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1.
Chemosphere ; 361: 142529, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38838862

RESUMO

A novel nanocomposite consisting of Fe3O4-loaded tin oxyhydroxy-chloride is demonstrated as an efficient adsorbent for the removal of hexavalent chromium in compliance to the new drinking water regulation. This study introduces a continuous-flow production of the nanocomposite through the separate synthesis of (i) 40 nm Fe3O4 nanoparticles and (ii) multilayered spherical arrangements of a tin hydroxy-chloride identified as abhurite, before the application of a wet-blending process. The homogeneous distribution of Fe3O4 nanoparticles on the abhurite's morphology, features nanocomposite with magnetic response whereas the 10 % loaded nanocomposite preserves a Cr(VI) uptake capacity of 7.2 mg/g for residual concentrations below 25 µg/L. Kinetic and thermodynamic examination of the uptake evolution indicates a relative rapid Cr(VI) capture dominated by interparticle diffusion and a spontaneous endothermic process mediated by reduction to Cr(III). The efficiency of the optimized nanocomposite was validated in a pilot unit operating in a sequence of a stirring reactor and a rotary magnetic separator showing an alternative and competitive application path than typical fixed-bed filtration, which is supported by the absence of any acute cellular toxicity according to human kidney cell viability tests.


Assuntos
Cromo , Água Potável , Nanocompostos , Poluentes Químicos da Água , Purificação da Água , Cromo/química , Nanocompostos/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Água Potável/química , Adsorção , Cinética , Humanos , Termodinâmica
2.
Chemosphere ; 361: 142531, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38838864

RESUMO

In site chromium (Cr) contaminated soil characterized by high alkalinity and carbonate content, protons are not effectively targeted for Cr(III) mobilization but rather accelerate the reduction of easily transportable Cr(VI) within the acidification electrokinetic (EK) system. As an alternative, the highly alkaline extraction conditions (HAECs) maintained by anolyte regulation are explored owing to the ability to desorb strong binding Cr(VI) and form anionic Cr(III)-hydroxides (Cr(OH)4-, Cr(OH)52-). The results demonstrate that HAECs were more efficient in mobilizing ions in severe alkalinity and electrical conductivity soil compared to organic acid acidifying extraction conditions (OAECs). Simultaneously, a limited amount of soluble Cr(III) was produced; however, its transportation was hindered and more noticeable in the case of Cr(VI), displaying a distinct retention phase within the intermediate soil chamber. The antagonistic interplay between electromigration and electroosmotic flow was considered the main responsible factor. The conversion intensity of Cr(VI) to Cr(III) was inhibited at HAECs. The promising mobilization and low conversion intensity contributed to total Cr removal. At HAECs, enhanced electromigration and electroosmotic flow combined with a favorable oxidation environment may facilitate in situ delivery of oxidants, offering practical implications for the EK detoxification of high alkalinity site soil contaminated with Cr. The practicability of HAECs is likely to be enhanced when the cost-benefit balance of providing a simultaneous energy supply during site treatment is resolved.


Assuntos
Cromo , Poluentes do Solo , Solo , Cromo/química , Poluentes do Solo/análise , Poluentes do Solo/química , Solo/química , Concentração de Íons de Hidrogênio , Recuperação e Remediação Ambiental/métodos , Oxirredução
3.
Chemosphere ; 361: 142539, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38844110

RESUMO

The feasibility of using hexagonal boron nitride (h-BN) to treat heavy metal Cr(III) from model contaminated groundwater was evaluated in this study by adsorption experiments and characterizations. To the best of our knowledge, this study is the first attempt to conduct the adsorption of Cr(III) by h-BN under various experimental conditions such as exposure time, ratio of adsorbates and adsorbents, solution pH, background ions with different ionic strength, and the presence of humic acids (HA) in model contaminated groundwater. The optimized h-BN showed excellent maximum adsorption capacity (i.e., 177 mg ∙ g-1) when the concentrations of Cr(III) and h-BN were 10 and 10 mg ∙ L-1, respectively. Subsequently, we confirmed there was a negligible change in the adsorption performance of Cr(III) by h-BN in the presence of co-ions (i.e., K and Mg) in concentrations in a range from 50 to 1000 mg ∙ L-1. Furthermore, the adsorption performance of Cr(III) gradually improved with HA concentrations from 2.5 to 25 mg ∙ L-1. Interestingly, the maximum adsorption performance of Cr(III) by both HA and h-BN increased until 500 mg ∙ g-1 in the presence of 25 mg ∙ L-1 HA. The adsorption mechanism was clarified by Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy. Additionally, we successfully confirmed that h-BN could be reused until five cycles. On the basis of the adsorption performance results and characterizations, h-BN can be utilized as an efficient and practical adsorbent to treat Cr(III) in groundwater treatment.


