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1.
J Environ Sci (China) ; 90: 87-97, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32081344

RESUMO

A novel insight on the role of interactions between target pollutants and the catalyst in the copper-containing layered double oxide (LDO)-catalyzed persulfate (PS) system was elucidated in the present study. 4-Chlorophenol (4-CP), as a representative benzene derivative with a hydroxyl group, was completely removed within 5 min, which was much faster than the reaction of monochlorobenzene (MCB) without a hydroxyl group, with the degradation efficiency of 31.7% in 240 min. Through the use of radical quenching and surface inhibition experiments, it could be concluded that the interaction between 4-CP and CuMgFe-LDO, rather than free radicals, played a key role in the decomposition of 4-CP, while only the free radicals participated in the MCB degradation process. According to electron paramagnetic resonance and X-ray photoelectron spectroscopy data, the formation of a Cu(II)-complex between phenolic hydroxyl groups and surface Cu(II) was primarily responsible for the degradation of phenolic compounds, in which PS accepted one electron from the complex and generated sulfate radicals and chelated radical cations. The chelated radical cations transferred one electron to Cu(II) followed by Cu(I) generation and pollutant degradation successively.


Assuntos
Derivados de Benzeno , Poluentes Ambientais , Catálise , Radical Hidroxila , Oxirredução , Óxidos , Sulfatos
2.
J Environ Manage ; 245: 238-244, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-31154170

RESUMO

To elucidate the effect of structure and property of biochar on the structure-activity relationship among the composites of biochar supported Pd/Fe and 1,2,4-trichlorobenzene (1,2,4-TCB) and its dechlorination products, biochar supported Pd/Fe nanoparticles with different mass ratios were investigated for the enhanced removal of 1,2,4-TCB (52 µmol/L) and its dechlorination products. 1,2,4-TCB was removed through the electrochemical dechlorination by Pd/Fe and adsorption by biochar simultaneously. As the mass ratio of CS700 to Pd/Fe was 0.1:1, biochar within the Pd/Fe-CS7000.1 system played a significant role in the adsorption of 1,2,4-TCB. However, there is little adsorption to biochar for dechlorination products due to strong competition by 1,2,4-TCB. As the mass ratio of CS700 to Pd/Fe was increased to 5:1, 1,2,4-TCB was completely removed from the solution by the composites within 0.5 h. The dechlorination products (1,2-DCB, MCB, benzene and trace 1,3-DCB) were completely sequestered on solid phase but absent in aqueous solution. However, the excessive biochar increased the inaccessibility of 1,2,4-TCB or decreased the reactive sites of Pd/Fe leading to the less dechlorination of 1,2,4-TCB. The alkaline biochar did not influence the chemical reactivity of Pd/Fe in the composites and buffered the acid and alkaline solutions with pH being maintained at neutral conditions under initial pH ranging from 3.07 to 10.03. The highly hydrophobicity of biochar could maintain the affinity of the composite for the chlorinated compounds even if the concentration of 1,2,4-TCB was up to 80.9% of its aqueous solubility. This study provides efficient synergistic removal support for the treatment of TCB affected groundwater.


Assuntos
Clorobenzenos , Ferro , Carvão Vegetal
3.
Int J Mol Sci ; 16(7): 14464-76, 2015 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-26121300

RESUMO

The objectives of this study were to evaluate the binding behavior of Cu(II) and Eu(III) with water extractable organic matter (WEOM) in soil, and assess the competitive effect of the cations. Excitation-emission matrix (EEM) fluorescence spectrometry was used in combination with parallel factor analysis (PARAFAC) to obtain four WEOM components: fulvic-like, humic-like, microbial degraded humic-like, and protein-like substances. Fluorescence titration experiments were performed to obtain the binding parameters of PARAFAC-derived components with Cu(II) and Eu(III). The conditional complexation stability constants (logKM) of Cu(II) with the four components ranged from 5.49 to 5.94, and the Eu(III) logKM values were between 5.26 to 5.81. The component-specific binding parameters obtained from competitive binding experiments revealed that Cu(II) and Eu(III) competed for the same binding sites on the WEOM components. These results would help understand the molecular binding mechanisms of Cu(II) and Eu(III) with WEOM in soil environment.


