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1.
Chemosphere ; : 142322, 2024 May 16.
Article in English | MEDLINE | ID: mdl-38761823

ABSTRACT

Selecting and cultivating low-accumulating crop varieties (LACVs) is the most effective strategy for the safe utilization of di-(2-ethylhexyl) phthalate (DEHP)-contaminated soils, promoting cleaner agricultural production. However, the adsorption-absorption-translocation mechanisms of DEHP along the root-shoot axis remains a formidable challenge to be solved, especially for the research and application of LACV, which are rarely reported. Here, systematic analyses of the root surface ad/desorption, root apexes longitudinal allocation, uptake and translocation pathway of DEHP in LACV were investigated compared with those in a high-accumulating crop variety (HACV) in terms of the root-shoot axis. Results indicated that DEHP adsorption was enhanced in HACV by root properties, elemental composition and functional groups, but the desorption of DEHP was greater in LACV than HACV. The migration of DEHP across the root surface was controlled by the longitudinal partitioning process mediated by root tips, where more DEHP accumulated in the root cap and meristem of LACV due to greater cell proliferation. Furthermore, the longitudinal translocation of DEHP in LACV was reduced, as evidenced by an increased proportion of DEHP in the root apoplast. The symplastic uptake and xylem translocation of DEHP were suppressed more effectively in LACV than HACV, because DEHP translocation in LACV required more energy, binding sites and transpiration. These results revealed the multifaceted regulation of DEHP accumulation in different choysum (Brassica parachinensis L.) varieties and quantified the pivotal regulatory processes integral to LACV formation.

2.
J Hazard Mater ; 471: 134439, 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38677123

ABSTRACT

Microcystins (MCs) have a significant influence on aquatic ecosystems, but little is known about their terrestrial fate and impact. Here, we investigated the fate of two MCs (MC-LR and MC-RR) in the soil-earthworm system, with consideration of their congener-specific impact on earthworm health, soil bacteria, and soil metabolome. Although MCs had little acute lethal effect on earthworms, they caused obvious growth inhibition and setae rupture. Relative to MC-RR, MC-LR exhibited higher bioaccumulation and the resulting dermal lesions and deformation of longitudinal muscles. While the incorporation of both MCs into soils stimulated pathogenic bacteria and depressed oxidative stress tolerant bacteria, the response among soil nitrification and glutathione metabolism differed between the two congeners. The dissipation kinetics of MCs obeyed the first-order model. Earthworms stimulated soil N-cycling enzyme activities, increased the abundance of MC-degrading bacteria, and promoted bacterial metabolic functions related to glutathione metabolism, xenobiotics biodegradation, and metabolism of amino acids that comprise MCs, which accelerated the dissipation of MC-LR and MC-RR by 227% and 82%, respectively. These results provide evidence of significant congener differences in the terrestrial fate and impact of MCs, which will enable a better understanding of their role in mediating soil functions and ecosystem services.


Subject(s)
Microcystins , Oligochaeta , Soil Microbiology , Soil Pollutants , Animals , Oligochaeta/metabolism , Soil Pollutants/metabolism , Soil Pollutants/toxicity , Microcystins/metabolism , Microcystins/toxicity , Soil/chemistry , Glutathione/metabolism , Biodegradation, Environmental , Bacteria/metabolism , Bioaccumulation
3.
J Hazard Mater ; 469: 133972, 2024 May 05.
Article in English | MEDLINE | ID: mdl-38461665

