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1.
Ecotoxicol Environ Saf ; 207: 111491, 2021 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-33254387

RESUMO

High-efficient and economic sorbents are highly desired for arsenic (As) emission control in flue gas from coal-fired power plant. A series of Fe-Mn binary oxides were prepared by a facile method, and their behaviors for gaseous arsenic removal in flue gas were investigated. The binary oxide exhibited a remarkable synergistic effect for arsenic removal compared with Mn or Fe monometallic oxide. The possible effects of CO2, NO, SO2, and O2 on the removal performance were also studied. The adsorption ability was excellent and stable in simulated flue gas conditions. X-ray photoelectron spectroscopy (XPS) and high-performance liquid chromatography atomic fluorescence spectroscopy (HPLC-AFS) coupling system were applied to analyze the species of surface-adsorbed arsenicals and soluble arsenicals. It was confirmed that the good sorption performance resulted from oxidation of As2O3 (As(III)) to As2O5 (As(V)) by Mn oxide and followed by efficient adsorption of As(V) on Fe oxide. Considering the toxicity of pentavalent arsenicals is lower than trivalent arsenicals, the oxidation of arsenic compounds can not only enhance its removal capacity but also decrease the toxicity of arsenicals after capture.


Assuntos
Poluentes Atmosféricos/química , Arsênico/química , Adsorção , Arsenicais , Gases , Oxirredução , Óxidos/química , Espectroscopia Fotoeletrônica
2.
Chemosphere ; 261: 128160, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-33113648

RESUMO

Up to now, complicated organoarsenicals were mainly identified in marine organisms, suggesting that these organisms play a critical role in arsenic biogeochemical cycling because of low phosphate and relatively high arsenic concentration in the marine environment. However, the response of marine macroalgae to inorganic arsenic remains unknown. In this study, Pyropia haitanensis were exposed to arsenate [As(V)] (0.1, 1, 10, 100 µM) or arsenite [As(III)] (0.1, 1, 10 µM) under laboratory conditions for 3 d. The species of water-soluble arsenic, the total concentration of lipid-soluble and cell residue arsenic of the algae cells was analyzed. As(V) was mainly transformed into oxo-arsenosugar-phosphate, with other arsenic compounds such as monomethylated, As(III), demethylated arsenic and oxo-arsenosugar-glycerol being likely the intermediates of arsenosugar synthesis. When high concentration of As(III) was toxic to P. haitanensis, As(III) entered into the cells and was transformed into less toxic organoarsenicals and As(V). Transcriptome results showed genes involved in DNA replication, mismatch repair, base excision repair, and nucleotide excision repair were up-regulated in the algae cells exposed to 10 µM As(V), and multiple genes involved in glutathione metabolism and photosynthetic were up-regulated by 1 µM As(III). A large number of ABC transporters were down-regulated by As(V) while ten genes related to ABC transporters were up-regulated by As(III), indicating that ABC transporters were involved in transporting As(III) to vacuoles in algae cells. These results indicated that P. haitanensis detoxifies inorganic arsenic via transforming them into organoarsenicals and enhancing the isolation of highly toxic As(III) in vacuoles.


Assuntos
Arsênico/toxicidade , Rodófitas/efeitos dos fármacos , Poluentes Químicos da Água/toxicidade , Arseniatos/química , Arseniatos/toxicidade , Arsênico/química , Arsenitos/química , Arsenitos/toxicidade , Cromatografia Líquida de Alta Pressão , Ecotoxicologia , Regulação da Expressão Gênica/efeitos dos fármacos , Espectrometria de Massas , Monossacarídeos/química , Rodófitas/genética , Rodófitas/metabolismo , Alga Marinha/efeitos dos fármacos , Poluentes Químicos da Água/química
3.
Bull Environ Contam Toxicol ; 105(4): 639-644, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32955595

RESUMO

Arsenic (As) and cadmium (Cd) are common soil pollutants whose opposing geochemical behaviors must be taken into account in the development of cost-effective, environmentally friendly remediation strategies. In this study, a pot experiment with lettuce and a field experiment with wheat were performed to examine the impacts of zeolite, biochar, MnO2, zero-valent iron (ZVI) individually and in binary combinations thereof on As-Cd pollution. The results of the pot experiment showed that biochar, MnO2 and ZVI had good passivation effects on As and Cd when provided individually, but the effects of a combination of 0.2% ZVI/0.5% biochar or 0.2% MnO2/0.5% ZVI were even better. These amendments were further investigated in a field experiment, which confirmed the positive effect of 0.2% MnO2/0.5% ZVI. Therefore, ZVI/biochar and MnO2/ZVI mixtures may offer effective solutions to the remediation of farmland soil contaminated with both As and Cd.