Assuntos
Cobre/química , Európio/química , Substâncias Húmicas , Absorção de Radiação , Análise Espectral , Água/química
4.
Chemosphere ; 350: 141059, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38163469

RESUMO

Phthalate acid esters (PAEs) are frequently detected in the global environment and can cause potential health hazards. In this study, quantitative exposure risk assessment was undertaken to derive soil generic assessment criteria (GAC) for six representative PAEs under the agricultural land use in the evaluated Chinese regions, which coupled multi-media transport and human exposure models based on multiple exposure pathways including vegetables consumption, dermal absorption, ingestion of soil and dust, and the exposure from non-soil sources. It is identified that the PAEs in agricultural soil are dominated by DEHP and DnBP representing 72-96% of the total PAEs. The GAC for BBP and DEHP, calculated on the basis of region-specific exposure parameters and soil properties in various locations, are stringent, signifying greater potential health risks from exposure to them, warranting more rigorous contamination management. The proposed soil GAC for plastic debris are 100, 107, 73 and 88 mg kg-1 for Heilongjiang Province, Beijing City, Jiangsu and Guangdong Provinces respectively. Additionally, the potential risks of 1.68 × 10-6 and 7 × 10-6 are identified for BBP and DEHP in Guangdong Province as indicated by the exceedance of target risk level of 1 × 10-6, with the consumption of vegetables being the dominant contributor to the total estimated PAEs exposure. Overall, this methodology based on the coupled contaminant transport and exposure models incorporating region-specific data provides a technical framework to derive science-based soil GAC for representative PAEs for maintaining and assessing soil quality and food safety under the agricultural land use.


Assuntos
Dietilexilftalato , Ácidos Ftálicos , Poluentes do Solo , Humanos , Poluentes do Solo/análise , Ésteres/análise , Ácidos Ftálicos/análise , Solo , Verduras , Medição de Risco , China , Dibutilftalato/análise
5.
J Hazard Mater ; 470: 134221, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38615651

RESUMO

Constructed wetlands (CWs) are a promising approach for treating acid mine drainage (AMD). However, the extreme acidity and high loads of heavy metals in AMD can easily lead to the collapse of CWs without proper pre-treatment. Therefore, it is considered essential to maintain efficient and stable performance for AMD treatment in CWs. In this study, pre-prepared attapulgite-soda residue (ASR) composites were used to improve the substrate of CWs. Compared with CWs filled with gravel (CWs-G), the removal efficiencies of sulfate and Fe, Mn, Cu, Zn Cd and Pb in CWs filled with ASR composites (CWs-ASR) were increased by 30% and 10-70%, respectively. These metals were mainly retained in the substrate in stable forms, such as carbonate-, Fe/Mn (oxide)hydroxide-, and sulfide-bound forms. Additionally, higher levels of photosynthetic pigments and antioxidant enzyme activities in plants, along with a richer microbial community, were observed in CWs-ASR than in CWs-G. The application of ASR composites alleviated the adverse effects of AMD stresses on wetland plants and microorganisms. In return, the increased bacteria abundance, particularly SRB genera (e.g., Thermodesulfovibrionia and Desulfobacca), promoted the formation of metal sulfides, enabling the saturated ASR adsorbed with metals to regenerate and continuously capture heavy metals. The synergistic adsorption of ASR composites and microbial sulfate reduction maintained the stable and efficient operation of CWs. This study contributes to the resource utilization of industrial alkaline by-products and promotes the breakthrough of new techniques for low-cost and passive treatment systems such as CWs.