ABSTRACT

Di-n-butyl phthalate (DBP) is one of the most extensively used phthalic acid esters (PAEs) and is considered to be an emerging, globally concerning pollutant. The genus Streptomyces holds promise as a degrader of various organic pollutants, but PAE biodegradation mechanisms by Streptomyces species remain unsolved. In this study, a novel PAE-degrading Streptomyces sp. FZ201 isolated from natural habitats efficiently degraded various PAEs. FZ201 had strong resilience against DBP and exhibited immediate degradation, with kinetics adhering to a first-order model. The comprehensive biodegradation of DBP involves de-esterification, ß-oxidation, trans-esterification, and aromatic ring cleavage. FZ201 contains numerous catabolic genes that potentially facilitate PAE biodegradation. The DBP metabolic pathway was reconstructed by genome annotation and intermediate identification. Streptomyces species have an open pangenome with substantial genome expansion events during the evolutionary process, enabling extensive genetic diversity and highly plastic genomes within the Streptomyces genus. FZ201 had a diverse array of highly expressed genes associated with the degradation of PAEs, potentially contributing significantly to its adaptive advantage and efficiency of PAE degradation. Thus, FZ201 is a promising candidate for remediating highly PAE-contaminated environments. These findings enhance our preliminary understanding of the molecular mechanisms employed by Streptomyces for the removal of PAEs.


Subject(s)
Diethylhexyl Phthalate , Environmental Pollutants , Phthalic Acids , Esters/metabolism , Phthalic Acids/metabolism , Dibutyl Phthalate/metabolism , Biodegradation, Environmental , Ecosystem , Diethylhexyl Phthalate/metabolism
4.
J Hazard Mater ; 466: 133571, 2024 Mar 15.
Article in English | MEDLINE | ID: mdl-38266588

ABSTRACT

Microbe-mediated DBP (dibutyl phthalate) mineralization is acknowledged to be affected by diverse extracellular factors. However, little is known about the regulatory effects from quorum sensing (QS) signals. In this study, extracellularly applied QS signals A-like (hydroxymethyl dihydrofuran) was discovered to significantly enhance DBP degradation efficiency in Streptomyces sp. SH5. Monobutyl phthalate, protocatechuic acid and beta-ketoadipate were discovered as degradation intermediates by HPLC-TOF-MS/MS. Multi-omics analysis revealed the up-regulation of multiple hydrolases, transferases and decarboxylases that potentially contributed to A-like accelerated DBP degradation. Transcription of Orf2708, an orthologue of global transcriptional activator, was significantly induced by A-like. Orf2708 was demonstrated to interact specifically with the promoter of hydrolase orf2879 gene by EMSA, and the overexpression of orf2879 led to an enhanced DBP degradation in SH5. Taken together with the molecular docking studies showing the stability of ligand-receptor complex of A-like and its potential receptor Orf3712, a hierarchical regulatory cascade underlying the QS signal mediated DBP degradation was proposed as A-like/Orf3712 duplex formation, enhanced orf2708 expression and the downstream specific activation of hydrolase Orf2879. Our study presents the first evidence of GBLs-type promoted DBP degradation among bacteria, and the elucidated signal transduction path indicates a universal application potential of this activation strategy.


Subject(s)
Quorum Sensing , Tandem Mass Spectrometry , Molecular Docking Simulation , Dibutyl Phthalate/metabolism , Hydrolases/metabolism , Signal Transduction
5.
Nat Food ; 5(1): 72-82, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38177223

ABSTRACT

Dietary exposure to methylmercury (MeHg) causes irreversible damage to human cognition and is mitigated by photolysis and microbial demethylation of MeHg. Rice (Oryza sativa L.) has been identified as a major dietary source of MeHg. However, it remains unknown what drives the process within plants for MeHg to make its way from soils to rice and the subsequent human dietary exposure to Hg. Here we report a hidden pathway of MeHg demethylation independent of light and microorganisms in rice plants. This natural pathway is driven by reactive oxygen species generated in vivo, rapidly transforming MeHg to inorganic Hg and then eliminating Hg from plants as gaseous Hg°. MeHg concentrations in rice grains would increase by 2.4- to 4.7-fold without this pathway, which equates to intelligence quotient losses of 0.01-0.51 points per newborn in major rice-consuming countries, corresponding to annual economic losses of US$30.7-84.2 billion globally. This discovered pathway effectively removes Hg from human food webs, playing an important role in exposure mitigation and global Hg cycling.


