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1.
J Environ Sci (China) ; 147: 714-725, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39003084

RESUMO

In this study, an efficient stabilizer material for cadmium (Cd2+) treatment was successfully prepared by simply co-milling olivine with magnesite. Several analytical methods including XRD, TEM, SEM and FTIR, combined with theoretical calculations (DFT), were used to investigate mechanochemical interfacial reaction between two minerals, and the reaction mechanism of Cd removal, with ion exchange between Cd2+ and Mg2+ as the main pathway. A fixation capacity of Cd2+ as high as 270.61 mg/g, much higher than that of the pristine minerals and even the individual/physical mixture of milled olivine and magnesite, has been obtained at optimized conditions, with a neutral pH value of the solution after treatment to allow its direct discharge. The as-proposed Mg-based stabilizer with various advantages such as cost benefits, green feature etc., will boosts the utilization efficiency of natural minerals over the elaborately prepared adsorbents.


Assuntos
Cádmio , Compostos de Ferro , Compostos de Magnésio , Silicatos , Poluentes Químicos da Água , Cádmio/química , Poluentes Químicos da Água/química , Compostos de Magnésio/química , Silicatos/química , Compostos de Ferro/química , Adsorção , Modelos Químicos , Purificação da Água/métodos
2.
Environ Sci Pollut Res Int ; 31(33): 45862-45874, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38980478

RESUMO

Anaerobic digestion of waste activated sludge (WAS) was one of the directions of sludge treatment, but how to effectively improve the production of methane as a resource product of anaerobic digestion of sludge still needs further research. The study examined how the combination of potassium ferrate (PF) and thermal hydrolysis (TH) pretreatment affected methane production from sludge. The results demonstrated a positive synergistic effect on methane production with PF-TH pretreatment. Specifically, by employing a 0.05 g/g TSS (total suspended solids) PF in conjunction with TH at 80 °C for 30 min, the methane yield increased from 170.66 ± 0.92 to 232.73 ± 2.21 mL/g VSS (volatile suspended solids). The co-pretreatment of PF and TH has been substantiated by mechanism studies to effectively enhance the disintegration and biodegradability of sludge. Additionally, the variation of microbial community revealed an enrichment of active microorganisms associated with anaerobic digestion after treated with PF + TH, resulting in a total abundance increase from 11.87 to 20.45% in the PF + TH group.


Assuntos
Metano , Compostos de Potássio , Esgotos , Eliminação de Resíduos Líquidos , Hidrólise , Eliminação de Resíduos Líquidos/métodos , Compostos de Ferro , Anaerobiose , Biodegradação Ambiental
3.
Environ Sci Technol ; 58(28): 12664-12673, 2024 Jul 16.
Artigo em Inglês | MEDLINE | ID: mdl-38953777

RESUMO

Investigating the fate of persistent organic pollutants in water distribution systems (WDSs) is of great significance for preventing human health risks. The role of iron corrosion scales in the migration and transformation of organics in such systems remains unclear. Herein, we determined that hydroxyl (•OH), chlorine, and chlorine oxide radicals are generated by Fenton-like reactions due to the coexistence of oxygen vacancy-related Fe(II) on goethite (a major constituent of iron corrosion scales) and hypochlorous acid (HClO, the main reactive chlorine species of residual chlorine at pH ∼ 7.0). •OH contributed mostly to the decomposition of atrazine (ATZ, model compound) more than other radicals, producing a series of relatively low-toxicity small molecular intermediates. A simplified kinetic model consisting of mass transfer of ATZ and HClO, •OH generation, and ATZ oxidation by •OH on the goethite surface was developed to simulate iron corrosion scale-triggered residual chlorine oxidation of organic compounds in a WDS. The model was validated by comparing the fitting results to the experimental data. Moreover, the model was comprehensively applicable to cases in which various inorganic ions (Ca2+, Na+, HCO3-, and SO42-) and natural organic matter were present. With further optimization, the model may be employed to predict the migration and accumulation of persistent organic pollutants under real environmental conditions in the WDSs.