Assuntos
Compostos de Magnésio , Metais Pesados , Mineração , Compostos de Silício , Sulfatos , Poluentes Químicos da Água , Áreas Alagadas , Sulfatos/química , Metais Pesados/química , Adsorção , Poluentes Químicos da Água/química , Poluentes Químicos da Água/metabolismo , Compostos de Silício/química , Compostos de Magnésio/química , Ácidos/química , Oxirredução , Biodegradação Ambiental , Concentração de Íons de Hidrogênio
6.
Water Res ; 258: 121822, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38796915

RESUMO

This study investigated the co-transport behaviors of nano zero-valent iron (nZVI) and Cd(II) in the presence of soil nanoparticles (SNPs) under various SNPs/nZVI mass ratios. It was illustrated that the mobility of colloidal Cd(II) was highly dependent on the nZVI-SNPs heteroaggregation behavior. In the case of 40 mg/L nZVI with SNPs/nZVI mass ratios > 1, the formation of stable SNPs-nZVI heteroaggregates with hydrodynamic diameters (Dh) < 500 nm facilitated the nZVI and colloidal Cd(II) transport at their effluent mass recoveries of 34.76-37.82 % and 9.81-17.17 %, respectively. However, in the case of 100 mg/L nZVI with SNPs/nZVI mass ratios of 0.4-2, the interception of nZVI-SNPs heteroaggregates with Dh > 1500 nm by quartz sands led to almost complete retention of nZVI and colloidal Cd(II) in the columns. Combined with analytical results of zeta potentials and XRD spectrum, it was revealed that the Cd(II) ions could accelerate nZVI corrosion. The positively charged Fe3O4 and γ-FeOOH on corroded nZVI surface could facilitate the heteroaggregation of nZVI-SNPs by the patch-charge attraction, which further reduced the environmental risk of colloidal Cd(II) transport. These findings revealed the important effects of heteroaggregation between nZVI and SNPs on the transport risk of Cd(II) in groundwater.


Assuntos
Cádmio , Ferro , Cádmio/química , Ferro/química , Dióxido de Silício/química , Poluentes Químicos da Água/química , Solo/química , Nanopartículas Metálicas/química
7.
Chemosphere ; 321: 138111, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36780998

RESUMO

Iron sulfides have attracted growing concern in heterogeneous Fenton reaction. However, the structure of iron sulfides is different from that of iron oxides and how the structures affect the activation property of hydrogen peroxide (H2O2) remains unclear. This study investigated benzene removal through the activation of H2O2 by the synthesized magnetite (Fe3O4) and greigite (Fe3S4). The structures of Fe3O4 and Fe3S4 were characterized by XRD and EPR, the electron transfer properties of Fe3O4 and Fe3S4 were analyzed by electrochemical workstation, XPS and DFT. It is revealed that the effective benzene removal rate of 88.86% in the Fe3S4/H2O2 was achieved, which compared to 15.58% obtainable from the Fe3O4/H2O2, with the apparent rate constant in the Fe3S4/H2O2 being approximately 65 times over that in the Fe3O4/H2O2. The better H2O2 activation by Fe3S4 was attributed to the significant roles of S (-II) and S vacancies in regulating the dissolution of ferrous iron ions, thus generating abundant free •OH radical. In addition, surface bounded ferrous iron of Fe3S4 could transfer more electrons to H2O2 and O2 to generate more surface bounded •OH and •O2-. This study revealed the combined action of dissolved and surface bounded ferrous iron of greigite on H2O2 activation, and provides an efficient heterogeneous H2O2 activator for the remediation of organic contaminants in groundwater.


Assuntos
Benzeno , Peróxido de Hidrogênio , Peróxido de Hidrogênio/química , Ferro/química , Sulfetos/química , Oxirredução
8.
Environ Pollut ; 335: 122368, 2023 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-37586685