Assuntos
Compostos de Boro , Cromo , Água Subterrânea , Poluentes Químicos da Água , Adsorção , Cromo/química , Água Subterrânea/química , Poluentes Químicos da Água/química , Compostos de Boro/química , Purificação da Água/métodos , Substâncias Húmicas/análise , Concentração de Íons de Hidrogênio , Íons/química
4.
Chemosphere ; 361: 142516, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38850691

RESUMO

Activated siderite, endowed with excellent properties, was simply prepared by co-grinding with Fe sulfate to enhance its high reducing ability for Cr(VI). Batch experiments were conducted to investigate the main affecting parameters, such as material ratio, pH, temperature, etc. The removal of Cr(VI) by activated siderite was completed within 4 h of the reaction. The activated siderite maintained a high removal effect of Cr(VI) within a wide pH range (3-9). Various analytical methods, including XRD, SEM/EDS, XPS, etc., were employed to characterize the samples and discover variations before and after the reaction. The Fe (Ⅱ) in activated siderite becomes highly active, and it can even be released from the solid phase in the mildly acidic liquid phase to efficiently reduce Cr(VI) and mitigate its toxicity. These findings introduce an innovative approach for activating various minerals widely distributed in nature to promote the recovery of the ecological system.


Assuntos
Cromo , Compostos Férricos , Oxirredução , Cromo/química , Compostos Férricos/química , Concentração de Íons de Hidrogênio , Ferro/química , Compostos Ferrosos/química , Minerais/química , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/química , Carbonatos
5.
Environ Monit Assess ; 196(7): 611, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38862850

RESUMO

The wastewater effluent is responsible for the major ecological impact of the dairy sectors. To avoid the negative consequences of heavy metal pollution on the ecosystem, creative, affordable, and efficient treatment methods are now required before the effluent flows into the surrounding area. This study was aimed at assessing the effectiveness of three different adsorbents for Cd+2 and Cr+6 ions from wastewater effluents of dairy farms, including chitosan (CS), clinoptilolite zeolite (CZ), and chitosan/clinoptilolite zeolite (CS/CZ) composite. The adsorption kinetics of the CS/CZ composite were established using the effects of the key variables (pH, agitation speed, adsorbent concentrations, and contact durations). The removal (%) and adsorption capacities, qe (mg/g), were calculated using the data from the adsorption kinetics. Wastewater samples (n = 60) were collected from the wastewater effluents of five farms. Cd+2 and Cr+6 ion concentrations in all collected samples were determined. Following the CS/CZ composite creation, it was characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (X-RD), and Fourier-transform infrared spectrum (FT-IR). The CS/CZ composite had an adsorption capacity of 92.4 and 96.5 mg/g for both Cd+2 and Cr+6 ions at a concentration of 2.0 g/100 ml, respectively, while the CZ adsorption capacities for the two ions were 87.5 mg/g and 61.0 mg/g, respectively, at 4.0 g/100 ml concentration. The CS was achieved at 55.56 mg/g and 33.3 mg/g, respectively, at the same concentration. The efficiency of heavy metal removal was enhanced by increasing adsorbent concentration, agitation speed, and contact duration. Using CS/CZ composite at 2.0 g/100 ml concentration, 180 min of contact time, and 300 rpm agitation speed, the greatest removal efficiencies for Cd+2 and Cr+6 ions (96.43 and 98.75%, respectively) were demonstrated.


Assuntos
Cádmio , Quitosana , Indústria de Laticínios , Eliminação de Resíduos Líquidos , Águas Residuárias , Poluentes Químicos da Água , Zeolitas , Zeolitas/química , Quitosana/química , Poluentes Químicos da Água/análise , Águas Residuárias/química , Adsorção , Cádmio/análise , Animais , Eliminação de Resíduos Líquidos/métodos , Bovinos , Cromo/análise , Cromo/química , Fazendas , Purificação da Água/métodos
6.
J Environ Manage ; 362: 121340, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38824889

RESUMO

Co-pyrolysis of biomass with phosphogypsum (PG) presents an effective strategy for facilitating the recycling of PG resources. However, it is crucial to note the environmental threats arising from the presence of Pb, Cr, Ni, and F in PG. This study investigated the effect of immobilization and transformation of four elements during co-pyrolysis with biomass and its components. The co-pyrolysis experiments were carried out in a tube furnace with a mixture of PG and corn stover (CS), cellulose (C), lignin (L), glucose (G). Co-pyrolysis occurred at varying temperatures (600 °C, 700 °C, 800 °C, and 900 °C) and different addition ratios (10%, 15%, and 20%). The results indicated that an increase in co-pyrolysis temperature was more conducive to the immobilization and transformation of harmful elements in PG, demonstrating significant efficacy in controlling F. Additionally, the addition of biomass components exerts a significant impact on inhibiting product toxicity, with small molecules such as glucose playing a prominent role in this process. The mechanism underlying the control of harmful elements during co-pyrolysis of PG and biomass was characterized by three main aspects. Firstly, biomass components have the potential to melt-encapsulate the harmful elements in PG, leading to precipitation. Secondly, the pyrolysis gas produced during the co-pyrolysis process contributes to the formation of a rich pore structure in the product. Finally, this process aids in transforming hazardous substances into less harmful forms and stabilizing these elements. The findings of this study are instrumental in optimizing the biomass and PG blend to mitigate the environmental impact of their co-pyrolysis products.