Assuntos
Poluentes Químicos da Água , Cinética , Radicais Livres/química , Poluentes Químicos da Água/química , Oxirredução , Ferro/química , Compostos de Ferro/química , Minerais/química
4.
Environ Sci Technol ; 58(26): 11748-11759, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38912726

RESUMO

Despite extensive study, geochemical modeling often fails to accurately predict lead (Pb) immobilization in environmental samples. This study employs the Charge Distribution MUlti-SIte Complexation (CD-MUSIC) model, X-ray absorption fine structure (XAFS), and density functional theory (DFT) to investigate mechanisms of phosphate (PO4) induced Pb immobilization on metal (hydr)oxides. The results reveal that PO4 mainly enhances bidentate-adsorbed Pb on goethite via electrostatic synergy at low PO4 concentrations. At relatively low pH (below 5.5) and elevated PO4 concentrations, the formation of the monodentate-O-sharing Pb-PO4 ternary structure on goethite becomes important. Precipitation of hydropyromorphite (Pb5(PO4)3OH) occurs at high pH and high concentrations of Pb and PO4, with an optimized log Ksp value of -82.02. The adjustment of log Ksp compared to that in the bulk solution allows for quantification of the overall Pb-PO4 precipitation enhanced by goethite. The CD-MUSIC model parameters for both the bidentate Pb complex and the monodentate-O-sharing Pb-PO4 ternary complex were optimized. The modeling results and parameters are further validated and specified with XAFS analysis and DFT calculations. This study provides quantitative molecular-level insights into the contributions of electrostatic enhancement, ternary complexation, and precipitation to phosphate-induced Pb immobilization on oxides, which will be helpful in resolving controversies regarding Pb distribution in environmental samples.


Assuntos
Chumbo , Fosfatos , Chumbo/química , Fosfatos/química , Compostos de Ferro/química , Minerais/química , Concentração de Íons de Hidrogênio , Adsorção
5.
Sci Total Environ ; 945: 174017, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-38897455

RESUMO

Schwertmannite (Sch), a typical Fe(III)-oxyhydroxysulphate mineral, is the precipitation reservoir of toxic elements in acid mine drainage (AMD). Acid-tolerant microbes in AMD can participate in the microbe-mediated transformation of Sch, while Sch affects the physiological characteristics of these acid-tolerant microbes. Based on our discovery of algae and Sch enrichment in a contaminated acid mine pit lake, we predicted the interaction between algae and Sch when incubated together. The acid-tolerant alga Graesiella sp. MA1 was isolated from the pit-lake surface water of an acidic mine and incubated with different contents of Sch. Sch was detected as the main product at the end of 81 d; however, there was a weak transformation. The presence of dissolved Fe(II) could be largely attributed to the photoreduction dissolution of Sch, which was promoted by Graesiella sp. MA1. The adaptation and growth phases of Graesiella sp. MA1 differed under Sch stress. The photosynthetic and metabolic activities increased and decreased at the adaptation and growth phases, respectively. The MDA contents and antioxidant activity of SOD, APX, and GSH in algal cells gradually enhanced as the Sch treatment content increased, indicating a defense strategy of Graesiella sp. MA1. Metabolomic analysis revealed that Sch affected the expression of significant differential metabolites in Graesiella sp. MA1. Organic carboxylic acid substances were essentially up-regulated in response to Sch stress. They were abundant in the medium-Sch system with the highest Fe(III) reduction, capable of complexing Fe(III), and underwent photochemical reactions via photo-induced charge transfer. The significant up-regulation of reducing sugars revealed the high energy requirement of Graesiella sp. MA1 under Sch stress. And first enriched KEGG pathway demonstrated the importance of sugar metabolism in Graesiella sp. MA1. Data acquired in this study provide novel insights into extreme acid stress adaptation of acid-tolerant algae and Sch, contributing to furthering understanding of AMD environments.


Assuntos
Compostos de Ferro , Compostos de Ferro/metabolismo , Poluentes Químicos da Água , Mineração , Lagos/microbiologia
6.
Sci Total Environ ; 946: 174275, 2024 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-38936727

RESUMO

Schwertmannite (Sch) is found in environments abundant in iron and sulfate. Microorganisms that utilize iron or sulfate can induce the phase transition of Schwertmannite, consequently leading to the redistribution of coexisting pollutants. However, the impact of the molar ratio of sulfate to iron (S/Fe) on the microbial-mediated transformation of Schwertmannite and its implications for the fate of cadmium (Cd) have not been elucidated. In this study, we examined how S/Fe influenced mineral transformation and the fate of Cd during microbial reduction of Cd-loaded Schwertmannite by Desulfovibrio vulgaris. Our findings revealed that an increase in the S/Fe ratio facilitated sulfate-reducing bacteria (SRB) in mitigating the toxicity of Cd, thereby expediting the generation of sulfide (S(-II)) and subsequently triggering mineral phase transformation. As the S/Fe ratio increased, the predominant minerals in the system transitioned from prismatic-cluster vivianite to rose-shaped mackinawite. The Cd phase and distribution underwent corresponding alterations. Cd primarily existed in its oxidizable state, with its distribution being directly linked not only to FeS content but also showing a robust correlation with phosphorus. The coexistence of vivianite and FeS minerals proved to be more favorable for Cd immobilization. These findings have significant implications for understanding the biogeochemistry of iron (oxyhydr)oxides and Cd fate in anaerobic environments.