Subject(s)
Mercury , Methylmercury Compounds , Oryza , Infant, Newborn , Humans , Mercury/metabolism , Oryza/metabolism , Food Chain , Methylmercury Compounds/metabolism , Demethylation
6.
Environ Sci Technol ; 57(42): 16053-16064, 2023 10 24.
Article in English | MEDLINE | ID: mdl-37824517

ABSTRACT

Rhizosphere microbiota are an important factor impacting plant uptake of pollutants. However, little is known about how microbial nitrogen (N) transformation in the rhizosphere affects the uptake and accumulation of antibiotics in plants. Here, we determined recruitment of N transformation functional bacteria upon ciprofloxacin (CIP) exposure, by comparing differences in assembly processes of both rhizospheric bacterial communities and N transformation between two choysum (Brassica parachinensis) varieties differing in CIP accumulation. The low accumulation variety (LAV) of CIP recruited more host bacteria (e.g., Nitrospiria and Nitrolancea) carrying nitrification genes (mainly nxrA) but fewer host bacteria carrying denitrification genes, especially narG, relative to the high accumulation variety (HAV) of CIP. The nxrA and narG abundance in the LAV rhizosphere were, respectively, 1.6-7.8 fold higher and 1.4-3.4 fold lower than those in the HAV rhizosphere. Considering that nitrate can decrease CIP uptake into choysum through competing for the proton motive force and energy, such specific bacteria recruitment in LAV favored the production and utilization of nitrate in its rhizosphere, thus limiting its CIP accumulation with 1.6-2.4 fold lower than the HAV. The findings give insight into the mechanism underlying low pollutant accumulation, filling the knowledge gap regarding the profound effects of rhizosphere microflora and N transformation processes on antibiotic accumulation in crops.


Subject(s)
Brassica , Ciprofloxacin , Rhizosphere , Nitrates , Nitrogen/analysis , Anti-Bacterial Agents , Bacteria/genetics , Plants , Soil , Soil Microbiology
7.
J Agric Food Chem ; 71(30): 11704-11715, 2023 Aug 02.
Article in English | MEDLINE | ID: mdl-37477475

ABSTRACT

Fluorotelomer alcohols (FTOHs), as precursors of perfluoroalkyl carboxylic acids, are difficult to analyze due to their high volatility and matrix interference. A method based on single-factor experiments and response surface methodology design was developed for simultaneous analysis of three common FTOHs in vegetables and soils, using single extraction, dispersive solid phase extraction cleanup, and gas chromatography-mass spectrometry in negative chemical ionization. The method improved the extraction efficiency up to ∼40 folds and showed a commendable linearity range (1-100 ng/mL, R2 > 0.991), low limit of detection (0.025-0.897 ng/g, dry weight (dw)), and high accuracy and precision (83 ± 7.2-117 ± 6.0% recoveries at 2-20 ng/g fortification levels). It was successfully applied to determine the FTOHs in real vegetables and soils, demonstrating its feasibility for routine analysis. Concentrations of the FTOHs ranged from 3.5 to 37.9 ng/g (dw) and from 6.5 to 141.0 ng/g (dw), respectively, in the vegetables and soils collected nearby fluorochemical factories, which warrants further investigations on FTOH pollution and food safety concerns for which the developed method will be useful.


