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1.
Water Res ; 251: 121113, 2024 Mar 01.
Article in English | MEDLINE | ID: mdl-38215539

ABSTRACT

A novel treatment technique by coupling granular activated carbon (GAC) adsorption and ozone regeneration was constructed for long-lasting water decontamination. The GAC adsorption showed high performance for atrazine (ATZ) removal (99.9 %), and the ozone regeneration ensured the recyclability of GAC for water purification. The regeneration process was evaluated via several paths to assist the efficient adsorption process. Employing ozone micro-nano bubbles (O3-MNBs) for regenerating GAC showed superior performance compared to traditional ozone. Meantime, inhibiting the formation of bromate (BrO3-). ATZ adsorption process suffered from the pore-filling, hydrogen bonding effect and π-π EDA interaction. The surface phenolic hydroxyl group, carboxyl group and pyridine nitrogen benefitted the triggering of ozone to generate reactive oxygen species, and regenerate the GAC surface. The superior performance of the adsorption and regeneration process was verified via a long-term running by a pilot study. It significantly improved the removal of organic micropollutants, UV254 and permanganate index. Additionally, the intermittent O3-MNBs regeneration process resulted in efficient decontamination within the pores structure of GAC, which also effectively preserved the pore structure from destruction. For actual application, the cost of water production can be saved around 0.63 kWh m-3. This work proposed new ideas and theoretical support for economic water production.


Subject(s)
Atrazine , Benzenesulfonates , Ozone , Water Pollutants, Chemical , Water Purification , Charcoal/chemistry , Pilot Projects , Ozone/chemistry , Water Purification/methods , Water Pollutants, Chemical/analysis , Water , Adsorption
2.
Environ Sci Pollut Res Int ; 30(30): 75156-75169, 2023 Jun.
Article in English | MEDLINE | ID: mdl-37217816

ABSTRACT

Nano zero-valent iron (nZVI) has a great potential for arsenic removal, but it would form aggregates easily and consume largely by H+ in the strongly acidic solution. In this work, 15%CaO doped with nZVI (15%CaO-nZVI) was successfully synthesized from a simplified ball milling mixture combined with a hydrogen reduction method, which had a high adsorption capacity for As(V) removal from high-arsenic acid wastewater. More than 97% As(V) was removed by 15%CaO-nZVI under the optimum reaction conditions of pH 1.34, initial As(V) concentration 16.21 g/L, and molar ratio of Fe/As (nFe/nAs) 2.5:1. The effluent pH solution was weakly acidic 6.72, and the secondary arsenic removal treatment reduced the solid waste and improved arsenic grade in slag from the mass fraction of 20.02% to 29.07%. Multiple mechanisms including Ca2+ enhanced effect, adsorption, reduction, and co-precipitation coexisted for As(V) removal from high-arsenic acid wastewater. Doping of CaO might lead to improving cracking channels which was benefit for electronic transmission and the confusion of atomic distribution. The in situ weak alkaline environment generated on the surface of 15%CaO-nZVI would increase the content of γ-Fe2O3/Fe3O4, which was in favor for As(V) adsorption. In addition, H+ in the strongly acidic solution could accelerate corrosion of 15%CaO-nZVI and abundant fresh and reactive iron oxides continuously generated, which would provide plenty specific reactive site and fast charge transfer and ionic mobility for arsenic removal.


Subject(s)
Arsenic , Water Pollutants, Chemical , Water Purification , Iron/chemistry , Arsenic/analysis , Wastewater , Water Pollutants, Chemical/analysis , Oxides/chemistry , Adsorption
3.
Environ Sci Technol ; 57(16): 6723-6732, 2023 04 25.
Article in English | MEDLINE | ID: mdl-37043741