Assuntos
Biomassa , Sulfato de Cálcio , Cromo , Flúor , Chumbo , Níquel , Níquel/química , Cromo/química , Chumbo/química , Flúor/química , Sulfato de Cálcio/química , Fósforo/química , Zea mays
7.
J Hazard Mater ; 475: 134580, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38865829

RESUMO

In this research, a new material, chitosan/polypyrrole (CS/PPy), was synthesized and linked with the Cr(VI)-reducing bacterial strain YL3 to treat Cr(VI)-polluted soil. The findings demonstrated that the synergistic application of strain YL3 and CS/PPy achieved the greatest reduction (99.6 %). During the remediation process, CS/PPy served as a mass-storage and sustained release agent in the soil, which initially decreased the toxic effects of high concentrations of Cr(VI) on strain YL3, thereby enhancing the Cr(VI) reduction efficiency of strain YL3. These combined effects significantly mitigated Cr(VI) stress in the soil and restored enzyme activities. Furthermore, wheat growth in the treated soil also significantly improved. High-throughput sequencing of the microorganisms in the treated soil revealed that CS/PPy was not only effective at removing Cr(VI) but also at preserving the original microbial diversity of the soil. This suggests that the combined treatment using strain YL3 and CS/PPy could rehabilitate Cr(VI)-contaminated soil, positioning CS/PPy as a promising composite material for future bioremediation efforts in Cr(VI)-contaminated soils.


Assuntos
Biodegradação Ambiental , Quitosana , Cromo , Microbacterium , Polímeros , Pirróis , Microbiologia do Solo , Poluentes do Solo , Poluentes do Solo/metabolismo , Cromo/metabolismo , Cromo/química , Quitosana/química , Polímeros/química , Polímeros/metabolismo , Pirróis/metabolismo , Pirróis/química , Microbacterium/metabolismo , Triticum/metabolismo
8.
Environ Sci Pollut Res Int ; 31(28): 41032-41045, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38842781

RESUMO

The problem of soil and water contamination caused by Cr(VI) discharged from the dyeing, electroplating, and metallurgical industries is becoming increasingly serious, posing a potentially great threat to the environment and public health. Therefore, it is crucial to develop a fast, efficient, and cost-effective adsorbent for remediating Cr-contaminated wastewater. In this work, MgAl-LDH/commercial-activated carbon nanocomposites (LDH-CACs) are prepared with hydrothermal. The effects of preparation and reaction conditions on the composite properties are first investigated, and then its adsorption behavior is thoroughly explored. Finally, a potential adsorption mechanism is proposed by several characterizations like SEM-EDS, XRD, FTIR, and XPS. The removal of Cr(VI) reaches 72.47% at optimal conditions, and the adsorption study demonstrates that LDH-CAC@1 has an extremely rapid adsorption rate and a maximum adsorption capacity of 116.7 mg/g. The primary removal mechanisms include adsorption-coupled reduction, ion exchange, surface precipitation, and electrostatic attraction. The reusability experiment illustrates that LDH-CAC@1 exhibits promising reusability. This study provides an effective adsorbent with a remarkably fast reaction, which has positive environmental significance for the treatment of Cr(VI) wastewater.


Assuntos
Carvão Vegetal , Cromo , Poluentes Químicos da Água , Adsorção , Cromo/química , Poluentes Químicos da Água/química , Carvão Vegetal/química , Nanocompostos/química , Purificação da Água/métodos , Águas Residuárias/química , Carbono/química
9.
Environ Sci Pollut Res Int ; 31(23): 33993-34009, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38696011