Assuntos
Cádmio , Sulfatos , Cádmio/metabolismo , Sulfatos/metabolismo , Compostos de Ferro/metabolismo , Desulfovibrio vulgaris/metabolismo , Oxirredução , Ferro/metabolismo , Biodegradação Ambiental , Sulfetos/metabolismo
7.
Environ Res ; 257: 119392, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38857857

RESUMO

Iron (Fe) and manganese (Mn) oxides can be used to remediate Cd-polluted soils due to their excellent performance in heavy metal adsorption. However, their remediation capability is rather limited, and a higher content of available Mn and Fe in soils can reduce Cd accumulation in wheat plants due to the competitive absorption effect. In this study, goethite and cryptomelane were first respectively used to immobilize Cd in Cd-polluted weakly alkaline soils, and sodium citrate was then added to increase the content of available Mn and Fe content for further reduction of wheat Cd absorption. In the first season, the content of soil-available Cd and Cd in wheat plants significantly decreased when cryptomelane, goethite and their mixture were used as the remediation agents. Cryptomelane showed a better remediation effect, which could be attributed to its higher adsorption performance. The grain Cd content could be decreased from 0.35 mg kg-1 to 0.25 mg kg-1 when the content of cryptomelane was controlled at 0.5%. In the second season, when sodium citrate at 20 mmol kg-1 was further added to the soils with 0.5% cryptomelane treatment in the first season, the content of soil available Cd was increased by 14.8%, and the available Mn content was increased by 19.5%, leading to a lower Cd content in wheat grains (0.16 mg kg-1) probably due to the competitive absorption. This work provides a new strategy for the remediation of slightly Cd-polluted arable soils with safe and high-quality production of wheat.


Assuntos
Cádmio , Compostos de Manganês , Óxidos , Poluentes do Solo , Triticum , Triticum/metabolismo , Triticum/química , Cádmio/metabolismo , Cádmio/análise , Poluentes do Solo/metabolismo , Poluentes do Solo/análise , Compostos de Manganês/química , Compostos de Manganês/metabolismo , Óxidos/química , Recuperação e Remediação Ambiental/métodos , Solo/química , Ácido Cítrico/metabolismo , Adsorção , Minerais/metabolismo , Minerais/química , Compostos de Ferro/metabolismo , Compostos de Ferro/química
8.
J Water Health ; 22(6): 1102-1110, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38935460

RESUMO

Ferrate (Fe(VI): HFeO4- /FeO42-), a potent oxidant, has been investigated as an alternative chemical disinfectant in water treatment due to its reduced production of disinfection by-products. In this study, we assessed the disinfecting ability of potassium ferrate against a variety of microorganisms, including waterborne pathogens, under varying pH and water temperature conditions. We presented CT values, a metric of ferrate concentrations (C) and contact time (T), to quantify microbial inactivation rates. Among the tested microorganisms, human adenovirus was the least resistant to ferrate, followed by waterborne bacteria such as Escherichia coli and Vibrio cholerae, and finally, the protozoan parasite Giardia duodenalis. We further investigated the impact of two pH values (7 and 8) and two temperatures (5 and 25 °C) on microbial inactivation rates, observing that inactivation rates increased with lower pH and higher temperature. In addition to showcasing ferrate's capacity to effectively inactivate a range of the tested microorganisms, we offer a ferrate CT table to facilitate the comparison of the effectiveness of various disinfection methods.