Subject(s)
Fluorocarbons , Vegetables , Soil , Fluorocarbons/analysis , Gas Chromatography-Mass Spectrometry/methods , Alcohols/chemistry
8.
Environ Sci Technol ; 57(46): 18317-18328, 2023 Nov 21.
Article in English | MEDLINE | ID: mdl-37186812

ABSTRACT

Machine learning (ML) models were developed for understanding the root uptake of per- and polyfluoroalkyl substances (PFASs) under complex PFAS-crop-soil interactions. Three hundred root concentration factor (RCF) data points and 26 features associated with PFAS structures, crop properties, soil properties, and cultivation conditions were used for the model development. The optimal ML model, obtained by stratified sampling, Bayesian optimization, and 5-fold cross-validation, was explained by permutation feature importance, individual conditional expectation plot, and 3D interaction plot. The results showed that soil organic carbon contents, pH, chemical logP, soil PFAS concentration, root protein contents, and exposure time greatly affected the root uptake of PFASs with 0.43, 0.25, 0.10, 0.05, 0.05, and 0.05 of relative importance, respectively. Furthermore, these factors presented the key threshold ranges in favor of the PFAS uptake. Carbon-chain length was identified as the critical molecular structure affecting root uptake of PFASs with 0.12 of relative importance, based on the extended connectivity fingerprints. A user-friendly model was established with symbolic regression for accurately predicting RCF values of the PFASs (including branched PFAS isomerides). The present study provides a novel approach for profound insight into the uptake of PFASs by crops under complex PFAS-crop-soil interactions, aiming to ensure food safety and human health.


Subject(s)
Fluorocarbons , Water Pollutants, Chemical , Humans , Soil/chemistry , Carbon , Bayes Theorem , Fluorocarbons/analysis , Machine Learning , Water Pollutants, Chemical/analysis
9.
J Hazard Mater ; 456: 131668, 2023 08 15.
Article in English | MEDLINE | ID: mdl-37224713

ABSTRACT

Aniline aerofloat (AAF) is a refractory organic pollutant in floatation wastewater. Little information is currently available on its biodegradation. In this study, a novel AAF-degrading strain named Burkholderia sp. WX-6 was isolated from mining sludge. The strain could degrade more than 80% of AAF at different initial concentrations (100-1000 mg/L) within 72 h. AAF degrading curves were fitted well with the four-parameter logistic model (R2 >0.97), with the degrading half-life ranging from 16.39 to 35.55 h. This strain harbors metabolic pathway for complete degradation of AAF and is resistant to salt, alkali, and heavy metals. Immobilization of the strain on biochar enhanced both tolerance to extreme conditions and AAF removal, with up to 88% of AAF removal rate in simulated wastewater under alkaline (pH 9.5) or heavy metal pollution condition. In addition, the biochar-immobilized bacteria removed 59.4% of COD in the wastewater containing AAF and mixed metal ions within 144 h, significantly (P < 0.05) higher than those by free bacteria (42.6%) and biochar (48.2%) only. This work is helpful to understand AAF biodegradation mechanism and provides viable references for developing practical biotreatment technique of mining wastewater.


Subject(s)
Charcoal , Wastewater , Biodegradation, Environmental , Aniline Compounds
10.
J Hazard Mater ; 449: 130994, 2023 05 05.
Article in English | MEDLINE | ID: mdl-36821898

ABSTRACT

Microplastics (MPs) usually coexist with heavy metals (HMs) in soil. MPs can influence HMs mobility and bioavailability, but the underlying mechanisms remain largely unexplored. Here, polyethylene and polypropylene MPs were selected to investigate their effects and mechanisms of sorption-desorption, bioaccessibility and bioavailability of cadmium (Cd) in paddy soil. Batch experiments indicated that MPs significantly reduced the Cd sorption in soil (p < 0.05). Accordingly, soil with the MPs had lower boundary diffusion constant of Cd (C1= 0.847∼1.020) and the Freundlich sorption constant (KF = 0.444-0.616) than that without the MPs (C1 = 0.894∼1.035, KF = 0.500-0.655). X-ray diffraction, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy analyses suggested that the MPs reduced Cd chemisorption, by covering the soil active sites and thus blocking complexation of Cd with active oxygen sites and interrupting the formation of CdCO3 and Cd3P2 precipitates. Such effects of MPs enhanced about 1.2-1.5 times of Cd bioaccessibility and bioavailability in soil. Almost the same effects but different mechanisms of polyethylene and polypropylene MPs on Cd sorption in the soil indicated the complexity and pervasiveness of their effects. The findings provide new insights into impacts of MPs on the fate and risk of HMs in agricultural soil.