RESUMO

Perfluoroalkyl acid substances (PFAAs), such as perfluorobutanoic acid (PFBA), perfluorobutanoic sulfonic acid (PFBS), perfluorooctane acid (PFOA) and perfluoroooctane sulfonic acid (PFOS) are frequently detected in the global environment and can cause potential health hazards even at low levels. In this study, quantitative human health risk assessment was undertaken to derive soil generic assessment criteria (GAC) for four PFAAs under the agricultural land scenario in the evaluated Chinese regions, which considered multiple exposure pathways including vegetables consumption, dermal absorption, ingestion of soil and dust, and exposure from non-soil sources. It is showed that the calculated GAC for four PFAAs in Guangdong and Shandong Provinces were less stringent than those in Zhejiang and Jiangsu Provinces, and Shanghai City, owing to the low exposure from non-soil sources in former two provinces. In addition, GAC of PFOS were the most stringent in the range of 0.28-0.50 µg kg-1 in the studied regions, followed by PFOA (1.36-2.20 µg kg-1), PFBA (42.59-68.03 µg kg-1) and PFBS (474.59-749.60 µg kg-1), mainly attributable to significantly more stringent toxicological values of PFOA and PFOS. Correspondingly, the potential health hazards exist for PFOA in the studied regions except Guangdong Province, and PFOS only in Zhejiang and Jiangsu Provinces as indicated by the hazard quotients ranging from 1.04 to 19.49, but no health hazards are identified for PFBA and PFBS. The dominant exposure pathway was found to be consumption of vegetables and attached soil for PFBA and PFBS, contributing to more than 93% of the total exposure, compared to 49.91-76.69% for PFOA and PFOS due to significant exposure from non-soil sources levels. Overall, this study provides a technical reference on how to derive scientifically justifiable soil GAC for representative PFAAs for maintaining and assessing soil quality and food safety internationally under the agricultural land use.


Assuntos
Ácidos Alcanossulfônicos , Fluorocarbonos , Ácidos Alcanossulfônicos/análise , Caprilatos/análise , China , Monitoramento Ambiental , Fluorocarbonos/análise , Medição de Risco , Solo , Ácidos Sulfônicos , Verduras
9.
Sci Total Environ ; 871: 162015, 2023 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-36746284

RESUMO

The agricultural soils in China are suffered from serious polychlorinated biphenyls (PCBs) contamination, however, the valid management standards for farmland are absent to efficiently control the health risks of PCBs exposure. This study analyzed the contamination characteristics and main composition of PCBs in agricultural soils of the southeastern China from the published literature over the past 20 years, and derived the regional generic assessment criteria (GAC) using an exposure modelling approach for individual and total PCBs (∑PCBs) via multiple exposure pathways such as ingestion of soil and dust, consumption of vegetables, dermal contact with soil and dust, ingestion of soil attached to vegetables, and inhalation of soil vapour and soil-derived dust outdoors under the agricultural land scenario. It is identified that the averaged ∑PCBs concentration of 80.03 ng g-1 under the 95 % lower confidence limit with an unacceptable health risk of 4.8 × 10-6 has significantly exceeded the integrated generic assessment criteria (expressed as GACint) of 16.5 ng g-1. Accordingly, the exposure pathways from the consumption of agricultural produces and indirect ingestion of soil attached to vegetables contributed up to 62 %-88 % of the total exposure, followed by 11 %-33 % of the soil ingestion and 2 %-6 % of dermal contact. The derived GACint for ∑PCBs is extremely valuable to effectively assess and manage the PCBs contamination in agricultural soils of China.


Assuntos
Bifenilos Policlorados , Poluentes do Solo , Bifenilos Policlorados/análise , Solo , Monitoramento Ambiental , Poluentes do Solo/análise , China , Verduras , Poeira
10.
J Hazard Mater ; 459: 132325, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37598515

RESUMO

This study discovered that nanosized zero valent magnesium (nZVMg) could be formed during the electrochemical corrosion of microsized ZVMg (mZVMg) in aqueous solution. It is observed that the nZVMg particle sizes were less than 50 nm with the specific surface area of 54.63 m2/g after it was corroded for 96 h (ZVMg96) at the expense of losing about 60 wt% Mg0. However, the XPS characterization indicated the thickness of Mg(OH)2 layer over ZVMg96 being less than 5 nm, accompanied by the faster electron transfer rate but slower corrosion rate than mZVMg. Most importantly, the removal efficiency of 82 % under high-level trichloroethylene (TCE) at 100 mg/L was achieved by ZVMg96 within one hour relative to 48 % by mZVMg. The rate constant normalized by surface area was 3.11 × 10-2 L/m2/h by ZVMg96 due to the high surface energy of nanoparticles. The degradation products were dependent on the initial TCE concentrations, with environmentally friendly and biodegradable degradation products being generated via hydrodechlorination, hydrogenation and polymerization pathways according to the density functional theory calculations. ZVMg corroded for 14 days illustrated a long-term chemical stability and excellent degradation performance, demonstrating significant application potential in remediating the TCE plumes in groundwater.