Assuntos
Arsênico/química , Cádmio/química , Recuperação e Remediação Ambiental/métodos , Poluentes do Solo/química , Arsênico/análise , Cádmio/análise , Carvão Vegetal , Poluição Ambiental , Fazendas , Ferro , Alface , Compostos de Manganês , Óxidos , Solo , Poluentes do Solo/análise , Triticum
4.
Chemosphere ; 260: 127574, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-32688316

RESUMO

Artisanal and small-scale gold mining (ASGM) operations are major contributors to the Philippines' annual gold (Au) output (at least 60%). Unfortunately, these ASGM activities lacked adequate tailings management strategies, so contamination of the environment is prevalent. In this study, soil contamination with copper (Cu), lead (Pb), zinc (Zn) and arsenic (As) due to ASGM activities in Nabunturan, Davao de Oro, Philippines was investigated. The results showed that ASGM-impacted soils had Cu, Pb, Zn and As up to 3.6, 83, 73 and 68 times higher than background levels, respectively and were classified as 'extremely' polluted (CD = 30-228; PLI = 5.5-34.8). Minerals typically found in porphyry copper-gold ores like pyrite, chalcopyrite, malachite, galena, sphalerite and goethite were identified by XRD and SEM-EDS analyses. Furthermore, sequential extraction results indicate substantial Cu (up to 90%), Pb (up to 50%), Zn (up to 65%) and As (up to 48%) partitioned with strongly adsorbed, weak acid soluble, reducible and oxidisable fractions, which are considered as 'geochemically mobile' phases in the environment. Although very high Pb and Zn were found in ASGM-impacted soils, they were relatively immobile under oxidising conditions around pH 8.5 because of their retention via adsorption to hydrous ferric oxides (HFOs), montmorillonite and kaolinite. In contrast, Cu and As release from the historic ASGM site samples exceeded the environmental limits for Class A and Class C effluents, which could be attributed to the removal of calcite and dolomite by weathering. The enhanced desorption of As at around pH 8.5 also likely contributed to its release from these soils.


Assuntos
Mineração , Poluentes do Solo/análise , Poluentes do Solo/química , Solo/química , Arsênico/análise , Arsênico/química , Cobre/análise , Cobre/química , Ouro/análise , Ferro/química , Compostos de Ferro/química , Chumbo/análise , Chumbo/química , Minerais/química , Filipinas , Sulfetos/química , Difração de Raios X , Zinco/análise , Zinco/química
5.
Chemosphere ; 259: 127403, 2020 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-32603963

RESUMO

The ability of thiol-modified humic acids (HAs) to release arsenic in tailings soil after being modified with different sulfur-containing reagents were significantly improved. The structure and physicochemical properties of humic acid (HA) before and after thiol-modification were characterized. The 3-MPTS-HA treated with 3-mercaptopropyltrimethoxysilane (3-MPTS) effectively improved the mobility of arsenic, and its reducing ability was increased from 2 mmol g-1 to 3.54 mmol g-1. The S content of humic acids were also significantly increased after treatment with sulfur-containing reagents, in which the oxygen-containing functional group (e.g., C = O, C-O) on the surface of HA may be the active sites for binding with sulfur-containing reagents. It was found in the XPS spectrum that because the thiol group is easily oxidized, there are many S forms in thiol-modified HA. The -SH content in Na2S·9H2O-HA, l (+)-Cysteine-HA (Cys-HA), thioglycolic acid (TGA-HA) and 3-MPTS-HA was determined by fluorescence method to be 13.9, 78.45, 90.34, and 192.29 µmol g-1, respectively. The study demonstrated that surface thiol modification can increase the abundance of thiol in HA and enhance reactivity, which will further promote the application of HA in the treatment of heavy metal contaminated tailing soil.