Assuntos
Desinfetantes , Giardia lamblia , Temperatura , Concentração de Íons de Hidrogênio , Desinfetantes/farmacologia , Giardia lamblia/efeitos dos fármacos , Adenovírus Humanos/efeitos dos fármacos , Compostos de Potássio/farmacologia , Compostos de Potássio/química , Microbiologia da Água , Desinfecção/métodos , Purificação da Água/métodos , Compostos de Ferro/farmacologia , Compostos de Ferro/química , Humanos , Escherichia coli/efeitos dos fármacos
9.
Ecotoxicol Environ Saf ; 281: 116570, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38896902

RESUMO

Rice is one of the most important staple food crops; however, it is prone to cadmium (Cd) accumulation, which has negative health effects. Therefore, methods to reduce Cd uptake by rice are necessary. At present, there is limited research on the effects of co-application of silicon (Si) and goethite in mitigating Cd stress in rice. Furthermore, the specific mechanisms underlying the effects of their combined application on iron plaque formation in rice roots remain unclear. Therefore, this study analyzed the effects of the combined application of Si and goethite on the biomass, physiological stress indicators, Cd concentration, and iron plaques of rice using hydroponic experiments. The results revealed that co-treatment with both Si and goethite increased the plant height and dry weight, superoxide dismutase and catalase activities, photosynthetic pigment concentration, and root activity. Moreover, this treatment decreased the malondialdehyde concentration, repaired epidermal cells, reduced the Cd concentration in the roots by 57.2 %, and increased the number of iron plaques and Cd concentration by 150.9 % and 266.2 % in the amorphous and crystalline fractions, respectively. The Cd/Fe ratio in amorphous iron plaques also increased. Our findings suggest that goethite serves as a raw material for iron plaque formation, while Si enhances the oxidation capacity of rice roots. The application of a combination of Si and goethite increases the quantity and quality of iron plaques, enhancing its Cd fixation capacity. This study provides theoretical evidence for the effective inhibition of Cd uptake by iron plaques in rice, providing insights into methods for the remediation of Cd contamination.


Assuntos
Cádmio , Compostos de Ferro , Ferro , Minerais , Oryza , Raízes de Plantas , Silício , Poluentes do Solo , Oryza/efeitos dos fármacos , Oryza/crescimento & desenvolvimento , Cádmio/toxicidade , Silício/farmacologia , Poluentes do Solo/toxicidade , Raízes de Plantas/efeitos dos fármacos , Estresse Fisiológico/efeitos dos fármacos , Superóxido Dismutase/metabolismo , Malondialdeído/metabolismo , Biomassa
10.
J Environ Sci (China) ; 145: 180-192, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-38844318

RESUMO

A pilot-scale filtration system was adopted to prepare filter media with catalytic activity to remove manganese (Mn2+) and ammonium (NH4+-N). Three different combinations of oxidants (KMnO4 and K2FeO4) and reductants (MnSO4 and FeCl2) were used during the start-up period. Filter R3 started up by KMnO4 and FeCl2 (Mn7+→MnOx) exhibited excellent catalytic property, and the NH4+-N and Mn2+ removal efficiency reached over 80% on the 10th and 35th days, respectively. Filter R1 started up by K2FeO4 and MnSO4 (MnOx←Mn2+) exhibited the worst catalytic property. Filter R2 started up by KMnO4 and MnSO4 (Mn7+→MnOx←Mn2+) were in between. According to Zeta potential results, the Mn-based oxides (MnOx) formed by Mn7+→MnOx performed the highest pHIEP and pHPZC. The higher the pHIEP and pHPZC, the more unfavorable the cation adsorption. However, it was inconsistent with its excellent Mn2+ and NH4+-N removal abilities, implying that catalytic oxidation played a key role. Combined with XRD and XPS analysis, the results showed that the MnOx produced by the reduction of KMnO4 showed early formation of buserite crystals, high degree of amorphous, high content of Mn3+ and lattice oxygen with the higher activity to form defects. The above results showed that MnOx produced by the reduction of KMnO4 was more conducive to the formation of active species for catalytic oxidation of NH4+-N and Mn2+ removal. This study provides new insights on the formation mechanisms of the active MnOx that could catalytic oxidation of NH4+-N and Mn2+.


Assuntos
Compostos de Amônio , Filtração , Manganês , Óxidos , Manganês/química , Óxidos/química , Compostos de Amônio/química , Filtração/métodos , Poluentes Químicos da Água/química , Permanganato de Potássio/química , Compostos de Manganês/química , Oxirredução , Eliminação de Resíduos Líquidos/métodos , Compostos de Potássio/química , Adsorção , Compostos Férricos/química , Compostos de Ferro
11.
Water Res ; 258: 121800, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38796909

