) in natural waters has aroused global concern due to their potential threat to the aquatic environment. Photocatalysis represents a promising mean to remediate polluted waters with the simple assistance of solar energy. Herein, we fabricated a Co-Cl bond reinforced CoAl-LDH/Bi12O17Cl2 heterogeneous photocatalyst to investigate the feasibility of photocatalysis to treat POPs-polluted water under environmental conditions. The optimum CoAl-LDH/Bi12O17Cl2 (5-LB) composite photocatalyst exhibited excellent photocatalytic performance, which could degrade 92.47 % of ciprofloxacin (CIP) and 95 % of bisphenol A (BPA) with 2h of actual solar light irradiation in Changsha, China (N 28.12 °, E 112.59 °). In view of the synergistic influence of water constituents, various water matrices greatly affected the degradation rate of CIP (BPA), with the degradation efficiency of 82.17% (84.37%) in tap water, 69.67% (71.63%) in wastewater effluent, and 44.07% (67.7%) in wastewater inflow. The results of electron spin resonance, and chemical trapping experiment, HPLC-MS and density functional theory calculation reflected that the degradation of CIP was mainly attributed to h+ and 1O2 attacking the active atoms of CIP molecule with high Fukui index. Furthermore, the non-toxicity of both 5-LB photocatalyst and treated CIP solution was proved by E.coli and B.subtilis cultivation, which further demonstrated the feasibility of the 5-LB to treat POPs in real water under irradiation of solar light.


Assuntos
Carvão Mineral , Poluentes Orgânicos Persistentes , Catálise , Ciprofloxacina , Escherichia coli , Luz , Águas Residuárias , Água
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