Assuntos
Arsênico/química , Poluentes do Solo/química , Substâncias Húmicas/análise , Metais Pesados/química , Solo/química , Poluentes do Solo/análise , Compostos de Sulfidrila
6.
Chemosphere ; 261: 127688, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-32721688

RESUMO

Arsenic(III) oxidation is a critical pre-treatment step for overall arsenic immobilization in concentrated industrial arsenic streams. Activated carbon (AC) catalysis is a green, economical and efficient method to oxidize As(III) from waters with high arsenic concentration prior to its removal through precipitation or adsorption. This research investigates AC-catalyzed oxidation process for oxidizing aqueous solutions of As(III) and proposed the possible reaction pathway. Batch tests were performed and efficient oxidation of 2.0 g/L acidic As(III) solution have been induced on AC surfaces in the presence of oxygen. The in-situ formation of reactive oxygen species on carbon surfaces and arsenic adsorption onto AC play important roles in As(III) oxidation. The kinetics of adsorption and catalyzed oxidation has been studied and the samples were characterized using ICP-OES, Zeta potential, TEM coupled with EDX and XPS techniques. A systematic reaction pathway was proposed, and reusability of AC has confirmed the economic viability of the proposed green process. This study offers a promising and facile solution for As(III) oxidation from waste water, mining and metal industrial waste streams under ambient conditions for arsenic immobilization.


Assuntos
Arsênico/química , Poluentes Químicos da Água/química , Adsorção , Catálise , Carvão Vegetal , Concentração de Íons de Hidrogênio , Resíduos Industriais , Cinética , Metais , Oxirredução , Oxigênio , Águas Residuárias , Água , Poluentes Químicos da Água/análise , Purificação da Água/métodos
7.
Environ Geochem Health ; 42(11): 3983-3993, 2020 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-32661877

RESUMO

Massive quantities of alkaline rocks are excavated from urban coastal and mountain areas to make underground spaces available for infrastructure projects; however, such excavated rock often releases arsenic. In the present study, arsenic release from the excavated rocks with steel slag was investigated using dialysis and batch leaching tests to understand where arsenic is immobilized and which components in the steel slag suppress arsenic release from the excavated rock. Dialysis test indicated that the addition of steel slag at 10 wt% could suppress arsenic release at a level greater than 66%. The total arsenic content in the steel slag did not increase as compared with that before the test. Sequential extraction analysis indicated that the arsenic released during the dialysis test is mainly derived from arsenic fraction 1 (nonspecifically bound) due to the higher amount of this arsenic fraction in the excavated rock with the steel slag. Moreover, the steel slag extract could suppress arsenic release from the excavated rock and remove the arsenic from aqueous solution. The pH dependence test further indicated that the arsenic immobilized by the steel slag extract was stable under alkaline pH conditions. The levels of arsenic release decreased with increasing calcium release from the steel slag regardless of the type of excavated rock with an alkaline pH and were particularly seen at calcium released > 500 mg kg-1. These results indicate that the arsenic immobilization could be occurred not on the surface of steel slag, but on the excavated rock, and the calcium dissolved from the steel slag regulates the behavior of arsenic release from the surface of excavated rock. The findings of the present study suggest that the steel slag could be utilized to enable the reuse of excavated sedimentary and metamorphic rock of alkaline pH for the control of arsenic release.


Assuntos
Arsênico/análise , Arsênico/química , Cálcio/química , Resíduos Industriais , Indústria da Construção , Concentração de Íons de Hidrogênio , Aço/química , Poluentes Químicos da Água/análise
8.
Chemosphere ; 259: 127503, 2020 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-32645597