RESUMO

Iron (hydr)oxides are abundant in surface environment, and actively participate in the transformation of organic pollutants due to their large specific surface areas and redox activity. This work investigated the transformation of tetracycline (TC) in the presence of three common iron (hydr)oxides, hematite (Hem), goethite (Goe), and ferrihydrite (Fh), under simulated sunlight irradiation. These iron (hydr)oxides exhibited photoactivity and facilitated the transformation of TC with the initial phototransformation rates decreasing in the order of: Hem > Fh > Goe. The linear correlation between TC removal efficiency and the yield of HO• suggests that HO• dominated TC transformation. The HO• was produced by UV-induced decomposition of self-generated H2O2 and surface Fe2+-triggered photo-Fenton reaction. The experimental results indicate that the generation of HO• was controlled by H2O2, while surface Fe2+ was in excess. Sunlight-driven H2O2 production in the presence of the highly crystalline Hem and Goe occurred through a one-step two-electron reduction pathway, while the process was contributed by both O2-induced Fe2+ oxidation and direct reduction of O2 by electrons on the conduction band in the presence of the poorly crystalline Fh. These findings demonstrate that sunlight may significantly accelerate the degradation of organic pollutants in the presence of iron (hydr)oxides.


Assuntos
Compostos Férricos , Peróxido de Hidrogênio , Luz Solar , Tetraciclina , Peróxido de Hidrogênio/química , Compostos Férricos/química , Tetraciclina/química , Compostos de Ferro/química , Oxirredução , Minerais/química , Poluentes Químicos da Água/química , Ferro/química
12.
Chemosphere ; 359: 142351, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38761821

RESUMO

Iron (hydr)oxides and humic acid (HA) are important active components in soils and usually coexist in the environment. The effects of HA on the adsorption and subsequent immobilization of phosphate on iron (hydr)oxide surface are of great importance in studies of soil fertility and eutrophication. In this study, two types of goethite with different particle sizes were prepared to investigate the phosphate adsorption behaviors and complexation mechanisms in the absence or presence of HA by combining multiple characterization and modeling studies. The adsorption capacity of micro- (M-Goe) and nano-sized goethite (N-Goe) for phosphate was 2.02 and 2.04 µmol/m2, which decreased by ∼25% and ∼45% in the presence of 100 and 200 mg/L HA, respectively. Moreover, an increase in equilibrium phosphate concentration significantly decreased the adsorption amount of goethite for HA. Charge distribution-multisite surface complexation (CD-MUSIC) and natural organic matter-charge distribution (NOM-CD) modeling identified five phosphate complexes and their corresponding affinity constants (logKP). Among these phosphate complexes, FeOPO2OH, (FeO)2PO2, and (FeO)2POOH species were predominant complexes on the surface of both M-Goe and N-Goe across a wide range of pH and initial phosphate concentrations. The presence of HA had little effect on the coordination mode and logKP of phosphate on goethite surface. These results and the obtained model parameters shed new lights on the interfacial reactivity of phosphate at the goethite-water interface in the presence of HA, and may facilitate further prediction of the environmental fate of phosphate in soils and sediments.


Assuntos
Substâncias Húmicas , Compostos de Ferro , Minerais , Fosfatos , Compostos de Ferro/química , Minerais/química , Fosfatos/química , Adsorção , Solo/química , Modelos Químicos , Poluentes do Solo/química , Poluentes do Solo/análise , Compostos Férricos/química
13.
Chemosphere ; 358: 142195, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38692368

RESUMO

Due to the anthropogenic increase of atmospheric CO2 emissions, humanity is facing the negative effects of rapid global climate change. Both active emission reduction and carbon dioxide removal (CDR) technologies are needed to meet the Paris Agreement and limit global warming to 1.5 °C by 2050. One promising CDR approach is coastal enhanced weathering (CEW), which involves the placement of sand composed of (ultra)mafic minerals like olivine in coastal zones. Although the large-scale placement of olivine sand could beneficially impact the planet through the consumption of atmospheric CO2 and reduction in ocean acidification, it may also have physical and geochemical impacts on benthic communities. The dissolution of olivine can release dissolved constituents such as trace metals that may affect marine organisms. Here we tested acute and chronic responses of marine invertebrates to olivine sand exposure, as well as examined metal accumulation in invertebrate tissue resulting from olivine dissolution. Two different ecotoxicological experiments were performed on a range of benthic marine invertebrates (amphipod, polychaete, bivalve). The first experiment included acute and chronic survival and growth tests (10 and 20 days, respectively) of olivine exposure while the second had longer (28 day) exposures to measure chronic survival and bioaccumulation of trace metals (e.g. Ni, Cr, Co) released during olivine sand dissolution. Across all fauna we observed no negative effects on acute survival or chronic growth resulting solely from olivine exposure. However, over 28 days of exposure, the bent-nosed clam Macoma nasuta experienced reduced burrowing and accumulated 4.2 ± 0.7 µg g ww-1 of Ni while the polychaete Alitta virens accumulated 3.5 ± 0.9 µg g ww-1 of Ni. No significant accumulation of any other metals was observed. Future work should include longer-term laboratory studies as well as CEW field studies to validate these findings under real-world scenarios.