ABSTRACT

Identifying reactive species in advanced oxidation process (AOP) is an essential and intriguing topic that is also challenging and requires continuous efforts. In this study, we exploited a novel AOP technology involving peracetic acid (PAA) activation mediated by a MnII-nitrilotriacetic acid (NTA) complex, which outperformed iron- and cobalt-based PAA activation processes for rapidly degrading phenolic and aniline contaminants from water. The proposed MnII/NTA/PAA system exhibited non-radical oxidation features and could stoichiometrically oxidize sulfoxide probes to the corresponding sulfone products. More importantly, we traced the origin of O atoms from the sulfone products by 18O isotope-tracing experiments and found that PAA was the only oxygen-donor, which is different from the oxidation process mediated by high-valence manganese-oxo intermediates. According to the results of theoretical calculations, we proposed that NTA could tune the coordination circumstance of the MnII center to elongate the O-O bond of the complexed PAA. Additionally, the NTA-MnII-PAA* molecular cluster presented a lower energy gap than the MnII-PAA complex, indicating that the MnII-peroxy complex was more reactive in the presence of NTA. Thus, the NTA-MnII-PAA* complex exhibited a stronger oxidation potential than PAA, which could rapidly oxidize organic contaminants from water. Further, we generalized our findings to the CoII/PAA oxidation process and highlighted that the CoII-PAA* complex might be the overlooked reactive cobalt species. The significance of this work lies in discovering that sometimes the metal-peroxy complex could directly oxidize the contaminants without the further generation of high-valence metal-oxo intermediates and/or radical species through interspecies oxygen and/or electron transfer.


Subject(s)
Coordination Complexes , Water Pollutants, Chemical , Peracetic Acid , Oxygen , Metals , Coordination Complexes/chemistry , Cobalt , Oxidation-Reduction , Water , Hydrogen Peroxide
4.
J Hazard Mater ; 453: 131322, 2023 07 05.
Article in English | MEDLINE | ID: mdl-37043851

ABSTRACT

A nationwide study of the occurrence, distribution, potential drivers, and ecological risks of 24 quinolone antibiotics (QNs) in 74 Chinese sludge samples from 48 wastewater treatment plants (WWTPs) was conducted. In domestic sludge, the ∑QNs concentrations were  3rd-generation QNs > 4th-generation QNs > 1st-generation QNs. Meanwhile, abundant veterinary and human/veterinary quinolones (

Subject(s)
Quinolones , Water Pollutants, Chemical , Humans , Sewage/analysis , Moxifloxacin , Water Pollutants, Chemical/analysis , Anti-Bacterial Agents/analysis , Quinolones/analysis , Risk Assessment , Ofloxacin , China , Environmental Monitoring
5.
Environ Sci Pollut Res Int ; 30(13): 38480-38499, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36577825

ABSTRACT

In this study, a novel in situ iron-loaded activated carbon (AFPAC) was prepared by a FeSO4/K2FeO4 impregnation and oxidation combination two-step supported on activated carbon for enhanced removal of Cr(VI) from aqueous solutions. Cr(VI) removal efficiency greatly increased by AFPAC more than 70% than that of fresh activated carbon (AC), which is due to rich iron oxides formed in situ and the synergistic effect between iron oxides and activated carbon. Cr(VI) adsorption behaviors on AFPAC under different water quality parameters were investigated. The maximum monolayer adsorption capacities for Cr(VI) by AFPAC are as high as 26.24 mg/g, 28.65 mg/g, and 32.05 mg/g at 25 °C, 35 °C and 45 °C at pH 4, respectively. Density functional theory (DFT) results showed that the adsorption energy of K2Cr2O7 on the surface of FeOOH was - 2.52 eV, which was greater than that on the surface of bare AC, and more charge transfer occurred during the adsorption of K2Cr2O7 on the surface of FeOOH, greatly promoting the formation of Cr = O-Fe. Cr(VI) removal by AFPAC included electrostatic attraction, redox reaction, coordinate complexation, and co-precipitation. Cr(VI) adsorption process on AFPAC consisted of the three reaction steps: (1) AFPAC was fast protonation and Cr2O72- would electrostatically attract to the positively charged AFPAC surface. (2) Cr2O72- was reduced into Cr2O3 by the carbons bond to the oxygen functionalities on activated carbon and the redox reaction process of FeSO4 and K2FeO4. (3) The inner-sphere complexes were formed, and adsorbed on AFPAC by iron oxides and then co-precipitation.