Subject(s)
Metals, Heavy , Soil Pollutants , Microplastics/chemistry , Cadmium/chemistry , Plastics/chemistry , Soil , Polyethylene/chemistry , Polypropylenes , Biological Availability , Adsorption , Soil Pollutants/analysis
11.
Sci Total Environ ; 864: 161013, 2023 Mar 15.
Article in English | MEDLINE | ID: mdl-36549521

ABSTRACT

Phthalates (PAEs) are ubiquitous in soils and food products and thus pose a high risk to human health. Herein, genome mining revealed a great diversity of bacteria with PAEs-degrading potential. Mining of the genome of Raoultella ornithinolytica XF201, a novel strain isolated from Dongxiang wild rice rhizosphere, revealed the presence of two silenced tandem genes pcdGH (encoding protocatechuate 3,4-dioxygenase, 3,4-PCD), key aromatic ring-cleaving genes in PAEs biodegradation. Ribosome engineering was successfully utilized to activate the expression of pcdGH genes to produce 3,4-PCD in the mutant XF201-G2U5. The mutant XF201-G2U5 showed high 3,4-PCD activity and could remove 94.5 % of di-n butyl phthalate (DBP) in 72 h. The degradation kinetics obeyed the first-order kinetic model. Strain XF201-G2U5 could also degrade the other PAEs and the main intermediate metabolites, ultimately leading to tricarboxylic acid cycle. Therefore, this strategy facilitates novel bacterial resources discovery for bioremediation of PAEs and other emerging contaminants.


Subject(s)
Diethylhexyl Phthalate , Phthalic Acids , Humans , Biodegradation, Environmental , Esters/metabolism , Phthalic Acids/metabolism , Dibutyl Phthalate/metabolism
12.
Chemosphere ; 310: 136770, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36228724

ABSTRACT

Huge volumes of wastewater containing organic flotation reagents such as xanthates have been released into the environment via mining activities, greatly threatening the eco-environment safety. A simple and fast method is urgently needed for accurate analysis of various xanthates in mining and environmental water. Here, a robust method is realized for simultaneous determination of three trace xanthates (i.e., potassium ethyl xanthate, potassium butyl xanthate, and potassium isopropyl xanthate) in environmental water samples, including eutrophic water and flotation wastewater using solid phase extraction (SPE) and HPLC-MS/MS. HPLC-MS/MS parameters, SPE cartridges and eluting solvents, pH values, and SPE procedures were optimized. The new method had an excellent linearity in the range of 1-1000 µg/L (R2 ≥ 0.998), low limits of detection (0.02-0.68 µg/L), and satisfactory accuracy and precision (72.9%-107.6% of average recoveries and <5% of relative standard deviations at 1, 10, 50, and 500 µg/L of xanthates). This is a first method developed for determination of trace xanthates in water samples. It was successfully applied to determine the target analytes in outdated flotation wastewater and river water samples, warranting the occurrence of trace xanthates (0.13-16.9 µg/L) in water and necessity of systematic investigation on environmental fate and risk of xanthates.


