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Defective magnesium ferrite nano-platelets for the adsorption of As(V): The role of surface hydroxyl groups
2018
Wu, Can | Tu, Jingwei | Tian, Chen | Geng, Junjie | Lin, Zhang | Dang, Zhi
In this work, magnesium ferrite (MgFe₂O₄) nano-platelets with rich defects and abundant surface hydroxyl groups were synthesized, and used for the removal of low concentration As(V) in aqueous solution. Results from scanning electron microscopy (SEM) showed that the as-synthesized MgFe₂O₄ nano-platelets were consisted of many individual nanospheres. Rietveld refinement of X-ray diffraction (XRD) data indicated that the Mg²⁺ ions substituted the Fe³⁺ ions at both the octahedral and the tetrahedral sites of the crystal structure. Batch adsorption experiment showed that the equilibrium concentration of As(V) could be reduced down to 4.9 μg·L⁻¹ when the initial concentration of As(V) is 1 mg·L⁻¹, which complied with the drinking water standard of WHO (10 μg·L⁻¹). The adsorption capacity of synthesized MgFe₂O₄ towards As(V) was higher than commonly used iron oxide adsorbents (Fe₃O₄, γ-Fe₂O₃ and α-Fe₂O₃). Mechanistic studies proved that the superior adsorption capacity was attributed to: (1) increased amount of surface hydroxyl groups that resulted from the surface defects. (2) formation of tridentate hexanuclear surface complexes instead of bidentate binuclear complexes, and (3) formation of excess Mg-OH surface hydroxyl groups and As-Mg monodentate mononuclear surface complexes. This work disclosed the correlation of the superior As(V) adsorption ability with the surface hydroxyl groups in defective MgFe₂O₄, and propose MgFe₂O₄ as a potential candidate for the remediation of As-contaminated water.
Show more [+] Less [-]Role of oxygen-containing functional groups in forest fire-generated and pyrolytic chars for immobilization of copper and nickel
2017
Esfandbod, Maryam | Merritt, Christopher R. | Rashti, Mehran Rezaei | Singh, Balwant | Boyd, Sue E. | Srivastava, Prashant | Brown, Christopher L. | Butler, Orpheus M. | Kookana, Rai S. | Chen, Chengrong
Char as a carbon-rich material, can be produced under pyrolytic conditions, wildfires or prescribed burn offs for fire management. The objective of this study was to elucidate mechanistic interactions of copper (Cu2+) and nickel (Ni2+) with different chars produced by pyrolysis (green waste, GW; blue-Mallee, BM) and forest fires (fresh-burnt by prescribed fire, FC; aged char produced by wild fire, AC). The pyrolytic chars were more effective sorbents of Cu2+ (∼11 times) and Ni2+ (∼5 times) compared with the forest fire chars. Both cross-polarization (CPMAS-NMR) and Bloch decay (BDMAS-NMR) 13C NMR spectroscopies showed that forest fire chars have higher woody components (aromatic functional groups) and lower polar groups (e.g. O-alkyl C) compared with the pyrolytic chars. The polarity index was greater in the pyrolytic chars (0.99–1.34) than in the fire-generated chars (0.98–1.15), while aromaticity was lower in the former than in the latter. Fourier transform infrared (FTIR) and Raman spectroscopies indicated the binding of carbonate and phosphate with both Cu2+ and Ni2+ in all chars, but with a greater extent in pyrolytic than forest fire-generated chars. These findings have demonstrated the key role of char's oxygen-containing functional groups in determining their sorption capacity for the Cu2+ and Ni2+ in contaminated lands.
Show more [+] Less [-]Influence of sediment resuspension on the efficacy of geoengineering materials in the control of internal phosphorous loading from shallow eutrophic lakes
2016
Yin, Hongbin | Kong, Ming | Han, Meixiang | Fan, Chengxin
Modified clay-based solid-phase phosphorous (P) sorbents are increasingly used as lake geoengineering materials for lake eutrophication control. However, some still dispute the feasibility of using these materials to control internal P loading from shallow eutrophic lakes. The lack of information about P behavior while undergoing frequent sediment resuspension greatly inhibits the modified minerals’ use. In this study, a sediment resuspension generating system was used to simulate the effect of both moderate winds (5.1 m/s) and strong winds (8.7 m/s) on the stability of sediment treated by two geoengineering materials, Phoslock® (a lanthanum modified bentonite) and thermally-treated calcium-rich attapulgite. This study also presents an analysis of the P dynamics across the sediment-water interface of two shallow eutrophic lakes. In addition, the effect of wind velocity on P forms and P supply from the treated sediment were studied using chemical extraction and diffusive gradients in thin films (DGT) technique, respectively. Results showed that adding geoengineering materials can enhance the stability of surface sediment and reduce the erosion depth caused by wind accordingly. All treatments can effectively reduce soluble reactive phosphorus (SRP) concentration in overlying water when sediment is capped with thermally-treated calcium-rich attapulgite, which performs better than sediment mixed with modified attapulgite but not as well as sediment treated with Phoslock®. However, their efficiency decreased with the increase in occurrences of sediment resuspension. The addition of the selected geoengineering materials effectively reduced the P fluxes across sediment-water interface and lowered P supply ability from the treated sediment during sediment resuspension. The reduction of mobile P and enhancement of calcium bound P and residual P fraction in the treated sediment was beneficial to the long-term lake internal P loading management. All of the results indicated that the studied geoengineering materials are suitable for application in shallow eutrophic lakes with frequent sediment resuspension activity.