Subject(s)
Iron , Water Pollutants, Chemical , Iron/chemistry , Charcoal/chemistry , Water Pollutants, Chemical/analysis , Chromium/chemistry , Adsorption , Ferrous Compounds , Oxides
6.
Chemosphere ; 313: 137251, 2023 Feb.
Article in English | MEDLINE | ID: mdl-36395895

ABSTRACT

This study was carried out to investigate the enhanced removal of arsenite (As(III)) by potassium ferrate (K2FeO4) coupled with three Al-based coagulants, which focused innovatively on the distribution and transformation of hydrolyzed aluminum species as well as the mechanism of K2FeO4 interacted with different aluminum hydrolyzed polymers during As(III) removal. Results demonstrated that As(III) removal efficiency could be substantially elevated by K2FeO4 coupled with three Al-based coagulants treatment and the optimum As(III) removal effect was occurred at pH 6 with more than 97%. K2FeO4 showed a great effect on the distribution and transformation of aluminum hydrolyzed polymers and then coupled with a variety of aluminum species produced by the hydrolysis of aluminum coagulants for arsenic removal. During enhanced coagulation, arsenic removal by AlCl3 was main through the charge neutralization of in situ Al13 and the sweep flocculation of Al(OH)3, while PACl1 mainly depended on the charge neutralization of preformed Al13 and the bridging adsorption of Al13 aggregates, whereas PACl2 mainly relied on the sweep flocculation of Al(OH)3. This study provided a new insight into the distribution and transformation of aluminum species for the mechanism of As(III) removal by K2FeO4 coupled with different Al-based coagulants.


Subject(s)
Arsenic , Water Purification , Aluminum , Water Purification/methods , Aluminum Hydroxide , Polymers , Flocculation
7.
Environ Sci Pollut Res Int ; 30(4): 10697-10709, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36083368

ABSTRACT

It is well known the capacity of potassium ferrate (Fe(VI)) for the oxidation of pollutants or co-precipitation and adsorption of hazardous species. However, little information has been paid on the adsorption and co-precipitation contribution of the Fe(VI) resultant nanoparticles, the in situ hydrolytic ferric iron oxides. Here, the removal of arsenate (As(V)) and arsenite (As(III)) by Fe(VI) was investigated, which focused on the interaction mechanisms of Fe(VI) with arsenic, especially in the contribution of the co-precipitation and adsorption of its hydrolytic ferric iron oxides. pH and Fe(VI) played significant roles on arsenic removal; over 97.8% and 98.1% of As(V) and As(III) removal were observed when Fe(VI):As(V) and Fe(VI):As(III) were 24:1 and 16:1 at pH 4, respectively. The removal of As(V) and As(III) by in situ and ex situ formed hydrolytic ferric iron oxides was examined respectively. The results revealed that As(III) was oxidized by Fe(VI) to As(V), and then was removed though co-precipitation and adsorption by the hydrolytic ferric iron oxides with the contribution content was about 1:3. For As(V), it could be removed directly by the in situ formed particles from Fe(VI) through co-precipitation and adsorption with the contribution content was about 1:1.5. By comparison, As(III) and As(V) were mainly removed through adsorption by the 30-min hydrolytic ferric iron oxides during the ex situ process. The hydrolytic ferric iron oxides size was obviously different in the process of in situ and ex situ, possessing abundant and multiple morphological structures ferric oxides, which was conducive for the efficient removal of arsenic. This study would provide a new perspective for understanding the potential of Fe(VI) treatment on arsenic control.


Subject(s)
Arsenic , Arsenites , Nanoparticles , Water Pollutants, Chemical , Arsenates , Arsenic/chemistry , Iron/chemistry , Ferric Compounds , Oxidation-Reduction , Oxides/chemistry , Adsorption , Water Pollutants, Chemical/chemistry , Hydrogen-Ion Concentration
8.
Molecules ; 27(22)2022 Nov 19.
Article in English | MEDLINE | ID: mdl-36432133

ABSTRACT

This study identified and detected the existence of major pollutants in northeast China. As an alpine region and an agricultural base, this region has representative significance in pollution research. We selected 56 samples from drinking water sources of typical villages and towns, focusing on the analysis of heavy metals and organic micropollutants in northeast China. The analysis results showed that Fe and Mn were the main metal elements exceeding the standard. The exceeding rates were 17.9% and 19.6%. Experiments showed that there were 19 kinds of pesticides, 6 kinds of OPEs, 2 kinds of PAEs, 22 kinds of PPCPs. The detection rate of these 49 kinds of organic micro-pollutants were 1.79~82.14%. The characteristics of organic pollution were extensive and varied. Many underground water samples had high level of micropollutants. The water quality parameters of drinking water sources in villages and towns showed close relation to local geological conditions and agricultural activities. Actions must be taken to control these parameters from the source of pollution.