RESUMO

Water contamination by hexavalent chromium (Cr(VI)) seriously jeopardizes human health, which is a pressing environmental concern. Biochar-loaded green-synthesized nZVI, as a green and environmentally friendly material, can efficiently reduce Cr(VI) to Cr(III) while removing Cr(VI) from water. Therefore, in this study, an efficient green-modified biochar material (TP-nZVI/BC) was successfully prepared using tea polyphenol (TP) and sludge biochar (BC) using a low-cost and environmentally friendly green synthesis method. The preparation conditions of TP-nZVI/BC were optimized using response surface methodology (RSM), revealing that the dosage of tea polyphenols plays a crucial role in the removal performance (R2 = 1271.09), followed by reaction time and temperature. The quadratic regression model proved accurate. The optimal preparation conditions are as follows: tea polyphenols (TP) dosage at 48 g/L, reaction temperature at 75 ℃, and a reaction time of 3 h. TP-nZVI/BC removed Cr(VI) from water at a rate 7.6 times greater than BC. The pseudo-second-order kinetic model (R2 = 0.987) accurately describes the adsorption process, suggesting that chemical adsorption predominantly controls the removal process. The adsorption of Cr(VI) by TP-nZVI/BC can be well described by the Langmuir model, and the maximum adsorption capacity reached 105.65 mg/g. FTIR and XPS analyses before and after adsorption demonstrate that nZVI plays a crucial role in the reduction process of Cr(VI), and the synergistic effects of surface adsorption, reduction, and co-precipitation enhance Cr(VI) removal. In summary, using green-modified biochar for Cr(VI) removal is a feasible and promising method with significant potential.


Assuntos
Carvão Vegetal , Cromo , Poluentes Químicos da Água , Carvão Vegetal/química , Cromo/química , Poluentes Químicos da Água/química , Adsorção , Purificação da Água/métodos , Cinética , Química Verde
10.
Environ Sci Pollut Res Int ; 31(23): 34607-34621, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38705925

RESUMO

A series of ZnO decorated reduced graphene oxide (rGO) (ZnrGOx) with different doping ratios were synthesized by the alkaline hydrothermal method using graphene oxide (GO) and Zn(NO3)2·6H2O as precursors, and subsequently used for the adsorption study of Cr(VI) in water. The morphology, crystalline phase structure, and surface elemental properties of ZnrGOx composites were revealed by XRD, SEM, BET, FT-IR, and XPS characterizations. The results showed that ZnO nanoparticles can be clearly seen on the surface of layered rGO. Meanwhile, as the doping rate increased, the C = C double bonds were broken and more carboxylic acid groups formed in ZnrGOx. In addition, the ZnrGO0.1 composite had the most excellent adsorption performance and good stability, and reusability. The adsorption removal rate of Cr(VI) can reach 99%, and the maximum adsorption amount of Cr(VI) was 68.9655 mg/g in 3 h. The isothermal and kinetic model simulations showed that Cr(VI) adsorption on ZnrGO0.1 composite is a chemical adsorption process, spontaneous and endothermic. Based on the concentrations of different valence states of Cr in the solid and liquid phases, 40% of Cr(VI) was reduced to Cr(III) on the surface of ZnrGO0.1 composite. Moreover, the adsorption-reduction mechanisms of Cr(VI) on ZnrGO0.1 composite were further elucidated. The ZnrGO0.1 composite manifested great potential as an efficient adsorbent for Cr(VI) removal.


Assuntos
Cromo , Grafite , Poluentes Químicos da Água , Óxido de Zinco , Óxido de Zinco/química , Adsorção , Grafite/química , Cromo/química , Poluentes Químicos da Água/química , Cinética , Purificação da Água/métodos
11.
Molecules ; 29(10)2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38792069

RESUMO

A highly efficient low-cost adsorbent was prepared using raw and chemically modified cellulose isolated from sugarcane bagasse for decontamination of Cr(VI) from wastewater. First, cellulose pulp was isolated from sugarcane bagasse by subjecting it to acid hydrolysis, alkaline hydrolysis and bleaching with sodium chlorate (NaClO3). Then, the bleached cellulose pulp was chemically modified with acrylonitrile monomer in the presence Fenton's reagent (Fe+2/H2O2) to carry out grafting of acrylonitrile onto cellulose by atom transfer radical polymerization. The developed adsorbent (acrylonitrile grafted cellulose) was analyzed by X-ray diffraction analysis (XRD), scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FT-IR). Both raw cellulose and acrylonitrile grafted cellulose were used for chromium removal from wastewater. The effects of metal ion concentration, pH, adsorbent dose and time were studied, and their values were optimized. The optimum conditions for the adsorption of Cr(VI) onto raw and chemically modified cellulose were: metal ion concentration: 50 ppm, adsorbent dose: 1 g, pH: 6, and time: 60 min. The maximum efficiencies of 73% and 94% and adsorption capacities of 125.95 mg/g and 267.93 mg/g were achieved for raw and acrylonitrile grafted cellulose, respectively. High removal efficiency was achieved, owing to high surface area of 79.92 m2/g and functional active binding cites on grafted cellulose. Isotherm and kinetics studies show that the experimental data were fully fitted by the Freundlich isotherm model and pseudo first-order model. The adsorbent (acrylonitrile grafted cellulose) was regenerated using three different types of regenerating reagents and reused thirty times, and there was negligible decrease (19%) in removal efficiency after using it for 30 times. Hence, it is anticipated that acrylonitrile could be utilized as potential candidate material for commercial scale Cr(VI) removal from wastewater.