11.
Environ Pollut ; 336: 122424, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37604391

RESUMO

Sulfidated zero-valent iron (ZVI) and biochar-supported ZVI have received increasing attention for their potential to dechlorinate trichloroethylene. However, minimal data are available regarding the combined effect of sulfur and biochar ZVI on trichloroethylene byproducts. The primary aim of the current study is to determine whether sulfur- and biochar-modified ZVI (ZVI-BC-S) enhances the removal of cis-1,2-dichloroethene (cDCE) and vinyl chloride (VC) from groundwater. Results show that biochar and sulfur facilitated the milling of ZVI-BC-S into micro- and nanoscale particles and increased FeS formation. Moreover, the rates of cDCE and VC removal by ZVI-S increased by 30.1% and 30.2%, respectively, compared to those obtained with ZVI, owing to enhanced dechlorination via ß-elimination by sulfur. Meanwhile, treatment with ZVI-BC-S harnessed the benefits of biochar and sulfur to enhance the cDCE and VC removal rates by 62.0% and 67.7%, respectively. Mechanistically, biochar enhanced the corrosion of ZVI-S to increase FeS production and enhance the electron transfer, ß-elimination, and hydrogenolysis involved in cDCE and VC dechlorination. The effectiveness of ZVI-BC-S was confirmed in a field demonstration, during which cDCE and VC concentrations significantly decreased within 10 days following injection. The findings of this study can help inform the rational design of ZVI for in-situ remediation of chlorinated hydrocarbons in groundwater.

12.
Sci Total Environ ; 889: 164243, 2023 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-37201809

RESUMO

The simultaneous removal of hexavalent chromium (Cr(VI)) and Trichloroethylene (TCE) is facing great challenges, and the influences of the biochar on their removal by nanoscale zero-valent iron (nZVI) are poorly understood and seldom addressed in the literature. The rice straw pyrolysis at 700 °C (RS700) and their supported nZVI composites were investigated on the removal of Cr(VI) and TCE by batch experiments. The surface area and chromium bonding state of biochar supported nZVI with and without Cr(VI)-TCE loading were analyzed by Brunauer-Emmett-Teller analysis and X-ray photoelectron spectroscopy. In single pollutants system, the highest removal amounts of Cr(VI) and TCE were observed in RS700-HF-nZVI (76.36 mg/g) and RS700-HF (32.32 mg/g), respectively. The Cr(VI) removal was attributed to the reduction by Fe(II) with the adsorption by biochar primarily controlling the TCE removal. The mutual inhibition was revealed in simultaneous removal of Cr(VI) and TCE, in which the reduction of Cr(VI) was decreased due to the adsorption of Fe(II) by biochar, while the TCE adsorption was primarily inhibited owing to the blockage of surface pores of biochar supported nZVI by chromium­iron oxides. Therefore, biochar supported nZVI could be potentially used for the combined contaminated groundwater remediation, but the mutual inhibition should be evaluated.


Assuntos
Tricloroetileno , Poluentes Químicos da Água , Ferro/química , Poluentes Químicos da Água/análise , Cromo/química , Carvão Vegetal/química , Adsorção , Compostos Ferrosos
13.
Nanomaterials (Basel) ; 13(9)2023 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-37177062