Subject(s)
Drinking Water , Environmental Pollutants , Metals, Heavy , Drinking Water/analysis , Cities , Metals, Heavy/analysis , Water Quality , Environmental Pollutants/analysis , China
9.
Molecules ; 27(21)2022 Nov 02.
Article in English | MEDLINE | ID: mdl-36364281

ABSTRACT

Natural organic matter (NOM) has always been considered the main precursor of disinfection by-products (DBPs) during the chlorine disinfection of drinking water. This research focuses on investigating the correlation between the functional group (carboxyl and carbonyl groups) content of NOM and the formation of trichloromethane (TCM) and chloral hydrate (CH). The quantitative determination of carboxyl groups, carbonyl groups, TCM, and CH were conducted during the drinking water treatment processes with different coagulant dosages and with/without pre-oxidation by KMnO4 or NaClO. The most appropriate coagulant for the removal of conventional components was polyaluminum chloride (PAC), and the dosage was 110 mg/L. Up to 43.7% and 14.5% of the carboxyl and carbonyl groups, respectively, were removed through the coagulation and sedimentation processes, which can be enhanced by increasing PAC dosage. The filtration process further increased the removal rates of these two functional groups to 59.8% and 33.5%, respectively. The formation potential of the TCM and CH decreased as the PAC dosage increased. Pre-oxidation by KMnO4 (0.8-1.0 mg/L) effectively controlled the formation of DBPs while increasing the carboxyl and carbonyl group content. Pre-oxidation by NaClO decreased the formation of TCM rather than CH, and a suitable amount (0.5-1.0 mg/L) decreased the carboxyl and carbonyl groups. It was found that there was a good linear correlation between carboxyl groups and TCM and CH. The linear fit R2 values of the carboxyl groups to TCM and CH were 0.6644 and 0.7957, respectively. The linear fit R2 values of the carbonyl groups to TCM and CH were 0.5373 and 0.7595, respectively.


Subject(s)
Disinfectants , Drinking Water , Water Pollutants, Chemical , Water Purification , Trihalomethanes/analysis , Chloral Hydrate/analysis , Drinking Water/analysis , Chlorine/analysis , Disinfection , Chloroform , Water Pollutants, Chemical/analysis , Halogenation , Disinfectants/analysis
10.
Chemosphere ; 308(Pt 1): 136264, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36064014

ABSTRACT

Peroxymonosulfate (PMS)-based advanced oxidation process is considered a potential technology for water treatment. Here, palygorskite (PAL)-mediated cobalt-copper-ferrite nanoparticles (16%-CoCu0.4Fe1·6O4@PAL, donated as 16%-CCFO@PAL) were employed for PMS activation to remove bisphenol S (BPS). BPS degradation was greater than 99% under the optimal conditions within 25 min, on which the effects of various influencing factors were explored. The adsorption dissociation energy of PMS over 16%-CCFO@PAL was -6.27 eV, which was lower than that of the Cu-free catalyst (-6.15 eV), demonstrating the excellent catalytic ability of 16%-CCFO@PAL. The efficient catalytic ability of 16%-CCFO@PAL was also verified in real water samples. The oxidation intermediates were identified and their generations were systematically analyzed by DFT calculations. The possible degradation pathways of BPS were proposed and the toxicity of products was predicted. BPS affected the normal development of zebrafish embryos and the levels of sex hormone in adult male zebrafish, and was harmful to the tissues, such as testis, liver, and intestine of zebrafish. The 16%-CCFO@PAL/PMS process can effectively reduce the toxicity of BPS-polluted water. This study paves the way for the real application of 16%-CCFO@PAL/PMS oxidation process and provides a new perspective for the evaluation of water toxicity.