Assuntos
Acrilonitrila , Celulose , Cromo , Saccharum , Águas Residuárias , Poluentes Químicos da Água , Purificação da Água , Celulose/química , Cromo/isolamento & purificação , Cromo/química , Acrilonitrila/química , Saccharum/química , Águas Residuárias/química , Adsorção , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Concentração de Íons de Hidrogênio , Cinética , Espectroscopia de Infravermelho com Transformada de Fourier , Difração de Raios X
12.
Bioresour Technol ; 402: 130830, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38734264

RESUMO

In this study, the sorption properties of Cr(VI), As(III), and Pb(II) on chitosan-modified magnetic biochar (CMBC) derived from residues of Ligusticum chuanxiong Hort. were investigated. CMBC was found to be a valuable material for removing three heavy metals from water simultaneously. Kinetic analysis suggested Cr(VI), As(III), and Pb(II) were chemisorbed onto CMBC, while isotherm data conformed well to Langmuir model, the maximum adsorption capacity of CMBC was found to be 65.74 mg/g for Cr(VI), 49.32 mg/g for As(III), and 69.45 mg/g for Pb(II). Experiments, characterization, and density functional theory (DFT) calculations were employed to explore the mechanisms. Furthermore, CMBC demonstrated excellent removal rates of over 95% for Cr(VI), 99% for As(III) and Pb(II) from contaminated water bodies. This work shows that CMBC holds significant potential for wastewater treatment of heavy metals and provides an effective solution for the utilization of Chinese herb residues in environmental remediation.


Assuntos
Carvão Vegetal , Quitosana , Metais Pesados , Poluentes Químicos da Água , Quitosana/química , Carvão Vegetal/química , Adsorção , Poluentes Químicos da Água/química , Cinética , Purificação da Água/métodos , Cromo/química , Medicamentos de Ervas Chinesas/química
13.
J Hazard Mater ; 472: 134583, 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38749250

RESUMO

Iron-based materials such as nanoscale zerovalent iron (nZVI) are effective candidates to in situ remediate hexachromium (Cr(VI))-contaminated groundwater. The anaerobic bacteria could influence the remediation efficiency of Cr(VI) during its cotransport with nZVI in porous media. To address this issue, the present study investigated the adsorption and reduction of Cr(VI) during its cotransport with green tea (GT) modified nZVI (nZVI@GT) and iron sulfides (FeS and FeS2) in the presence of D. vulgaris or S. putrefaciens in water-saturated sand columns. Experimental results showed that the nZVI@GT preferred to heteroaggregate with FeS2 rather than FeS, forming nZVI@GT-FeS2 heteroaggregates. Although the presence of D. vulgaris further induced nZVI@GT-FeS2 heteroaggregates to form larger clusters, it pronouncedly improved the dissolution of FeS and FeS2 for more Cr(VI) reduction associated with lower Cr(VI) flux through sand. In contrast, S. putrefaciens could promote the dispersion of the heteroaggregates of nZVI@GT-FeS2 and the homoaggregates of nZVI@GT or FeS by adsorption on the extracellular polymeric substances, leading to the improved transport of Fe-based materials for a much higher Cr(VI) immobilization in sand media. Overall, our study provides the essential perspectives into a chem-biological remediation technique through the synergistic removal of Cr(VI) by nZVI@GT and FeS in contaminated groundwater. ENVIRONMENTAL IMPLICATION: The green-synthesized nano-zero-valent iron particles (nZVI@GT) using plant extracts (or iron sulfides) have been used for in situ remediation of Cr(VI) contaminated groundwater. Nevertheless, the removal of Cr(VI) (including Cr(VI) adsorption and Cr(III) generation) could be influenced by the anaerobic bacteria governing the transport of engineered nanoparticles in groundwater. This study aims to reveal the inherent mechanisms of D. vulgaris and S. putrefaciens governing the cotransport of nZVI@GT combined with FeS (or FeS2) to further influence the Cr(VI) removal in simulated complex groundwater media. Our findings provides a chemical and biological synergistic remediation strategy for nZVI@GT application in Cr(VI)-contaminated groundwater.