RESUMO

In this study, efficient remediation of p-chloroaniline (PCA)-contaminated soil by activated persulfate (PS) using nanosized zero-valent iron/biochar (B-nZVI/BC) through the ball milling method was conducted. Under the conditions of 4.8 g kg-1 B-nZVI/BC and 42.0 mmol L-1 PS with pH 7.49, the concentration of PCA in soil was dramatically decreased from 3.64 mg kg-1 to 1.33 mg kg-1, which was much lower than the remediation target value of 1.96 mg kg-1. Further increasing B-nZVI/BC dosage and PS concentration to 14.4 g kg-1 and 126.0 mmol L-1, the concentration of PCA was as low as 0.15 mg kg-1, corresponding to a degradation efficiency of 95.9%. Electron paramagnetic resonance (EPR) signals indicated SO4•-, •OH, and O2•- radicals were generated and accounted for PCA degradation with the effect of low-valence iron and through the electron transfer process of the sp2 hybridized carbon structure of biochar. 1-chlorobutane and glycine were formed and subsequently decomposed into butanol, butyric acid, ethylene glycol, and glycolic acid, and the degradation pathway of PCA in the B-nZVI/BC-PS system was proposed accordingly. The findings provide a significant implication for cost-effective and environmentally friendly remediation of PCA-contaminated soil using a facile ball milling preparation of B-nZVI/BC and PS.

14.
Sci Total Environ ; 903: 166601, 2023 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-37634714

RESUMO

Acid mine drainage (AMD) rich in arsenic (As) and antimony (Sb) is considered as a significant environmental challenge internationally. However, simultaneous removal of As and Sb from AMD is still inadequately studied. In this study, a highly effective and simple approach was proposed for mitigating As and Sb-rich AMD, which involves in-situ formation of layered double hydroxides (LDHs). Following the treatment, the residual concentrations of iron (Fe), magnesium (Mg), sulfate, As and Sb in field AMD were decreased from their initial concentrations of 1690, 1524, 2055, 7.8 and 10.6 mg L-1, respectively, to 1.3, 12.4, 623, 0.006 and 0.004 mg L-1, respectively. Chemical formula of the resulting As and Sb-loaded LDHs can be identified as Mg4.226Fe2.024OH2SO4AsSb0.006∙mH2O. The dissolution rates of metal(loid)s in As and Sb-loaded LDH were lower than 1% under strongly acidic and alkaline environments. In presence of the mixed adsorbates, the As immobilization capacity by LDHs was significantly decreased, with an apparent intervention from Sb. However, As did not have a significant effect on the immobilization of Sb by LDH. As was immobilized by LDHs through anion exchange and complexation with -OH groups, while Sb was captured by anion exchange and complexation with [Formula: see text] . Density functional theory (DFT) calculations further proved the above conclusions. This novel approach is effective and can be applied for in-situ AMD treatment from abandoned mines.

15.
J Hazard Mater ; 445: 130588, 2023 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-37055992

RESUMO

CoFe2O4/hydrochar composites (FeCo@HC) were synthesized via a facile one-step hydrothermal method and utilized to activate peroxymonosulfate (PMS) for simultaneous degradation of monochlorobenzene (MCB) and p-chloroaniline (PCA). Additionally, the effects of humic acid, Cl-, HCO3-, H2PO4-, HPO42- and water matrices were investigated and degradation pathways of MCB and PCA were proposed. The removal efficiencies of MCB and PCA were higher in FeCo@HC140-10/PMS system obtained under hydrothermal temperature of 140 °C than FeCo@HC180-10/PMS and FeCo@HC220-10/PMS systems obtained under higher temperatures. Radical species (i.e., SO4•-, •OH) and nonradical pathways (i.e., 1O2, Fe (IV)/Co (IV) and electron transfer through surface FeCo@HC140-10/PMS* complex) co-occurred in the FeCo@HC140-10/PMS system, while radical and nonradical pathways were dominant in degrading MCB and PCA respectively. The surface functional groups (i.e., C-OH and CO) and Fe/Co redox cycles played crucial roles in the PMS activation. MCB degradation was significantly inhibited in the mixed MCB/PCA solution over that in the single MCB solution, whereas PCA degradation was slightly promoted in the mixed MCB/PCA solution. These findings are significant for the provision of a low-cost and environmentally-benign synthesis of bimetal-hydrochar composites and more detailed understanding of the related mechanisms on PMS activation for simultaneous removal of the mixed contaminants in groundwater.