Subject(s)
Insecticides , Water Pollutants, Chemical , Tandem Mass Spectrometry/methods , Wastewater/chemistry , Water/chemistry , Water Pollutants, Chemical/analysis , Solid Phase Extraction/methods , Chromatography, Liquid/methods , Chromatography, High Pressure Liquid/methods , Insecticides/analysis , Potassium
13.
Eco Environ Health ; 2(4): 278-286, 2023 Dec.
Article in English | MEDLINE | ID: mdl-38435362

ABSTRACT

Perfluoroalkyl acids (PFAAs) are considered forever chemicals, gaining increasing attention for their hazardous impacts. However, the ecological effects of PFAAs remain unclear. Environmental DNA (eDNA), as the environmental gene pool, is often collected for evaluating the ecotoxicological effects of pollutants. In this study, we found that all PFAAs investigated, including perfluorohexanoic acid, perfluorooctanoic acid, perfluorononanoic acid, and perfluorooctane sulfonate, even at low concentrations (0.02 and 0.05 mg/L), expedited the enzymatic degradation of DNA in a nonlinear dose-effect relationship, with DNA degradation fragment sizes being lower than 1,000 bp and 200 bp after 15 and 30 min of degradation, respectively. This phenomenon was attributed to the binding interaction between PFAAs and AT bases in DNA via groove binding. van der Waals force (especially dispersion force) and hydrogen bonding are the main binding forces. DNA binding with PFAAs led to decreased base stacking and right-handed helicity, resulting in loose DNA structure exposing more digestion sites for degrading enzymes, and accelerating the enzymatic degradation of DNA. The global ecological risk evaluation results indicated that PFAA contamination could cause medium and high molecular ecological risk in 497 samples from 11 contamination-hot countries (such as the USA, Canada, and China). The findings of this study show new insights into the influence of PFAAs on the environmental fates of biomacromolecules and reveal the hidden molecular ecological effects of PFAAs in the environment.

14.
Bioresour Technol ; 360: 127523, 2022 Sep.
Article in English | MEDLINE | ID: mdl-35772714

ABSTRACT

The succession of fungal community and effects of heavy metals on fungi during industrial-scale hyperthermophilic composting of municipal sludge remain unclear. Results showed hyperthermophilic composting enhanced decomposition and humification of municipal sludge in the short terms, while heavy metal concentrations and speciation had no significant change with high copper and zinc levels (101-122 and 292-337 mg/kg, respectively) in compost samples. The fungal community and its ecological assembly displayed dynamic change during hyperthermophilic composting. Some thermophilic-resistant fungi, such as phylum Ascomycota and genera Candida, Aspergillus, Thermomyces and Petriella dominated in hyperthermophilic phase. Heavy metals served important effects on fungal community structure and functions during composting. Some fungal drivers (e.g., Thermomyces, Petriella and Schizophyllum) and keystone fungi (e.g., Candida and Pichia) might be thermophilic- and heavy metal-resistant fungi which played important roles in decomposition and humification of municipal sludge. This study reveals fungal community accelerating humification and its influencing factors during composting.


Subject(s)
Composting , Metals, Heavy , Mycobiome , Archaea , Fungi , Sewage/chemistry , Soil
15.
Water Res ; 221: 118778, 2022 Aug 01.
Article in English | MEDLINE | ID: mdl-35752093

ABSTRACT

The electrochemical oxidation method is a promising technology for the degradation of perfluorooctane sulfonate (PFOS). However, the elimination processes of PFOS are still unknown, including the electron transfer pathway, key reactive sites, and degradation mechanism. Here, we fabricated diatomite and cerium (Ce) co-modified Sb2O3 (D-Ce/Sb2O3) anode to realize efficient degradation of PFOS via peroxymonosulfate (PMS) activation. The transferred electron and the generated hydroxyl radical (•OH) can high-effectively decompose PFOS. The electron can be rapidly transferred from the highest occupied molecular orbital of the PFOS to the lowest unoccupied molecular orbital of the PMS via the D-Ce/Sb2O3 driven by a potential energy difference under electrochemical process. The active site of Ce-O in the D-Ce/Sb2O3 can greatly reduce the migration distance of the electron and the •OH, and thus improving the catalytic activity for degrading various organic micropollutants with high stability. In addition, the electrochemical process shows strong resistance and tolerance to the changing pH, inorganic ions, and organic matter. This study offers insights into the electron transfer pathway and PMS activation mechanism in PFOS removal via electrochemical oxidation, paving the way for its potential application in water purification.