Assuntos
Cromo , Água Subterrânea , Ferro , Nanopartículas Metálicas , Poluentes Químicos da Água , Água Subterrânea/química , Poluentes Químicos da Água/química , Cromo/química , Ferro/química , Nanopartículas Metálicas/química , Sulfetos/química , Adsorção , Chá/química , Purificação da Água/métodos , Compostos Ferrosos
14.
J Hazard Mater ; 472: 134447, 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38692000

RESUMO

Sulfur-based denitrification is a promising technology for efficient nitrogen removal in low-carbon wastewater, while it is easily affected by toxic substances. This study revealed the inhibitory mechanism of Cr(VI) on thiosulfate-based denitrification, including bio-toxicity and bio-electron characteristics response. The activity of nitrite reductase (NIR) was more sensitive to Cr(VI) than that of nitrate reductase (NAR), and NIR was inhibited by 21.32 % and 19.86 % under 5 and 10 mg/L Cr(VI), resulting in 10.12 and 15.62 mg/L of NO2--N accumulation. The biofilm intercepted 36.57 % of chromium extracellularly by increasing 25.78 % of extracellular polymeric substances, thereby protecting microbes from bio-toxicity under 5 mg/L Cr(VI). However, it was unable to resist 20-30 mg/L of Cr(VI) bio-toxicity as 19.95 and 14.29 mg Cr/(g volatile suspended solids) invaded intracellularly, inducing the accumulation of reactive oxygen species by 165.98 % and 169.12 %, which triggered microbial oxidative-stress and damaged the cells. In terms of electron transfer, S2O32- oxidation was inhibited, and parts of electrons were redirected intracellularly to maintain microbial activity, resulting in insufficient electron donors. Meanwhile, the contents of flavin adenine dinucleotide and cytochrome c decreased under 5-30 mg/L Cr(VI), reducing the electron acquisition rate of denitrification. Thermomonas (the dominant genus) possessed denitrification and Cr(VI) resistance abilities, playing an important role in antioxidant stress and biofilm formation. ENVIRONMENTAL IMPLICATION: Sulfur-based denitrification (SBD) is a promising method for nitrate removal in low-carbon wastewater, while toxic heavy metals such as Cr(VI) negatively impair denitrification. This study elucidated Cr(VI) inhibitory mechanisms on SBD, including bio-toxicity response, bio-electron characteristics, and microbial community structure. Higher concentrations Cr(VI) led to intracellular invasion and oxidative stress, evidenced by ROS accumulation. Moreover, Cr(VI) disrupted electron flow by inhibiting thiosulfate oxidation and affecting electron acquisition by denitrifying enzymes. This study provided valuable insights into Cr(VI) toxicity, which is of great significance for improving wastewater treatment technologies and maintaining efficient and stable operation of SBD in the face of complex environmental challenges.


Assuntos
Biofilmes , Cromo , Desnitrificação , Enxofre , Cromo/toxicidade , Cromo/metabolismo , Cromo/química , Desnitrificação/efeitos dos fármacos , Enxofre/química , Enxofre/metabolismo , Biofilmes/efeitos dos fármacos , Poluentes Químicos da Água/toxicidade , Poluentes Químicos da Água/química , Poluentes Químicos da Água/metabolismo , Nitrito Redutases/metabolismo , Nitrato Redutase/metabolismo , Águas Residuárias/química , Espécies Reativas de Oxigênio/metabolismo , Bactérias/metabolismo , Bactérias/efeitos dos fármacos , Elétrons , Estresse Oxidativo/efeitos dos fármacos
15.
Environ Sci Technol ; 58(19): 8501-8509, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38696244

RESUMO

Iron/chromium hydroxide coprecipitation controls the fate and transport of toxic chromium (Cr) in many natural and engineered systems. Organic coatings on soil and engineered surfaces are ubiquitous; however, mechanistic controls of these organic coatings over Fe/Cr hydroxide coprecipitation are poorly understood. Here, Fe/Cr hydroxide coprecipitation was conducted on model organic coatings of humic acid (HA), sodium alginate (SA), and bovine serum albumin (BSA). The organics bonded with SiO2 through ligand exchange with carboxyl (-COOH), and the adsorbed amounts and pKa values of -COOH controlled surface charges of coatings. The adsorbed organic films also had different complexation capacities with Fe/Cr ions and Fe/Cr hydroxide particles, resulting in significant differences in both the amount (on HA > SA(-COOH) ≫ BSA(-NH2)) and composition (Cr/Fe molar ratio: on BSA(-NH2) ≫ HA > SA(-COOH)) of heterogeneous precipitates. Negatively charged -COOH attracted more Fe ions and oligomers of hydrolyzed Fe/Cr species and subsequently promoted heterogeneous precipitation of Fe/Cr hydroxide nanoparticles. Organic coatings containing -NH2 were positively charged at acidic pH because of the high pKa value of the functional group, limiting cation adsorption and formation of coprecipitates. Meanwhile, the higher local pH near the -NH2 coatings promoted the formation of Cr(OH)3. This study advances fundamental understanding of heterogeneous Fe/Cr hydroxide coprecipitation on organics, which is essential for successful Cr remediation and removal in both natural and engineered settings, as well as the synthesis of Cr-doped iron (oxy)hydroxides for material applications.