RESUMO

Fe-Mn nodules affect the speciation, transformation and migration of arsenic (As) via redox and adsorption reactions. However, few studies have been concerned with their interaction in the presence of dissolved oxygen. In this work, the interaction mechanism of As(III) and Fe-Mn nodules was studied in different atmospheres. The influence of pH, dissolved oxygen concentration and chemical composition of nodules on the reaction was also investigated. The results indicated that manganese oxides and iron oxides in nodules respectively contribute to As(III) oxidation and As(III,V) adsorption. Under oxic conditions, Fe-Mn nodules acted as a catalyst to accelerate the oxidation of Mn(II) to Mn(III,V) oxides, which significantly enhanced As(III) oxidation. In the system containing 10 mg L-1 As(III) and 1.0 g L-1 Fe-Mn nodules, the maximum oxidation capacity of As(III) reached 3.22, 3.48 and 3.71 mg g-1, and the corresponding As(III,V) adsorption capacity reached 2.49, 2.40, and 2.39 mg g-1 in nitrogen, air and oxygen atmosphere, respectively. The oxidation capacity of As(III) increased and decreased with increasing dissolved oxygen concentration and pH, respectively. This work clarifies the mechanism of As(III) oxidation by soil Fe-Mn nodules in various systems and contributes to a better understanding of the behaviors and fate of As in environments.


Assuntos
Arsênico/química , Arsenitos/química , Compostos Férricos/química , Compostos de Manganês/química , Óxidos/química , Oxigênio/química , Adsorção , Catálise , Oxirredução
9.
Chemosphere ; 258: 127329, 2020 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-32540535

RESUMO

Due to the neutral charge of As(III) oxy-ions that make approaching the traditional adsorbent very improbable compared to the As(V) case, making it harder to be separated. To enhance the adsorption of As(Ш), the FeOOH coated cellulose acetate (CA) membrane doped with MnO2 nanoparticles (FeOOH@MnO2@CAM) was fabricated and then to removes As(Ш) in water through the synergistic effect of oxidation and adsorption, and the maximum adsorption capacity can reach 50.34 mg/g. FeOOH@MnO2@CAM was fabricated with CA as a substrate by dipping-precipitation phase inversion and hydrothermal method. Langmuir and pseudo-second-order model showed that As(Ш) was adsorbed by chemical interactions through the monolayer and thermodynamic showed that As(Ш) adsorption was an exothermic and spontaneous process. The results of the pH study showed that as the pH increases from 3 to 11, the adsorption capacity of As(Ш) decreases from 50.34 to 14.32 mg/g, which was attributed to the acidic environment promoting the protonation of the surface of FeOOH@MnO2@CAM, which increases the electrostatic attraction, and the alkaline environment increases electrostatic repulsion due to deprotonation. The competitive ions exhibited the PO43- significantly reduce the adsorption capacity of As(Ш),and as the PO43- content increases, the adsorption capacity of As(Ш) decreases from 29.76 to 18.57 mg/g, which was attributed to the similar chemical properties of PO43- and arsenate. Importantly, FeOOH@MnO2@CAM still maintains an adsorption capacity of 20.19 mg/g after seven cycles, demonstrating that it is a kind of environmentally friendly material to remove As(Ш) in the water environment.


Assuntos
Arsênico/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Compostos de Manganês/química , Oxirredução , Óxidos/química , Água
10.
Chemosphere ; 254: 126780, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32353809

RESUMO

The presence of As(V) and Mn(VII) in water beyond the permissible concentration allowed by World Health Organization (WHO) standard affects human beings, animals and the environment adversely. Hence, there is need for an efficient material to remove these potentially toxic elements from wastewater prior to discharge into water bodies. This research focused on the application of response surface method (RSM) assisted optimization of Fe-Ni/Activated carbon (AC) catalyst for the synthesis of MWCNTs. Also, the MWCNTs was carboxylated and the adsorption behaviors of both nano-adsorbents in the removal of As(V) and Mn(VII) from industrial wastewater was investigated through experimental and computational techniques. The prepared Fe-Ni/AC, MWCNTs and MWCNTs-OCH2CO2H were characterized using BET, TGA, FTIR, HRSEM, HRTEM, XRD and XPS. The result showed the BET surface area of Fe-Ni/AC, MWCNTs and MWCNTs-OCH2CO2H were obtained as 1100, 1250 and 1172 m2/g, respectively. Due to the enhanced impact of carboxylation, the adsorption capacity of As(V) and Mn(VII) removal increased from 200 to 192 mg/g for MWCNTs to 250 and 298 mg/g for MWCNTs-OCH2CO2H. The isotherm and kinetic models were best fitted by Langmuir and pseudo-second order kinetics, while the thermodynamic investigation found that the adsorption process was endothermic, spontaneous and chemisorptions controlled. The regeneration potential of MWCNTs and MWCNTs-OCH2CO2H after six repeated applications revealed good stability of adsorption efficiency. The study demonstrated optimization importance of Fe-Ni/AC catalyst design for MWCNTs adsorbents and the potentials of utilizing both MWCNTs and MWCNTs-OCH2CO2H in the removal of selected heavy metals from water and soil.