Assuntos
Organismos Aquáticos , Compostos de Ferro , Compostos de Magnésio , Poluentes Químicos da Água , Animais , Poluentes Químicos da Água/metabolismo , Organismos Aquáticos/metabolismo , Organismos Aquáticos/efeitos dos fármacos , Compostos de Magnésio/química , Compostos de Ferro/química , Bioacumulação , Metais/metabolismo , Silicatos , Invertebrados/efeitos dos fármacos , Invertebrados/metabolismo , Dióxido de Silício/química , Poliquetos/metabolismo , Poliquetos/efeitos dos fármacos , Poliquetos/fisiologia , Bivalves/metabolismo , Bivalves/efeitos dos fármacos
14.
J Colloid Interface Sci ; 669: 64-74, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38705113

RESUMO

The intricate organization of goethite nanorods within a silica-rich matrix makes limpet teeth the strongest known natural material. However, the mineralization pathway of goethite in organisms under ambient conditions remains elusive. Here, by investigating the multi-level structure of limpet teeth at different growth stages, it is revealed that the growth of goethite crystals proceeds by the attachment of amorphous nanoparticles, a nonclassical crystallization pathway widely observed during the formation of calcium-based biominerals. Importantly, these nanoparticles contain a high amount of silica, which is gradually expelled during the growth of goethite. Moreover, in mature teeth of limpet, the content of silica correlates with the size of goethite crystals, where smaller goethite crystals are densely packed in the leading part with higher content of silica. Correspondingly, the leading part exhibits higher hardness and elastic modulus. Thus, this study not only reveals the nonclassical crystallization pathway of goethite nanorods in limpet teeth, but also highlights the critical roles of silica in controlling the hierarchical structure and the mechanical properties of limpet teeth, thus providing inspirations for fabricating biomimetic materials with excellent properties.


Assuntos
Cristalização , Compostos de Ferro , Minerais , Nanopartículas , Nanotubos , Dióxido de Silício , Dióxido de Silício/química , Minerais/química , Nanotubos/química , Compostos de Ferro/química , Nanopartículas/química , Animais , Dente/química , Gastrópodes/química , Tamanho da Partícula
15.
J Environ Sci (China) ; 143: 1-11, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38644008

RESUMO

Potential health risks related to environmental endocrine disruptors (EEDs) have aroused research hotspots at the forefront of water treatment technologies. Herein, nitrogen-doped titanium dioxide/schwertmannite nanocomposites (N-TiO2/SCH) have been successfully developed as heterogeneous catalysts for the degradation of typical EEDs via photo-Fenton processes. Due to the sustainable Fe(III)/Fe(II) conversion induced by photoelectrons, as-prepared N-TiO2/SCH nanocomposites exhibit much enhanced efficiency for the degradation of bisphenol A (BPA; ca. 100% within 60 min under visible irradiation) in a wide pH range of 3.0-7.8, which is significantly higher than that of the pristine schwertmannite (ca. 74.5%) or N-TiO2 (ca. 10.8%). In this photo-Fenton system, the efficient degradation of BPA is mainly attributed to the oxidation by hydroxyl radical (•OH) and singlet oxygen (1O2). Moreover, the possible catalytic mechanisms and reaction pathway of BPA degradation are systematically investigated based on analytical and photoelectrochemical analyses. This work not only provides a feasible means for the development of novel heterogeneous photo-Fenton catalysts, but also lays a theoretical foundation for the potential application of mineral-based materials in wastewater treatment.