16.
J Hazard Mater ; 429: 128349, 2022 05 05.
Artigo em Inglês | MEDLINE | ID: mdl-35101763

RESUMO

Since little is known about the sorption/desorption behaviors of the mixed chlorobenzenes (CBs) on fresh and aged biochar, this study evaluated the co-sorption/co-desorption mechanism of the mixed monochlorobenzene (MCB), 1,2-dichlorobenzene (1,2-DCB) and 1,2,4-tirchlorobenzene (1,2,4-TCB) on the fresh bulk biochar derived from pinewood sawdust and corn straw under the heat treatment temperature (HTT) of 300 and 500 °C, and elucidated the aging-induced changes in the sorption/desorption of mixed CBs by biochar. The distinct sorption capacities of MCB< 1,2-DCB< 1,2,4-TCB were observed on all the tested biochar with the differences being further enhanced following the rise of HTT, as the main sorption mechanism was converted from phase partitioning to π-π interaction between graphitized biochar moieties and more hydrophobic aromatic chemicals. In comparison to the fresh biochar, the sorption suppression of the mixed CBs on the aged biochar was likely attributable to the reduction in accessibility to the aromatic carbon in biochar by introducing O-containing polar moieties on the biochar surfaces. Intriguingly, the kinetics of desorption was decreased with the aging of biochar may be caused by the increase in surface steric hindrance. These findings can provide new insights on understanding the co-sorption/co-desorption mechanism of the mixed CBs and help assess and manage the application of biochar on the treatment of contaminated soil and groundwater under field conditions.


Assuntos
Carvão Vegetal , Poluentes do Solo , Adsorção , Carbono , Carvão Vegetal/química , Clorobenzenos/química , Solo/química , Poluentes do Solo/análise
17.
J Hazard Mater ; 436: 129155, 2022 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-35596993

RESUMO

The heteroaggregation mechanism of nZVI with four types of natural soil nanoparticles (SNPs) extracted from representative soils in northern and southern China was investigated. Heteroaggregation rates between nZVI and SNPs were quantified by dynamic light scattering and evaluated as a function of ionic strength at pH 7. The nZVI-SNPs heteroaggregates were stable with hydrodynamic diameters (Dh) ranging from 400 to 600 nm in 0.1 mM solution. Based on the extended Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, nZVI underwent heteroaggregation with SNPs to form stable nZVI-SNPs nanohybrid due to the attachment of nZVI on the SNPs. However, with enhanced ionic strength, SNPs accelerated the aggregation of nZVI and formed large heteroaggregates with Dh in the range from 1200 to 2000 nm, owing to insignificant electrostatic repulsions and oppositely charged patches. In addition, the differences in the heteroaggregation rates of nZVI with four SNPs were negligible, caused by the negligible impacts of SNPs components such as soil organic matter and Fe/Al oxyhydroxides on the heteroaggregation of nZVI in the 10 mM NaCl solution. These findings are helpful for understanding the interaction between nZVI and SNPs and of significance to groundwater remediation using nZVI.


Assuntos
Nanopartículas , Solo , China , Concentração Osmolar , Eletricidade Estática
18.
Sci Total Environ ; 843: 157120, 2022 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-35787898

RESUMO

Implementing an economical and effective measure for treating acid mine drainage (AMD) from abandoned mines using low-cost restoration reagents present a significant challenge. In this study, natural attapulgite (AT) and soda residue (SR) composite particles (AT-SR) were firstly prepared and utilized in AMD treatment. The efficiencies and mechanisms of AT-SR composites for regulating acidity and removing metals in AMD, the critical factors influencing the treatment efficiencies, and the regeneration performance and environmental risk were investigated. It is illustrated that AT and SR quality ratio of 5:5, dosage of 0.5 g L-1, particle size < 1.5 mm, concentrations of 150 mg L-1 for Fe, 75 mg L-1 for Mn and 100 mg L-1 for Cu, Zn, Cd and Pb, and adsorption time of 120 min were the optimized conditions. The maximum adsorption capacities of Fe, Mn, Cu, Zn, Cd and Pb under single metal scenarios were 51.61, 22.30, 37.05, 40.21, 37.39 and 49.53 mg g-1, respectively. Under the mixed metal scenarios, competitive adsorption was predominated with the rate constants in the reducing order of 3.169 for Fe > 0.841 for Cu > 0.657 for Pb > 0.083 for Zn > 0.024 for Cd > 0.006 for Mn. The experimental data was fitted well with the pseudo-second-order and the Freundlich isotherm models. AT-SR is an outstanding neutralizer for AMD due to its richness in calcium and magnesium oxides and the spent AT-SR composites could be easily regenerated while maintaining high metal removal efficiencies under the subsequent usages. It is determined under the aqua regia digestion and Toxicity Characteristic Leaching Procedure (TCLP) tests that AT-SR can be used safely without posing environmental risks, thus promoting the resource recovery and utilization of soda residue and providing a green and effective method for treating AMD.