Assuntos
Arsênico/química , Manganês/química , Nanotubos de Carbono/química , Águas Residuárias/química , Poluentes Químicos da Água/análise , Adsorção , Carvão Vegetal , Concentração de Íons de Hidrogênio , Cinética , Metais Pesados , Termodinâmica , Eliminação de Resíduos Líquidos , Água , Purificação da Água/métodos
11.
Food Chem ; 327: 127033, 2020 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-32464459

RESUMO

Some varieties of edible mushrooms can accumulate high contents of arsenic, which is a public health concern. In this study, we developed a high-performance liquid chromatography method linked to inductively coupled plasma triple quadrupole mass spectrometry (HPLC-ICP-MS/MS) for sensitive and accurate determination of arsenite, arsenate, monomethylarsonic acid, dimethylarsinic acid, arsenocholine and arsenobetaine in edible mushrooms. The six arsenic species were extracted ultrasonically from mushrooms using ultrapure water at 60 °C as the solvent, separated on a PRP-X100 anion exchange column (4.1 × 250 mm, 10 µm), with 20 mmol/L NH4HCO3 and 50 mmol/L (NH4)2CO3 as the mobile phase, and quantified using ICP-MS/MS in the oxygen reaction mode. The linear range of the method was 0.5 µg/L-100 µg/L with detection and quantification limits of 2.5 µg/kg-10 µg/kg (S/N = 3), and 8 µg/kg-33 µg/kg (S/N = 10), respectively. This method was applied successfully to the detection and speciation of arsenic in eight varieties (266 samples) of mushrooms. Our results indicated that most wild edible mushrooms contained organic arsenic, mainly arsenobetaine and arsenocholine. However, the inorganic arsenic content of Armillariella tabescens (3.63 mg/kg) and parts of the cultivated Agaricus blazei murrill (up to 4.50 mg/kg) were relatively high, which is potential risk to the health of consumers.


Assuntos
Agaricus/química , Arsênico/análise , Arsênico/química , Cromatografia Líquida de Alta Pressão , Análise de Alimentos/métodos , Espectrometria de Massas
12.
Chemosphere ; 251: 126388, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32443223

RESUMO

Over the last few decades, the global pollution of surface and groundwater poses a serious threat not only to human beings but also towards aquatic lives due to the presence of emerging contaminants. Among the others, the presence of arsenic, fluoride, and iron are considered as the most common toxic pollutants in water bodies. The emergence of metal organic frameworks (MOFs) with high porosity and surface area is represented as significant inclusion into the era of entrapping contaminants present in drinking water. In the present review article, an in-depth insight is provided on the recent developments in the removal of arsenic, fluoride, and iron from drinking water using MOFs. Various aspects related to the synthesis, latest technologies adopted for the modifications in the synthesis process and advanced applications of MOFs for the removal of such contaminants are explicitly discussed. A detailed insight was provided to understand the mechanism of various interactions of MOFs with arsenic and fluoride. With respect to arsenic, fluoride, and iron removal the ultrastructural morphology of MOFs is assessed based on different molecular arrangements. Further, commercial aspects of various MOFs are presented in order to highlight the process feasibility. Finally, various perspectives and challenges involved in process scale up are comprehensively narrated with an aspiration of futuristic developments. The paper will be beneficial to the readers for acquiring a piece of in-depth knowledge on MOFs and its various synthesis approaches along with remarkable achievements for the removal of arsenic, fluoride, and iron from contaminated drinking water.