Subject(s)
Alkanesulfonic Acids , Water Pollutants, Chemical , Catalytic Domain , Fluorocarbons , Peroxides/chemistry , Water , Water Pollutants, Chemical/chemistry
16.
Water Res ; 215: 118259, 2022 May 15.
Article in English | MEDLINE | ID: mdl-35294910

ABSTRACT

Polyfluoroalkyl and perfluoroalkyl chemicals (PFCs) widely used in lubricants, surfactant, textiles, paper coatings, cosmetics, and fire-fighting foams can release a large deal of organics contaminants into wastewater and pose great risks to the health of humans and eco-environments. Although advanced oxidation processes can effectively deconstruct various organic contaminants via reactive radicals, the stable structure of PFCs makes it difficult to be degraded. Here, we confirm that electrochemical oxidation process coupled with peroxymonosulfate (PMS) reaction can efficiently destroy stable structure of PFCs via electron transfer and meanwhile completely degrade PFCs via generated active radicals. We further studies via capturing and scavenging radicals, and DFT calculations find that electron hydroxyl radials play a dominant role in degrading PFCs. Based on the calculations of adsorption energy and molecular orbital energy we further demonstrate that many active sites on the surface of Ti4O7 (1 0 4) plane can rapidly take part in electrochemical reaction for generating radials and removing organic contaminants. These results give a promising insight towards high-effective and deep degradation of PFCs via electrochemical reaction coupled with advanced oxidation processes, as well as providing guidance and technical support for the remove of multiple organic contaminants.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Electron Transport , Electrons , Humans
17.
Water Res ; 207: 117849, 2021 Dec 01.
Article in English | MEDLINE | ID: mdl-34785408

ABSTRACT

Perfluorooctane sulfonate (PFOS), normally present in groundwater and surface water, is an emerging environmental contaminants, but is extremely difficult to be degraded due to high energy of the C-F bond. Here, an electrocoagulation (EC) technique coupled with peroxymonosulfate (PMS) activation was used to deeply degrade PFOS. Results showed that approximately 100% PFOS was removed from the solution in the monopolar serial (MS) mode within 60 min and achieved a high kinetic rate of 0.074 min-1, which was significantly higher than those of reported studies (Table S3). Energy consumption (2.06 kWh/kg) in the MS mode was significantly lower than that of Al (52.30 kWh/kg) and Zn (213.50 kWh/kg) electrodes, which further confirmed the potential application prospects of EC technique. The quenching experiments, electron spin response (ESR) analysis, and DFT calculations can verify that ·OH was the main radical from the reaction of Fe2+-OH reaction site with PMS. In addition, results from fluorine balance and TOC removal also indicated the complete mineralization and degradation of PFOS in the EC process. Quantum chemical calculations can confirm the PFOS degradation mechanism and key active sites for direct electron transfer and radical attack. After five cycle operations of PFOS degradation, the EC process was still effective in degrading PFOS with a removal efficiency above 98%. Thus, this work provided a novel alternative for the high-effective treatment of PFOS from contaminated environmental water bodies.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Water Pollutants, Chemical , Catalytic Domain , Electrocoagulation , Fluorocarbons/analysis , Peroxides , Water Pollutants, Chemical/analysis
18.
J Agric Food Chem ; 69(40): 11825-11834, 2021 Oct 13.
Article in English | MEDLINE | ID: mdl-34582220