Subject(s)
Nanoparticles , Water Pollutants, Chemical , Animals , Cobalt/toxicity , Copper/toxicity , Ferric Compounds , Magnesium Compounds , Male , Peroxides , Phenols , Silicon Compounds , Sulfones , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/toxicity , Zebrafish
11.
Chemosphere ; 301: 134769, 2022 Aug.
Article in English | MEDLINE | ID: mdl-35500634

ABSTRACT

The severe cold in winter with harsh natural conditions in Northeastern China seriously affect the water quality of the reservoir, showing the increased content and more complex types of organic matter, which brings severe challenges to the control of disinfection by-products (DBPs) in drinking water treatment with reservoir water as the water source. In this study, the fractions of dissolved organic matter (DOM) in source water at before ice formation period (P1), ice-age period (P2), and ice begin to melt period (P3) were separated by membrane separation technology. Subsequently, the contributions of DOM fractions with different molecular weights (MW) to DOC, UV254, and SUVA254, and their disinfection by-product formation potential (DBPFP) were evaluated. Although DOM with high MW (5-10 kDa) contributed the most to dissolved organic carbon (DOC) and UV254, but the contribution of DOM with low MW (0-1 kDa) to DBPs formation could not be ignored, especially during ice-age period. There was no significant difference in the total numbers of DOM formula belonged to low MW fraction at these three periods, mainly including lignin, followed by N-containing saturated compounds and tannins. Additionally, redundancy analysis revealed that DOC and UV254 as the predictors had good correlation with DBPFP, while SUVA254 could not be used as a single indicator to predict the generation potential of DBPs, and could be used as the prediction factors together with AImodwa parameter closely related to DBPFP. The study provided key information for controlling the DBPs formation of DOM in water, especially in the ice-age period, and provided the theoretical basis for water plant production.


Subject(s)
Water Pollutants, Chemical , Water Purification , Disinfection , Dissolved Organic Matter , Halogenation , Ice , Water Pollutants, Chemical/analysis
12.
J Hazard Mater ; 435: 128968, 2022 08 05.
Article in English | MEDLINE | ID: mdl-35487000

ABSTRACT

Extensive studies revealed that Cl- could inhibit the removal of targeted pollutants under low Cl- conditions in the peroxymonosulfate (PMS) system. However, the enhanced effect of Cl- has always been overlooked under high Cl- conditions. Here, we find that high concentration of Cl- played a critical role in bisphenol S (BPS) degradation by activating PMS using 16%-CoFe2O4@PAL (16%-CFO@PAL). The removal of BPS was sharply enhanced after introducing 0.5 and 1.0 M Cl-, and the corresponding kobs increased to 0.922 min-1 and 1.103 min-1, which was 6-fold and 7-fold higher than the control (0.144 min-1), respectively. HOCl was demonstrated as the dominant species for removing BPS in 16%-CFO@PAL/PMS system under high Cl- circumstances. The typical chlorinated BPS intermediates were identified, which showed higher eco-toxicity than BPS. The chlorinated byproducts along with their toxicity could be effectively eliminated after 30 min. The possible formation mechanism of chlorinated products was further revealed by theoretical calculations. Toxicity assessment experiments showed that BPS significantly affected hormone levels of zebrafish and showed toxicity on the testis and liver of zebrafish, which could be reduced using 16%-CFO@PAL/PMS system. This study attracts attention to the overlooked HOCl in PMS-based processes under high salinity conditions.


Subject(s)
Salinity , Water Pollutants, Chemical , Animals , Peroxides , Phenols , Sulfones , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/toxicity , Zebrafish
13.
J Hazard Mater ; 432: 128757, 2022 06 15.
Article in English | MEDLINE | ID: mdl-35344892