Show more [+] Less [-]LSER model for organic compounds adsorption by single-walled carbon nanotubes: Comparison with multi-walled carbon nanotubes and activated carbon
2015
Yu, Xiangquan | Sun, Weiling | Ni, Jinren
LSER models for organic compounds adsorption by single and multi-walled carbon nanotubes and activated carbon were successfully developed. The cavity formation and dispersion interactions (vV), hydrogen bond acidity interactions (bB) and π-/n-electron interactions (eE) are the most influential adsorption mechanisms. SWCNTs is more polarizable, less polar, more hydrophobic, and has weaker hydrogen bond accepting and donating abilities than MWCNTs and AC. Compared with SWCNTs and MWCNTs, AC has much less hydrophobic and less hydrophilic adsorption sites. The regression coefficients (e, s, a, b, v) vary in different ways with increasing chemical saturation. Nonspecific interactions (represented by eE and vV) have great positive contribution to organic compounds adsorption, and follow the order of SWCNTs > MWCNTs > AC, while hydrogen bond interactions (represented by aA and bB) demonstrate negative contribution. These models will be valuable for understanding adsorption mechanisms, comparing adsorbent characteristics, and selecting the proper adsorbents for certain organic compounds.
Show more [+] Less [-]Adsorption of sulfonamides to demineralized pine wood biochars prepared under different thermochemical conditions
2014
Xie, Mengxing | Chen, Wei | Xu, Zhaoyi | Zheng, Shourong | Zhu, Dongqiang
The main objective of this study was to understand the key factors and mechanisms controlling adsorption of sulfonamides to biochars. Batch adsorption experiments were performed for sulfamethoxazole and sulfapyridine to three pine-wood biochars prepared under different thermochemical conditions: pyrolysis at 400 °C (C400) and 500 °C (C500), and pyrolysis at 500 °C followed with hydrogenation (C500-H). For both sulfonamides, the adsorbent surface area-normalized adsorption was stronger to C500 than to C400. This is attributable to the enhanced π–π electron-donor–acceptor interaction with the carbon surface of C500 due to the higher degree of graphitization. Despite the relatively large difference in surface O-functionality content between C500 (12.2%) and C500-H (6.6%), the two biochars exhibited nearly identical adsorbent surface area-normalized adsorption, indicating negligible role of surface O-functionalities in the adsorption to these adsorbents. Effects of solution chemistry conditions (pH, Cu2+, and dissolved soil humic acid) on adsorption were examined.
Show more [+] Less [-]Sorption mechanisms of perfluorinated compounds on carbon nanotubes
2012
Deng, Shubo | Zhang, Qiaoying | Nie, Yao | Wei, Haoran | Wang, Bin | Huang, Jun | Yu, Gang | Xing, Baoshan
Sorption of perfluorinated compounds (PFCs) on carbon nanotubes (CNTs) is critical for understanding their subsequent transport and fate in aqueous environments, but the sorption mechanisms remain largely unknown. In this study, the sorption of six PFCs on CNTs increased with increasing C-F chain length when they had a same functional group, and the CNTs with hydroxyl and carboxyl groups had much lower adsorbed amount than the pristine CNTs, indicating that hydrophobic interaction dominated the sorption of PFCs on the CNTs. Electrostatic repulsion suppressed the sorption of PFCs on the CNTs, resulting in the lower sorption with increasing pH. Hydrogen bonding interaction was negligible. The hydrophobic C-F chains can be closely adsorbed on the CNTs surface in parallel to the axis or along the curvature, making it impossible to form micelles on the CNT surface, leading to the lower sorption than other adsorbents.
Show more [+] Less [-]Remediation of organic and inorganic arsenic contaminated groundwater using a nanocrystalline TiO2-based adsorbent
2009
Jing, Chuanyong | Meng, Xiaoguang | Calvache, Edwin | Jiang, Guibin
A nanocrystalline TiO₂-based adsorbent was evaluated for the simultaneous removal of As(V), As(III), monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA) in contaminated groundwater. Batch experimental results show that As adsorption followed pseudo-second order rate kinetics. The competitive adsorption was described with the charge distribution multi-site surface complexation model (CD-MUSIC). The groundwater containing an average of 329 μg L⁻¹ As(III), 246 μg L⁻¹ As(V), 151 μg L⁻¹ MMA, and 202 μg L⁻¹ DMA was continuously passed through a TiO₂ filter at an empty bed contact time of 6 min for 4 months. Approximately 11 000, 14 000, and 9900 bed volumes of water had been treated before the As(III), As(V), and MMA concentration in the effluent increased to 10 μg L⁻¹. However, very little DMA was removed. The EXAFS results demonstrate the existence of a bidentate binuclear As(V) surface complex on spent adsorbent, indicating the oxidation of adsorbed As(III). A nanocrystalline TiO₂-based adsorbent could be used for the simultaneous removal of As(V), As(III), MMA, and DMA in contaminated groundwater.