Assuntos
Metais Pesados , Poluentes Químicos da Água , Ácidos , Cádmio , Chumbo , Compostos de Magnésio , Metais Pesados/análise , Mineração , Compostos de Silício , Poluentes Químicos da Água/análise
19.
Environ Int ; 170: 107619, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36379201

RESUMO

In this work, S doped Fe2B (Fe2B-S) was synthesized by sintering method and applied for the enhanced dechlorination of trichlorethylene (TCE). The degradation ratio (D) of TCE was 99.8% with reaction rate constant (kobs) of 0.956 h-1 by 10.0at% S doped Fe2B (corresponding to Fe2B-S10.0), compared to D and kobs values 37.3% and 0.067 h-1 by Fe2B, respectively. The major dechlorination products of acetylene, ethene, ethane and C3-C6 hydrocarbon compounds were observed from a reductive ß-elimination pathway. S doped and undoped Fe2B could form the first-level in-situ galvanic cell, and the returned S provided a second-level galvanic cell to further enhance electron transfer. The doped S worked as electron donor to increase the density of localized unpaired electrons, and the electron enriched Fe atoms leading to stronger reducibility were verified by the density functional theory (DFT) calculation. This work provides a complete insight into the enhancement mechanism of S doped Fe2B and guides the potential design of zero-valent iron (ZVI) with properties tailored for chlorinated hydrocarbons dechlorination.

20.
Sci Total Environ ; 802: 149759, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34464793

RESUMO

Numerous studies have explored the transport mechanism of biochar colloids in porous medium. However, the effect of feedstock biopolymer compositions and pyrolytic temperature on carbon stability and mobility of biochar colloids is limited. This study prepared four ball milled biochar colloids pyrolyzed from lignin-rich pinewoods and cellulose-rich corn stalks under 300 °C and 500 °C (termed as PW300, PW500, CS300, CS500) and analyzed their differences in the chemical stability and transport behaviors. The results indicated that high contents of lignin in biomass and pyrolytic temperature could enhance the compact aromatic structures of biochar colloids characterized by the elemental composition, FTIR, 13C NMR and XRD analyses. Therefore, PW500 with the strongest chemical stabilities (least C loss of 13%), electronegativity (-44.9 mV vs. -41.6-28.3 mV) and smallest hydrodynamic diameter (608.7 nm vs. 622-997.2 nm) was obtained under ball milling. Moreover, both the critical coagulation concentrations (CCC) and the maximum relative effluent concentration (C/C0) with the NaCl ionic strength of 1 mM were demonstrated to be in the increase order of CS300 (76.1 mM, 70%) < PW300 (183.1 mM, 78%) < CS500 (363.9 mM, 89%) < PW500 (563.1 mM, 95%), which suggested stronger colloidal stability and mobility of PW biochar colloids than those of CS biochar colloids. In addition, the C/C0 for CS300, PW300 and CS500 were about 7.3%-36% lower than that for PW500 with the NaCl ionic strength increasing to 50 mM indicated the notable superiority in the mobility of PW500. These findings can provide new insights toward understanding the transformation and migration, and evaluating the environmental risk of biochar colloids.


Assuntos
Carbono , Lignina , Celulose , Carvão Vegetal , Coloides
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