ABSTRACT

Novel nitrogen (N)-doped cellulose biochar (NC1000-10) with large adsorption capacity (103.59 mg g-1) for atrazine (ATZ) was synthesized through the one-pot method. It has the best adsorption efficiency than N-doped biochars prepared from hemicellulose and lignin. The adsorption behaviors of ATZ by N-doped biochars with different N doping ratios (NC1000-5, NC1000-10, NC1000-20 and NC1000-30) were significantly different, which was attributed to the difference of sp2 conjugate C (ID/IG = 0.99-1.18) and doped heteroatom N (pyridinic N, pyrrolic N and graphitic N). Adsorption performance of ATZ on NC1000-10 conformed to the pseudo-second-order kinetic and Langmuir adsorption isotherm model. Thermodynamic calculations showed that adsorption performance was favorable. Besides, wide pH adaptability (pH = 2-10), good resistance to ionic strength and excellent recycling efficiency make it have extensive practical application potential. Further material characterizations and the density functional theory (DFT) calculations indicated that good adsorption performance of NC1000-10 for ATZ mainly depended on chemisorption, and π-π electron donor-acceptor (EDA) interaction contributed the most due to high graphitization degree. Specifically, pyridinic N and graphitic N further promoted adsorption performance by hydrophobic effect and π-π EDA interaction between ATZ and NC1000-10, respectively. Pyrrolic N and other surface functional groups (-COOH, -OH) facilitated the hydrogen bond effect.


Subject(s)
Atrazine , Water Pollutants, Chemical , Adsorption , Charcoal/chemistry , Electrons , Kinetics , Oxidants , Water Pollutants, Chemical/analysis
14.
Sci Total Environ ; 825: 153706, 2022 Jun 15.
Article in English | MEDLINE | ID: mdl-35143787

ABSTRACT

In this study, the dissolved organic matter (DOM) profiles of water samples from a water source in northeastern China were analyzed by high-resolution mass spectrometry (HRMS), and its changes after chlorination were investigated. The results showed that lignin substances accounted for a significant proportion in DOM and chlorinated products and were the main precursors of disinfection by-products (DBPs). During disinfection, macromolecular DOM was transformed into small molecules, and lignin substances have the most obvious and complex changes in reaction. Two lignin monomers 4-propylphenol (4PP) and 4-propylguaiacol (4PG) were used as model compounds to study their reaction kinetics and degradation pathways during disinfection. The degradation of both lignin monomers conformed to pseudo-first-order reaction kinetics, and the reaction rate constant of 4PG was higher than that of 4PP. The effects of chlorine dosage, pH and temperature on the degradation reaction kinetics of two lignin monomers were investigated. The degradation rates of 4PP and 4PG increased with increasing chlorine dosage, pH and temperature. The two monomers showed similar properties in the chlorination degradation process, and generated multiple intermediates, which were mainly transformed into small molecules by chlorine electrophilic substitution and nucleophilic substitution, and further generated DBPs.


Subject(s)
Disinfectants , Water Pollutants, Chemical , Water Purification , Chlorine/chemistry , Disinfectants/analysis , Disinfection/methods , Halogenation , Lignin , Water , Water Pollutants, Chemical/analysis , Water Purification/methods
15.
J Hazard Mater ; 428: 128264, 2022 04 15.
Article in English | MEDLINE | ID: mdl-35051770

ABSTRACT

The regrowth of chlorine-resistant bacteria in drinking water can deteriorate water quality. The study evaluated the relationship between organic carbon and the regrowth potential of chlorine-resistant bacteria remaining in chloraminated water samples. The results showed that the community structure of bacteria changed with the increase of chloramine dosage. The order in which organic carbon utilized by bacteria was affected by the composition of bacterial community. The biodegradable dissolved organic carbon (BDOC), assimilable organic carbon (AOC), bacterial regrowth potential (BRP) and total cell concentration (TCC) in cultivated water sample after disinfection with 1.8 mg/L chloramine increased form 0.22 mg/L, 33.68 µg/L, 2.70 × 105 cells/mL and 3.48 × 104 cells/mL before cultivation to 1.20 mg/L, 193.90 µg/L, 4.74 × 105 cells/mL and 1.46 × 105 cells/mL, respectively. The increase of TCC did not result in the decrease of BDOC, AOC and BRP in the cultivated water samples. The results showed that other biodegradable organic carbon in chloraminated water samples assimilated by residual chlorine-resistant bacteria besides AOC, BDOC, and organic carbon assimilated by indigenous bacteria. AOC, BDOC, and BRP indicators used to characterize the biostability of drinking water were not enough to accurately assess the regrowth potential of chlorine-resistant bacteria remaining in drinking water. It is suggested to supplement the index of TCC in cultivated water samples, which might be able to more accurately evaluate the regrowth potential of chlorine-resistant bacteria remaining in drinking water.