Assuntos
Cromo , Hidróxidos , Ferro , Hidróxidos/química , Ferro/química , Cromo/química , Soroalbumina Bovina/química , Adsorção , Substâncias Húmicas , Água/química , Precipitação Química , Alginatos/química
16.
Molecules ; 29(9)2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38731488

RESUMO

This study synthesized a novel oat ß-glucan (OBG)-Cr(III) complex (OBG-Cr(III)) and explored its structure, inhibitory effects on α-amylase and α-glucosidase, and hypoglycemic activities and mechanism in vitro using an insulin-resistant HepG2 (IR-HepG2) cell model. The Cr(III) content in the complex was found to be 10.87%. The molecular weight of OBG-Cr(III) was determined to be 7.736 × 104 Da with chromium ions binding to the hydroxyl groups of OBG. This binding resulted in the increased asymmetry and altered spatial conformation of the complex along with significant changes in morphology and crystallinity. Our findings demonstrated that OBG-Cr(III) exhibited inhibitory effects on α-amylase and α-glucosidase. Furthermore, OBG-Cr(III) enhanced the insulin sensitivity of IR-HepG2 cells, promoting glucose uptake and metabolism more efficiently than OBG alone. The underlying mechanism of its hypoglycemic effect involved the modulation of the c-Cbl/PI3K/AKT/GLUT4 signaling pathway, as revealed by Western blot analysis. This research not only broadened the applications of OBG but also positioned OBG-Cr(III) as a promising Cr(III) supplement with enhanced hypoglycemic benefits.


Assuntos
Cromo , Hipoglicemiantes , alfa-Glucosidases , beta-Glucanas , Humanos , Cromo/química , Cromo/farmacologia , Hipoglicemiantes/farmacologia , Hipoglicemiantes/química , Hipoglicemiantes/síntese química , beta-Glucanas/química , beta-Glucanas/farmacologia , Células Hep G2 , alfa-Glucosidases/metabolismo , alfa-Amilases/antagonistas & inibidores , alfa-Amilases/metabolismo , Resistência à Insulina , Glucose/metabolismo , Transdução de Sinais/efeitos dos fármacos , Transportador de Glucose Tipo 4/metabolismo , Avena/química , Inibidores de Glicosídeo Hidrolases/farmacologia , Inibidores de Glicosídeo Hidrolases/química , Complexos de Coordenação/química , Complexos de Coordenação/farmacologia , Complexos de Coordenação/síntese química
17.
Bioresour Technol ; 401: 130761, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38692370

RESUMO

Cr (VI) is a common heavy metal pollutant in electroplating wastewater. This study introduces the liquid-phase product from the hydrothermal reaction of coffee grounds (CGHCL) into the synthesis process of molybdenum disulfide, assisting in the fabrication of an intercalated, expanded core-shell structured molybdenum disulfide adsorbent (C-MoS2), designed for the adsorption and reduction of Cr (VI) from electroplating wastewater. The addition of CGHCL significantly enhances the adsorption performance of MoS2. Furthermore, C-MoS2 exhibits exceedingly high removal efficiency and excellent regenerative capability for Cr (VI)-containing electroplating wastewater. The core-shell structure effectively minimizes molybdenum leaching to the greatest extent, while the oleophobic interface is unaffected by oily substances in water, and the expanded interlayer structure ensures the long-term stability of C-MoS2 in air (90 days). This study provides a viable pathway for the resource utilization of biomass and the application of molybdenum disulfide-based materials in wastewater treatment.


Assuntos
Biomassa , Cromo , Dissulfetos , Molibdênio , Águas Residuárias , Purificação da Água , Molibdênio/química , Dissulfetos/química , Adsorção , Águas Residuárias/química , Purificação da Água/métodos , Cromo/química , Galvanoplastia , Poluentes Químicos da Água , Soluções
18.
Environ Res ; 252(Pt 3): 119043, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38692422