Assuntos
Arsênico/química , Água Potável/química , Fluoretos/química , Ferro/química , Poluentes Químicos da Água/química , Arsênico/análise , Poluentes Ambientais , Água Subterrânea/química , Humanos , Ferro/análise , Estruturas Metalorgânicas , Poluentes Químicos da Água/análise , Poluição da Água , Purificação da Água/métodos
13.
Chemosphere ; 255: 126938, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32388258

RESUMO

Jarosite is an important scavenger for arsenic (As) due to its strong adsorption capacity and ability to co-precipitate metal(loid)s in acid mine drainage (AMD) environments. When subjected to natural organic matter (NOM), metastable jarosite may undergo dissolution and transformation, affecting the mobility behavior of As. Therefore, the present study systematically explored the dissolution and transformation of jarosite, and the consequent redistribution of coprecipitated As(V) under anoxic condition in the presence of a common phenolic acid-gallic acid (GA). The results suggested that As(V) incorporating into the jarosite structure stabilized the mineral and inhibited the dissolution process. Jarosite persisted as the dominant mineral phase at pH 2.5 up to 60 d, though a large amount of structural Fe(III) was reduced by GA. However, at pH 5.5, jarosite mainly transformed to ferrohexahydrite (FeSO4·6H2O) with GA addition, while the principal end-product was goethite in GA-free system. The dissolution process enhanced As(V) mobilization into aqueous and surface-complexed phase at pH 2.5, while co-precipitated fraction of As(V) remained dominant under pH 5.5 condition. Result of XPS indicated that no reduction of As(V) occurred during the interaction between GA and As(V)-bearing jarosite, which would limit the toxicity to the environment. The reductive process involved that GA promoted the dissolution of jarosite via the synergistic effect of ligand and reduction, following by GA and release As(V) competing for active sites on mineral surface. The findings demonstrated that phenolic groups in NOM can exert great influence on the stability of jarosite and partitioning behavior of As(V).


Assuntos
Arsênico/química , Compostos Férricos/química , Ácido Gálico/química , Sulfatos/química , Adsorção , Compostos de Ferro , Minerais , Mineração , Oxirredução
14.
Chemosphere ; 255: 126937, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32402882

RESUMO

Phosphate competes with arsenate for sorption sites on poorly crystalline iron and aluminum (hydr)oxides. The competition has implications e.g. for the management of arsenic-contaminated soil and water. Phosphate competition with arsenate on mixed phases containing both iron and aluminum (hydr)oxides has rarely been investigated. Here, the phosphate competition with arsenate on mixtures of poorly crystalline aluminum hydroxide (Alhox) and ferrihydrite (Fh), was investigated in batch experiments at pH 6.5. X-ray absorption spectroscopy (XAS) was performed on the phosphorus and arsenic K edges, which offered a unique insight in the partitioning of arsenate and phosphate on mixed Alhox-Fh sorbents. Under the studied conditions the sorption capacity of the mixed sorbents (per mol Al or Fe) increased at higher Alhox to Fh ratios. The XAS measurements provided direct evidence that phosphate competed more effectively with arsenate for sorption sites on Alhox than on Fh. For example, in a mixture with 50% of both sorbents and with similar additions of arsenate and phosphate, 71% of the oxyanions adsorbed on Fh and 46% on Alhox were arsenate. Consequently, phosphate may mobilize arsenate more easily from mixed iron-aluminum matrices that are rich in aluminum.


Assuntos
Hidróxido de Alumínio/química , Arseniatos/química , Fosfatos/química , Adsorção , Alumínio/química , Arsênico/química , Compostos Férricos , Ferro/química , Óxidos/química , Água
15.
Chemosphere ; 254: 126769, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32361537

RESUMO

A series of alginate-derived porous graphitic carbon (PGC) wrapped iron-based organic frameworks (Fe-MIL-88B) composites were synthesized and checked their ability for the removal of arsenite (As(III)) and arsenate (As(V)) from water. Various amounts of PGC (5, 10, 20, and 50 wt/wt %) were utilized as a wrapping material for the development of composites with Fe-MIL-88B@PGCx% and optimized for As(III)/As(V) adsorption. The chemical functionalities, structure, morphology, porous properties and bonding nature of the adsorbents were analyzed using FTIR, PXRD, SEM, BET, and XPS, respectively. Fe-MIL-88B@PGC20% composite was explored to have maximum removal efficiency and fastest adsorption kinetics for As(III)/As(V), of all Fe-MIL-88B@PGCx% composites and pristine Fe-MIL-88B studied here. The developed adsorbents are highly pH dependent and selective in common co-existing anions except for F-, PO43- and humic acid. The Langmuir isotherm studies of As(III) and As(V) adsorption suggest maximum adsorption capacities of 1.6853 and 2.2636 mmol/g, at pH of 3.0 and 9.2, respectively. The XPS analysis of As(III)-sorbed Fe-MIL-88B@PGC20% composite reveals that a portion of As(III) has been oxidized into As(V) during the adsorption process. The continuous flow-bed column study indicates that bed volumes of 249.6 and 452.8 mL of As(III) and As(V) contaminated water was treated, respectively, also reduced the concentration of As(III)/As(V) to less than WHO standards (<10 µg/L).