Assuntos
Compostos Benzidrílicos , Compostos de Ferro , Nanocompostos , Nitrogênio , Fenóis , Titânio , Poluentes Químicos da Água , Titânio/química , Compostos Benzidrílicos/química , Fenóis/química , Nanocompostos/química , Poluentes Químicos da Água/química , Nitrogênio/química , Catálise , Ferro/química , Peróxido de Hidrogênio/química , Disruptores Endócrinos/química , Purificação da Água/métodos
16.
J Hazard Mater ; 470: 134193, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38569341

RESUMO

Arsenopyrite and pyrite often coexist in metal deposits and tailings, thus simultaneous bioleaching of both sulfides has economic (as well as environmental) significance. Important targets in bio-oxidation operations are high solubilization rates and minimized accumulation of Fe(III)/As-bearing secondary products. This study investigated the role of pyrite bioleaching in the enhancement of arsenopyrite dissolution. At a pyrite to arsenopyrite mass ratio of 1:1, 93.6% of As and 93.0% of Fe were solubilized. The results show that pyrite bio-oxidation can promote arsenopyrite dissolution, enhance S0 bio-oxidation, and inhibit the formation of jarosites, tooeleite, and amorphous ferric arsenate. The dry weight of the pyrite & arsenopyrite residue was reduced by 95.1% after bioleaching, compared to the initial load, while only 5% weight loss was observed when pyrite was absent. A biofilm was formed on the arsenopyrite surface in the presence of pyrite, while a dense passivation layer was observed in the absence of pyrite. As(III) (as As2O3) was a dominant As species in the pyrite & arsenopyrite residue. Novel and detailed findings are presented on arsenopyrite bio-dissolution in the presence of pyrite, and the presented approach could contribute to the development of novel cost-effective extractive bioprocesses. ENVIRONMENTAL IMPLICATION: The oxidation of arsenopyrite presents significant environmental hazards, as it can contribute to acid mine drainage generation and arsenic mobilization from sulfidic mine wastes. Bioleaching is a proven cost-effective and environmentally friendly extractive technology, which has been applied for decades in metal recovery from minerals or tailings. In this work, efficient extraction of arsenic from arsenopyrite bioleaching was presented through coupling the process with bio-oxidation of pyrite, resulting in lowered accumulation of hazardous and metastable Fe(III)/As-bearing secondary phases. The results could help improve current biomining operations and/or contribute to the development of novel cost-effective bioprocesses for metal extraction.


Assuntos
Arsenicais , Compostos de Ferro , Ferro , Minerais , Sulfetos , Sulfetos/química , Ferro/química , Arsenicais/química , Cinética , Minerais/química , Compostos de Ferro/química , Oxirredução , Solubilidade , Arsênio/química , Biofilmes , Acidithiobacillus/metabolismo
17.
Talanta ; 274: 126074, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38608632

RESUMO

Monitoring acetylcholinesterase (AChE) is crucial in clinical diagnosis and drug screening. Traditional methods for detecting AChE usually require the addition of intermediates like acetylthiocholine, which complicates the detection process and introduces interference risks. Herein, we develop a direct colorimetric assay based on alkaline iron formate nanosheets (Fe(HCOO)2.6(OH)0.3·H2O NSs, Fef NSs) for the detection of AChE without any intermediates. The as-prepared Fef NSs exhibit oxidase-like activity, catalyzing the generation of O2·-, 1O2 and ·OH, which leads to a color change from colorless to blue when exposed to 3,3',5,5'-tetramethylbenzidine. AChE directly inhibits the oxidase-like activity of Fef NSs, resulting in a hindered color reaction, enabling the detection of AChE. The biosensor has a linear detection range of 0.1-30 mU/mL, with a minimum detection limit of 0.0083 mU/mL (S/N = 3), representing a 100-fold improvement in detection sensitivity over the traditional Ellman's method. Satisfactory results were obtained when analyzing real AChE samples. Attractively, a method for the quantitative detection of AChE by a smartphone is established based on the Fef NSs. This method enables instant acquisition of AChE concentrations, achieving real-time visualized detection.


Assuntos
Acetilcolinesterase , Técnicas Biossensoriais , Colorimetria , Nanoestruturas , Smartphone , Acetilcolinesterase/metabolismo , Acetilcolinesterase/química , Colorimetria/métodos , Nanoestruturas/química , Técnicas Biossensoriais/métodos , Limite de Detecção , Oxirredutases/metabolismo , Oxirredutases/química , Humanos , Compostos de Ferro/química
18.
Water Res ; 256: 121580, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38614029