RESUMO

It is of great significance to establish an effective method for removing Cr(VI) from wastewater. Herein, Fe-doped g-C3N4 (namely Fe-g-C3N4-2) was synthesized and then employed as photocatalyst to conduct the test of Cr(VI) reduction. Notably, the embedding of Fe ion in g-C3N4 can offer the Fe2+/Fe3+ redox couples, so reducing the interfacial resistance of charge transfer and suppressing the recombination of photogenerated electrons and holes. The impurity energy levels will form in g-C3N4 after the introduction of Fe ion, thereby boosting the light absorption capacity of catalyst. Thus, Fe-g-C3N4-2 showed good performance in photocatalytic Cr(VI) reduction, and the reduction efficiency of Cr(VI) can reach 39.9% within 40 min. Different with many previous studies, current work unexpectedly found that the addition of p-benzoquinone (BQ) can promote the Cr(VI) reduction, and the reduction efficiency of Cr(VI) over Fe-g-C3N4-2 was as high as 93.2% in the presence of BQ (1.5 mM). Further analyses showed that BQ can be reduced to hydroquinone (HQ) by photogenerated electrons, and UV light can also directly induce BQ to generate HQ by using H2O as the hydrogen donor. The HQ with reducing ability can accelerate the Cr(VI) reduction. In short, current work shared some novel insights into photocatalytic Cr(VI) reduction in the presence of BQ. Future research should consider possible reactions between photogenerated electrons and BQ. For the UV-induced photocatalysis, the suitability of BQ as the scavenger of O2•‒ must be given carefully consideration.


Assuntos
Benzoquinonas , Cromo , Ferro , Oxirredução , Benzoquinonas/química , Cromo/química , Catálise , Ferro/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/efeitos da radiação , Processos Fotoquímicos , Compostos de Nitrogênio/química , Compostos de Nitrogênio/efeitos da radiação , Grafite
19.
Environ Res ; 252(Pt 4): 119065, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38723990

RESUMO

The present research study combines chitin from shrimp waste with the oxide-rich metakaolin. Metakaolin is a blend of mixed oxides rich in silica and alumina with good adsorbent properties. The chitin@metakaolin (CHt@M.K.) composite was synthesized and characterized using FTIR, SEM, TGA, XRD and XPS techniques. Cr(VI) removal studies were compared for chitin and CHt@M.K. through adsorption. It was found that the adsorption capacity of CHt@M.K. is 278.88 mg/g, almost double that of chitin, at pH 5.0 in just 120 min of adsorption. Isotherm models like Langmuir, Freundlich, Temkin and Dubinin-Radushkevich were investigated to comprehend the adsorption process. It was revealed that Langmuir adsorption isotherm is most suitable to elucidate Cr(VI) adsorption on CHt@M.K. The adsorption kinetics indicate that pseudo first order was followed, indicating that the physisorption was the process that limited the sorption process rate. The positive enthalpy change (20.23 kJ/mol) and positive entropy change (0.083 kJ/mol K) showed that the adsorption process was endothermic and more random at the solid-liquid interface. The negative free energy change over entire temperature range was an indicator of spontaneity of the process. Apart from all these, the non-covalent interactions between Cr(VI) and composite were explained by quantum calculations based models.


Assuntos
Exoesqueleto , Quitina , Cromo , Poluentes Químicos da Água , Quitina/química , Animais , Cromo/química , Adsorção , Poluentes Químicos da Água/química , Exoesqueleto/química , Braquiúros/química , Cinética
20.
Chemosphere ; 359: 142304, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38734253

RESUMO

Toxic organic and heavy metal contaminants commonly exist in industrial waste stream(s) and treatment is of great challenge. In this study, a dielectric barrier discharge (DBD) non-thermal plasma technology was employed for the simultaneous treatment of two important contaminants, chloramphenicol (CAP) and Cr(VI) in an aqueous solution through redox transformations. More than 70% of CAP and 20% of TOC were degraded in 60 min, while Cr(VI) was completely removed in 10 min. The hydroxyl radicals were the main active species for the degradation. Meanwhile, the consumption of hydroxyl radicals was beneficial to the reduction of Cr(VI). The synergistic effect was investigated between CAP degradation and Cr(VI) reduction. The reduction of Cr(VI) would be enhanced in the presence of CAP with a low concentration and could be inhibited under a high concentration, because part of hydroxyl radicals could be consumed by the low-concentration CAP and the obtained intermediates with a higher kinetic rate. However, CAP with a high concentration could react with such reductive species as eaq- and •H, which could compete with Cr(VI) and inhibit the reduction. In addition, the presence of Cr(VI) enhanced the degradation and mineralization of CAP; the study of obtained intermediates indicated that the presence of Cr(VI) changed the degradation path of CAP as Cr(VI) would react with reductive species, enhance the generation of hydroxyl radicals, and cause more hydroxylation reactions. Moreover, the mechanism for the simultaneous redox transformations of CAP and Cr(VI) was illustrated. This study indicates that the DBD non-thermal plasma technology can be one of better solutions for simultaneous elimination of heavy metal and organic contaminants in aquatic environments.


Assuntos
Cloranfenicol , Cromo , Oxirredução , Poluentes Químicos da Água , Cloranfenicol/química , Cromo/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Gases em Plasma/química , Radical Hidroxila/química , Eliminação de Resíduos Líquidos/métodos
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