Assuntos
Arsênico/química , Estruturas Metalorgânicas/química , Poluentes Químicos da Água/química , Adsorção , Arsenitos , Biopolímeros , Carbono , Grafite , Ferro/química , Cinética , Oxirredução , Porosidade , Purificação da Água
16.
Mater Sci Eng C Mater Biol Appl ; 111: 110755, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32279796

RESUMO

Tooeleite is the only known ferric arsenite sulfate mineral and has environmental significance for arsenic remediation. This study investigated the formation and stability of biogenic tooeleite in Fe(II)-As(III)-SO42- environment using Acidithiobacillus ferrooxidans under the ambient conditions. The results show that bacteria facilitated the formation and crystallization of tooeleite owing to the microbial oxidation of Fe(II) to Fe(III). Due to the better growth of bacteria, the higher removal of As(III) by tooeleite formation was achieved under 8.978-10.806 g/L initial Fe(II) concentration and 2.00-3.00 initial pH, and the highest efficiency was ~95%. Fe(III) and As(III) precipitated simultaneously into two types of tooeleite. The relatively stable tooeleite is featured by the developed (020) crystal face and the bulk-like structure with thick flakes. This study yields a better understanding of biogenic tooeleite, and the importance of tooeleite formation in As(III)-rich environment for arsenic remediation.


Assuntos
Acidithiobacillus/metabolismo , Arsênico/metabolismo , Compostos Férricos/química , Ferro/metabolismo , Acidithiobacillus/química , Arsênico/química , Arsênico/isolamento & purificação , Cristalização , Concentração de Íons de Hidrogênio , Ferro/química , Oxirredução
17.
Chemosphere ; 250: 126268, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32234619

RESUMO

The effectiveness of rice waste biochars on heavy metal and metalloid abatement and detoxification was investigated using comprehensive studies based on As and Cd immobilization, bioaccumulation in tubifex, and microbial community changes in contaminated sediment. The remediation effects of biochars produced at different pyrolytic temperatures (400-700 °C) were evaluated. Bioaccumulation of heavy metal and metalloid in the tubifex tissue and change of indigenous microbial community under treatment of different biochars were assessed. Biochars produced at 700 °C exhibited greater effect on decreasing the concentrations of As and Cd in aqueous phase, and TCLP extractable and bioavailable metal(loid) in solid phase of sediment. The concentration of As and Cd in water phase decreased by 26%-89% and 22%-71% under the treatment of straw biochar, and decreased by 13%-92% and 5%-64% under the treatment of rice husk biochar, respectively. As and Cd contents in the tubifex tissue were positively correlated with their concentrations in aqueous phase. High-temperature biochars significantly reduced metal(loid) bioaccumulation in tubifex. The richness and biodiversity of microbial community were both greater in all biochars remediated sediment compared to non-treated sediment. These results indicated that rice waste biochars could effectively inhibit the bio-availability and toxicity of heavy metal and metalloid in sediment, and the higher-temperature biochar exhibited better performance.


Assuntos
Arsênico/química , Cádmio/química , Carvão Vegetal/química , Recuperação e Remediação Ambiental , Disponibilidade Biológica , Inativação Metabólica , Metais Pesados , Oryza , Pirólise , Temperatura , Água
18.
Chemosphere ; 253: 126702, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32302903