Subject(s)
Drinking Water , Water Purification , Bacteria , Carbon/analysis , Chlorine/analysis , Water Microbiology , Water Supply
16.
J Hazard Mater ; 428: 128191, 2022 04 15.
Article in English | MEDLINE | ID: mdl-35033910

ABSTRACT

This study found that peroxymonosulfate (PMS) oxidation without activation has the potential to generate a suspected human carcinogen, N-nitrosodimethylamine (NDMA), in water containing N,N-dimethylhydrazine compounds. Considerable amounts of NDMA formed from three compounds by PMS oxidation were observed. 1,1,1',1'-Tetramethyl-4,4'-(methylene-di-p-phenylene) disemicarbazide (TMDS), which is an industrial antiyellowing agent and light stabilizer, was used as a representative to elucidate the kinetics, transformation products, mechanism and NDMA formation pathways of PMS oxidation. TMDS degradation and NDMA formation involved direct PMS oxidation and singlet oxygen (1O2) oxidation. The oxidation by PMS/1O2 was pH-dependent, which was related to the pH-dependent characteristics of the reactive oxygen species and intermediates. The degradation mechanism of TMDS mainly included the side chain cleavage, dealkylation, and O-addition. NDMA was generated from TMDS mainly via O-addition and 1,1-dimethylhydrazine (UDMH) generation. The cleavage of amide nitrogen in O-addition products and primary amine nitrogen in UDMH are likely the key steps in NDMA generation. The results emphasized that the formation of harmful by-products should be taken into account when assessing the feasibility of PMS oxidation.


Subject(s)
Dimethylnitrosamine , Water Pollutants, Chemical , Dimethylhydrazines , Humans , Kinetics , Oxidation-Reduction , Peroxides , Water Pollutants, Chemical/analysis
17.
Chemosphere ; 287(Pt 3): 132260, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34543907

ABSTRACT

Cementitious membrane (CM) is a promising microfiltration membrane with low cost for raw materials and low energy consumption of non-sintering fabrication process. A novel carbon-cementitious microfiltration membrane (CCM) was fabricated with powdered activated carbon (PAC) as an additive based on CM, to solve the low mechanical strength of CM during multiple practical uses. While maintaining adequate pure water flux and porosity, the mechanical strength of the membrane was greatly improved to ensure the stability of the membrane in the filtration process. The bending strength of the CCM was 2-3 times higher than that of CM. 10 wt% CCM has the smallest critical pore size and optimal permeability, which was chosen to be the optimal PAC doping ratio. The X-ray diffraction and FT-IR results indicated that the addition of PAC did not change the mineral composition of cement hydration products, and the appropriate amount of PAC acted as a nucleation site and accelerated hydration. The effect of size effect on bending strength was more obvious with the decrease of membrane thickness. In the membrane adsorption experiments of benzophenone-4, nitrobenzene and p-chloronitrobenzene, the CCM exhibited prominent adsorption properties than CM. These results broaden the application scope of microfiltration membranes in water treatment process.


Subject(s)
Charcoal , Water Purification , Adsorption , Membranes, Artificial , Powders , Spectroscopy, Fourier Transform Infrared
18.
Chemosphere ; 289: 133198, 2022 Feb.
Article in English | MEDLINE | ID: mdl-34890616