ABSTRACT

Microcystins (MCs) are hepatotoxic heptapeptides identified in cyanobacterial bloom-impacted waters and soils. However, their environmental fate in soils is poorly understood, preventing reliable site assessment. This study aims to clarify the variant-specific adsorption, desorption, and dissipation of MC-LR and MC-RR in agricultural soils. Results revealed that their adsorption isotherms followed the Freundlich model (R2 ≥ 0.96), exhibiting a higher nonlinear trend and lower adsorption capacity for MC-LR than for MC-RR. The soils had low desorption rates of 8.14-21.06% and 3.06-34.04%, respectively, following a 24 h desorption cycle. Pairwise comparison indicated that soil pH and clay played key roles in MC-LR adsorption and desorption, while organic matter and cation exchange capacity played key roles in those of MC-RR. MC-LR dissipation half-lives in soils were 27.18-42.52 days, compared with 35.19-43.87 days for MC-RR. Specifically, an appreciable decrease in MC concentration in sterile soils suggested the significant role of abiotic degradation. This study demonstrates that the minor structural changes in MCs might have major effects on their environmental fates in agricultural soil and indicates that the toxic effects of MCs should be of high concern due to high adsorption, low desorption, and slow dissipation.


Subject(s)
Cyanobacteria , Microcystins , Adsorption , Agriculture , Soil
19.
Bioresour Technol ; 328: 124847, 2021 May.
Article in English | MEDLINE | ID: mdl-33609883

ABSTRACT

Sewage sludge contains various classes of organic pollutants, limiting its land application. Sludge composting can effectively remove some organic pollutants. This review summarizesrecent researches on concentration changes and dissipation of different organic pollutants including persistent organic pollutants during sludge composting, and discusses their dissipation pathways and the current understanding on dissipation mechanism. Some organic pollutants like PAHs and phthalates were removed mainly through biodegradation or mineralization, and their dissipation percentages were higher than those of PCDD/Fs and PCBs. Nevertheless, some recalcitrant organic pollutants could be sequestrated in organic fractions of sludge mixtures, and their levels and ARG abundance even increased after sludge composting in some studies, posing potential risks for land application. This review demonstrated that microbial community and their corresponding degradation for organic pollutants were influenced by different pollutants, bulking agents, composting methods and processes. Further research perspectives on removing organic pollutants during sludge composting were highlighted.


Subject(s)
Composting , Environmental Pollutants , Polychlorinated Dibenzodioxins , Dibenzofurans , Sewage , Soil
20.
Sci Total Environ ; 763: 143028, 2021 Apr 01.
Article in English | MEDLINE | ID: mdl-33129529

ABSTRACT

The growing incidence of microcystins (MCs) in the environment has become an issue of global concern for the high ecological and human health risks. Herein, a comparative adsorption of three MCs (MC-LR, MC-YR and MC-RR) by spent mushroom substrate (SMS)-derived biochars from contrasting pyrolytic conditions (temperature: 600/300 °C; and gas steam: CO2/N2) was surveyed to better understand the mechanisms and factors affecting the adsorption performance. For biochar preparation, 600 °C and CO2 led to greater levels of aromaticity, ash, SBET, and porosity, while 300 °C and N2 created more surface functional groups. The adsorption of MCs by biochars was a pH-dependent and endothermic physisorption process, following the pseudo-second-order kinetics (R2 = 0.99) and linear isotherm model (R2 > 0.88). The distribution coefficients Kd (0.98-19.2 L/kg) varied greatly among MCs (MC-YR > MC-RR > MC-LR) and biochars (BC600 > BN600 > BC300 > BN300), which depends on the combined effects of hydrophobicity, electrostatic attraction, H-bonding, cation bridging, and the amounts of adsorption sites on biochars. Higher ash, SBET, and total pore volume of BC600 facilitated the adsorption capacity for MCs relative to other biochars. Furthermore, the co-adsorption efficacy for MCs (Kd = 1.09-8.86 L/kg) was far below those for the single adsorption, indicating strong conflicts among competing MCs. This study sheds light on the roles of pyrolytic temperature and gas steam in biochar properties, and elucidates the mechanisms and factors affecting the adsorption performance of different MCs, which lays a foundation for MCs removal from water.


Subject(s)
Charcoal , Microcystins , Adsorption , Humans , Pyrolysis
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