RESUMO

Iron (Fe)-based adsorbents have been promoted for aqueous arsenic adsorption because of their low cost and potential ease of scale-up in production. However, their field application is, so far, limited because of their low Fe use efficiency (i.e., not all available Fe is used), slow adsorption kinetics, and low adsorption capacity. In this study, we synthesized graphene oxide iron nanohybrid (GFeN) by decorating iron/iron oxide (Fe/FexOy) core-shell structured iron nanoparticles (FeNPs) on the surface of graphene oxide (GO) via a sol-gel process. The deposition of FeNPs on GO for the nanohybrid (GFeN) improves Fe use efficiency and arsenic mobility in the nanohybrid, thereby improving the arsenic removal capacity and kinetics. We achieved removal capacities of 306 mg/g for As(III) and 431 mg/g for As(V) using GFeN. Rapid reduction (>99% in <10 min) of As(III) and As(V) (initial concentration, C0 = 100 µg/L) was achieved with the nanohybrid (250 mg/L). There were no significant interferences by the coexisting anions and organic matters at environmentally relevant concentrations. Based on the experimental data, we have proposed that both electrostatic interaction and surface complexation contributed to ultra-high arsenic removal by GFeN. The GO sheets acted as the reservoirs for the electrons released during surface corrosion of the FeNPs and the electrons were transferred back to the FeNPs to rejuvenate the oxidized surface. The rejuvenated FeNP surface layer helped in additional arsenic removal.


Assuntos
Arsênico/química , Poluentes Químicos da Água/química , Adsorção , Ânions , Arsênico/análise , Compostos Férricos/química , Grafite/química , Concentração de Íons de Hidrogênio , Ferro , Cinética , Nanopartículas , Oxirredução , Água , Poluentes Químicos da Água/análise , Purificação da Água/métodos
19.
Chemosphere ; 254: 126700, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32334244

RESUMO

Arsenic is easily evaporated with coal combustion, which not only causes serious environmental issues but also leads to the deactivation of selective catalytic reduction (SCR) catalyst. This study focused on the re-using of coal-fired fly ash for arsenic vapors in-situ retention before SCR catalyst in the furnace. Experiments were carried out to estimate the effects of typical fly ash compounds (Ca-, Fe-, and Al-bearing components) as well as acid gases (SO2/NO) on arsenic capture at temperatures of high-temperature furnace stage (900 °C) or SCR system entry stage (450 °C). The results demonstrated that, regardless of collection plants, all the ash samples showed certain capacity in arsenic vapors retention and the capture performance was enhanced at 900 °C than at 450 °C. Both physical and chemical adsorptions occurred for arsenic capture at low temperature, while chemical adsorption by effective mineral components dominated at high temperature. The role of Ca-compounds was more remarkable than Fe/Al-compounds and CaSO4/calcium silicates were identified as the key calcium compounds that acted on arsenic adsorption by fly ash. Insignificant effects were found regarding the acid gases (SO2 and NO) on arsenic retention by fly ash owing to the high resistance of CaSO4 and calcium silicates to acid gases. These findings provided reference for the in-situ retention of arsenic by reusing fly ash that enriched in specific compositions.


Assuntos
Arsênico/química , Cinza de Carvão/química , Adsorção , Compostos de Cálcio , Catálise , Carvão Mineral/análise , Gases , Modelos Químicos , Silicatos , Temperatura
20.
PLoS One ; 15(4): e0231475, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32330139

RESUMO

The threat of arsenic contamination to public health, particularly in developing countries, has become a serious problem. Millions of people in their daily lives are still highly dependent on groundwater containing high levels of arsenic, which causes excessive exposure to this toxic element, due to the high cost and lack of water-treatment infrastructures. Therefore, a technique for large-scale treatment of water in rural areas to remove arsenic is needed and should be low-cost, be easily customized, and not rely on electrical power. In this study, in an effort to fulfill those requirements, we introduce a three-dimensional (3D), printed water-filtration system for arsenic removal. Three-dimensional printing can provide a compact, customized filtration system that can fulfill the above-mentioned requirements and that can be made from plastic materials, which are abundant. Armed with the versatility of 3D printing, we were able to design the internal surface areas of filters, after which we modified the surfaces of the 3D, printed filters by using iron (III) oxide as an adsorbent for arsenite. We investigated the effects of the controlled surface area on the flow rate and the deposition of the adsorbent, which are directly related to the adsorption of arsenic. We conducted isotherm studies to quantify the adsorption of arsenic on our 3D, printed filtration system.


Assuntos
Arsênico/química , Arsenitos/química , Filtração/métodos , Poluentes Químicos da Água/química , Purificação da Água/métodos , Água/química , Adsorção , Água Subterrânea/química , Ferro/química
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