ABSTRACT

Iohexol as an iodinated X-ray contrast agent is widely used, and it is the potential precursor for toxic iodinated disinfection by-products in the disinfection process. In this study, a series of CuFe2O4 catalysts were prepared by sol-gel method with different molar ratios of total metal cations to citric acid ([Men+]T/CA) and employed as heterogeneous catalysts to activate peroxymonosulfate (PMS) for the removal of iohexol. The catalysts were characterized by various technologies, and the effect of [Men+]T/CA molar ratio on the catalysts' properties was explored. The CuFe2O4 synthesized with [Men+]T/CA molar ratio of 1:1 showed the best catalytic activity to PMS, and 95.0% of 1.0 mg/L iohexol was removed within 15 min by using 50 mg/L CuFe2O4 and 20 mg/L PMS. The quenching experiment and electron spin resonance (ESR) spectra indicated the generation of SO4- and OH in the CuFe2O4/PMS system, and the quantity experiments revealed that the generation concentration of SO4- was ten times higher than that of OH. The generation mechanism of SO4- and ·OH were investigated by ATR-FTIR and X-ray photoelectron spectroscopy (XPS) spectra. The effects of catalyst dosage, PMS and iohexol concentration on the removal of iohexol were studied, and various water matrix factors including solution pH, natural organic matter (NOM) concentration and inorganic ions were also considered. Based on the twelve intermediate products of iohexol detected by UPLC-QTOF/MS, the degradation pathway was proposed. The high catalytic activity and reusability of CuFe2O4 indicated that CuFe2O4 activating PMS is an effective and sustainable way for the treatment of iohexol.


Subject(s)
Iohexol , Water , Catalysis , Peroxides
19.
Environ Pollut ; 293: 118524, 2022 Jan 15.
Article in English | MEDLINE | ID: mdl-34793916

ABSTRACT

Although concerns have been raised about co-selection for antibiotic resistance and various antibiotics and non-antibiotic agents, the data on their association in urban sludge is still limited. In addition, antibiotic contamination can result in not only the toxicity but also the antibiotic resistance. In this study, the first large-scale identification of antibiotics and non-antibiotic agents concern for co-selection of resistance against antibiotics was conducted in urban sludge. Co-occurrence analysis showed that antibiotic resistance genes (ARGs) had no significant correlation with the corresponding antibiotics. Therefore, the results of co-occurrence analysis based on antibiotic concentration and ARG abundance were always ambiguous and difficult to interpret. However, antibiotic resistance was positively correlated with highly toxic compounds such as diclofenac, enrofloxacin and nicotine, suggesting that environmental contaminants might influence antibiotic resistance while exerting toxicity through mechanisms such as changes in microbial community and enzyme activity. The close correlation between class 1 integrase gene (intI1) and diclofenac/enrofloxacin indicated that the co-selection scenario between environmental contaminants and ARGs was likely mediated via intI1. In total, the derived co-occurrence patterns improve our understanding of the co-selection between ARGs, antibiotics and non-antibiotic agents, and also reaffirm the importance of potential role of non-antibiotic agents in the global spread of antibiotic resistance.


Subject(s)
Anti-Bacterial Agents , Microbiota , Anti-Bacterial Agents/toxicity , Drug Resistance, Microbial/genetics , Genes, Bacterial , Sewage
20.
J Agric Food Chem ; 69(50): 15362-15373, 2021 Dec 22.
Article in English | MEDLINE | ID: mdl-34904826

ABSTRACT

Black tea, as the most consumed kind of tea, is shown to have beneficial effects on human health. However, its impact on particulate matter (PM) induced lung injury and the mechanisms involved have been sparsely addressed. Here, we show that PM-exposed mice exhibited oxidative stress and inflammation in the lungs, which was significantly alleviated by a daily intake of black tea infusion (TI) in a concentration-dependent manner. Interestingly, both the ethanol-soluble fraction (ES) and the ethanol precipitate fraction (EP) exhibited better effects than those of TI; moreover, EP tended to have stronger protection than ES in some indicators, implying that EP played a dominant role in the prevention effects. Furthermore, fecal microbiota transplantation (FMT) revealed that the gut microbiota was differentially reshaped by TI and its fractions were able to directly alleviate the injury induced by PMs. These results indicate that daily intake of black tea and its fractions, especially EP, may alleviate particulate matter-induced lung injury via the gut-lung axis in mice. In addition, the Lachnospiraceae_NK4A136_group could be the core gut microbe contributing to the protection of EP and thus should be further studied in the future.


Subject(s)
Camellia sinensis , Lung Injury , Animals , Lung , Lung Injury/etiology , Lung Injury/prevention & control , Mice , Mice, Inbred C57BL , Particulate Matter/toxicity , Tea
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