RESUMO

This study aimed to develop surface complexation modeling-machine learning (SCM-ML) hybrid model for chromate and arsenate adsorption on goethite. The feasibility of two SCM-ML hybrid modeling approaches was investigated. Firstly, we attempted to utilize ML algorithms and establish the parameter model, to link factors influencing the adsorption amount of oxyanions with optimized surface complexation constants. However, the results revealed the optimized chromate or arsenate surface complexation constants might fall into local extrema, making it unable to establish a reasonable mapping relationship between adsorption conditions and surface complexation constants by ML algorithms. In contrast, species-informed models were successfully obtained, by incorporating the surface species information calculated from the unoptimized SCM with the adsorption condition as input features. Compared with the optimized SCM, the species-informed model could make more accurate predictions on pH edges, isotherms, and kinetic data for various input conditions (for chromate: root mean square error (RMSE) on test set = 5.90 %; for arsenate: RMSE on test set = 4.84 %). Furthermore, the utilization of the interpretable formula based on Local Interpretable Model-Agnostic Explanations (LIME) enabled the species-informed model to provide surface species information like SCM. The species-informed SCM-ML hybrid modeling method proposed in this study has great practicality and application potential, and is expected to become a new paradigm in surface adsorption model.


Assuntos
Cromo , Compostos de Ferro , Aprendizado de Máquina , Adsorção , Cromo/química , Compostos de Ferro/química , Arsênio/química , Minerais/química , Arseniatos/química , Poluentes Químicos da Água/química , Cinética
19.
J Environ Manage ; 358: 120904, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38643624

RESUMO

This study focused on the economic feasibility of two potential industrial-scale bioleaching technologies for metal recovery from specific metallurgical by-products, mainly basic oxygen steelmaking dust (BOS-D) and goethite. The investigation compared two bioleaching scaling technology configurations, including an aerated bioreactor and an aerated and stirred bioreactor across different scenarios. Results indicated that bioleaching using Acidithiobacillus ferrooxidans proved financially viable for copper extraction from goethite, particularly when 5% and 10% pulp densities were used in the aerated bioreactor, and when 10% pulp density was used in the aerated and stirred bioreactor. Notably, a net present value (NPV) of $1,275,499k and an internal rate of return (IRR) of 65% for Cu recovery from goethite were achieved over 20-years after project started using the aerated and stirred bioreactor plant with a capital expenditure (CAPEX) of $119,816,550 and an operational expenditure (OPEX) of $5,896,580/year. It is expected that plant will start to make profit after one year of operation. Aerated and stirred bioreactor plant appeared more reliable alternative compared to the aerated bioreactor plant as the plant consists of 12 reactors which can allow better management and operation in small volume with multiple reactors. Despite the limitations, this techno-economic assessment emphasized the significance of selective metal recovery and plant design, and underscored the major expenses associated with the process.


Assuntos
Acidithiobacillus , Reatores Biológicos , Metalurgia , Acidithiobacillus/metabolismo , Cobre , Minerais , Compostos de Ferro
20.
Environ Pollut ; 350: 124005, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38648965

RESUMO

Simultaneously stabilizing of arsenic (As) and cadmium (Cd) in co-contaminated soil presents substantial challenges due to their contrasting chemical properties. Schwertmannite (Sch) is recognized as a potent adsorbent for As pollution, with alkali modification showing promising results in the simultaneous immobilization of both As and Cd. This study systematically investigated the long-term stabilization efficacy of alkali-modified Sch in Cd-As co-contaminated farmland soil over a 200-day flooding-drying period. The results revealed that As showed significant mobility in flooded conditions, whereas Cd exhibited increased soil availability under drying phases. The addition of Sch did not affect the trends in soil pH and Eh fluctuations; nonetheless, it led to an augmentation in the levels of amorphous iron oxides and SO42- concentration in soil pore water. At a dosage of 0.5% Sch, there was a notable decrease in the mobility and soil availability of As and Cd under both flooding (34.5% and 53.6% at Day 50) and drying conditions (27.0% and 29.4% at Day 130), primarily promoting the transformation of labile metal(loid) fraction into amorphous iron oxide-bound forms. Throughout the flooding-drying treatment period, Sch maintained stable mineral morphology and mineralogical phase, highlighting its long-term stabilization effect. The findings of this study emphasize the promising application of Sch-based soil remediation agents in mitigating the challenges arising from As-Cd co-contamination. Further research is warranted to explore their application in real farmland settings and their impact on the uptake of toxic metal(loid)s by plants.


Assuntos
Arsênio , Cádmio , Recuperação e Remediação Ambiental , Inundações , Poluentes do Solo , Solo , Arsênio/análise , Cádmio/análise , Solo/química , Recuperação e Remediação Ambiental/métodos , Compostos de Ferro/química , Fazendas , Adsorção
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