Show more [+] Less [-]Quantification of activated carbon contents in soils and sediments using chemothermal and wet oxidation methods
2009
Brändli, Rahel C. | Bergsli, Anders | Ghosh, Upal | Hartnik, Thomas | Breedveld, Gijs D. | Cornelissen, Gerard
Activated carbon (AC) strongly sorbs organic pollutants and can be used for remediation of soils and sediments. A method for AC quantification is essential to monitor AC (re)distribution. Since AC is black carbon (BC), two methods for BC quantification were tested for AC mixed in different soils and sediments: i) chemothermal oxidation (CTO) at a range of temperatures and ii) wet-chemical oxidation with a potassium dichromate/sulfuric acid solution. For three soils, the amount of AC was accurately determined by CTO at 375 °C. For two sediments, however, much of the AC disappeared during combustion at 375 °C, which could probably be explained by catalytic effects by sediment constituents. CTO at lower temperatures (325–350 °C) was a feasible alternative for one of the sediments. Wet oxidation effectively functioned for AC quantification in sediments, with almost complete AC recovery (81–92%) and low remaining amounts of native organic carbon (5–16%). Activated carbon quantification is best performed for soils with chemothermal oxidation at 375 °C, and for sediments with wet oxidation with potassium dichromate/sulfuric acid.
Show more [+] Less [-]Fabrication of activated carbon supported modified with bimetallic-platin ruthenium nano sorbent for removal of azo dye from aqueous media using enhanced ultrasonic wave
2022
Herein, activated carbon supported modified with bimetallic-platin ruthenium nano sorbent (PtRu@AC) was synthesized by a thermal decomposition process and used in the removal of methylene blue (MB) from aqueous solutions. The synthesized nano sorbents were characterized by X-ray Diffraction (XRD), Transmission Electron Microscopy (TEM), and X-ray Photoelectron Spectroscopy (XPS) spectroscopic techniques. The data obtained from characterization studies showed that PtRu@AC nano sorbent was highly crystalline and in a form of PtRu alloy with a monodispersed composition. The results indicated that the maximum adsorption capacity (qemax) for the removal of MB with PtRu@AC under optimum conditions was detected to be 1.788 mmol/g (569.4 mg/g). The experimental kinetic results of the study revealed that the adsorption of methylene blue was found to be more compatible with the false second-order model compared to some tested models. Calculations for thermodynamic functions including enthalpy change (ΔHo), entropy change (ΔSo), and Gibbs free energy change (ΔGo) values were performed to get an idea about the adsorption mechanism. As a result, the synthesized PtRu@AC nano adsorbent was detected as a highly effective adsorbent material in the removal of MB from aquatic mediums.
Show more [+] Less [-]Simultaneous capturing of mixed contaminants from wastewater using novel one-pot chitosan functionalized with EDTA and graphene oxide adsorbent
2022
Verma, Monu | Ashwani Kumar, | Lee, Ingyu | Kumar, Vinod | Park, Ju-Hyun | Kim, Hyunook
The emergence of inorganic and organic contaminants has raised great concerns owing to their adverse impact on human health and ecological security. Herein, first time one-pot process was applied for chitosan (CS) functionalization using graphene oxide (GO) and ethylenediaminetetraacetic acid (EDTA) for simultaneous capturing of toxic inorganic (lead (Pb²⁺) and cadmium (Cd²⁺)) and organic (ciprofloxacin (CIP) and sildenafil (SDF)) contaminants from wastewater. In this approach, we believe that CS would work as a backbone, GO would capture both inorganic and organic contaminants via electrostatic interactions, while EDTA would make complexation with heavy metals. Various parameters including pH, reaction time, concentration, reusability etc. were evaluated to achieve the best experimental result in monocomponent system. The prepared adsorbent displayed an excellent monolayer adsorption capacity of 351.20 and 264.10 mg g⁻¹ for Pb²⁺ and Cd²⁺, respectively, while a heterogeneous sorption capacity of 75.40 and 40.90 mg g⁻¹ for CIP and SDF, respectively. The kinetics data fitted well to Pseudo-second order (PSO) kinetics model for both types of contaminants and gave faster interaction towards metal ions (higher k₂) than organic contaminants. Experimental results showed excellent adsorption efficiencies at environmental levels in the capturing of both inorganic and organic contaminants at the same time from polluted water. The capturing mechanism of both types of contaminants was explained by elemental mapping, EDS, and FT−IR spectra. Overall, easy synthesis, excellent capturing capacity, and reusability imply that the prepared adsorbent has a sufficient potential for the treatment of co-existing toxic contaminants in water.
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