1. |
- Zou, Yidong, et al.
(författare)
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Glycerol-Modified Binary Layered Double Hydroxide Nanocomposites for Uranium Immobilization via Extended X-ray Absorption Fine Structure Technique and Density Functional Theory Calculation
- 2017
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Ingår i: ACS Sustainable Chemistry and Engineering. - : AMER CHEMICAL SOC. - 2168-0485. ; 5:4, s. 3583-3595
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Tidskriftsartikel (refereegranskat)abstract
- Novel, efficient, glycerol-modified nanoscale layered double hydroxides (rods Ca/Al LDH-Gl and flocculent Ni/Al LDH-Gl) were successfully synthesized by a simple one-step hydrothermal synthesis route and showed excellent adsorption capacities for U(VI) from aqueous solutions under various environmental conditions. The advanced spectroscopy analysis confirmed the existence of abundant oxygen-containing functional groups (e.g., C-O, O-C=O, and C=O) on the surfaces of Ca/AI LDH-Gl and Ni/Al LDH-Gl, which could provide enough free active sites for the binding of U(VI). The maximum adsorption capacities of Macro-application (Environment U(VI) calculated from the Sips model were 266.5 mg.g(-1) for Ca/Al LDH-Gl and 142.3 mg.g(-1) for Ni/Al LDH-Gl at 298.15 K, and the higher adsorption capacity of Ca/Al LDH-Gl might be due to more functional groups and abundant high-activity "Ca-O" groups. Macroscopic experiments proved that the interaction of U(VI) on Ca/Al LDH-Gl and Ni/Al LDH-Gl was due to surface complexation and electrostatic interactions. The extended Xray absorption fine structure analysis confirmed that U(IV) did not transformation to U(VI) on solid particles, and stable inner sphere complexes were not formed by reduction interaction but by chemical adsorption. The density functional theory (DFT) calculations further evidenced that the higher adsorption energies (i.e., E-ad = 4.00 eV for Ca/AI LDH-Gl-UO22+ and E-ad = 2.43 eV for Ca/Al LDH-Gl-UO2CO3) were mainly attributed to stronger hydrogen bonds and electrostatic interactions. The superior immobilization performance of Ca/AI LDH-Gl supports a potential strategy for decontamination of UO22+ from wastewater, and it may provide new insights for the efficient removal of radionuclides in environmental pollution cleanup.
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2. |
- Zou, Yidong, et al.
(författare)
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beta-Cyclodextrin modified graphitic carbon nitride for the removal of pollutants from aqueous solution : experimental and theoretical calculation study
- 2016
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 4:37, s. 14170-14179
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Tidskriftsartikel (refereegranskat)abstract
- A novel beta-cyclodextrin modified, multifunctional, layer-by-layer graphitic carbon nitride (g-C3N4/beta-CD) was successfully synthesized and applied as an effective adsorbent for the removal of methyl orange (MO) and Pb(II) from aqueous solutions under various environmental conditions (e.g., solution pH, solid content, contact time and temperature). The kinetic results indicated that the adsorption was dominated by chemisorption, and the higher adsorption capacity of g-C3N4/beta-CD was attributed to it having more oxygen-containing functional groups than g-C3N4. The Langmuir, Freundlich and Sips models were applied to simulate the adsorption isotherms of MO and Pb(II), and the results demonstrated that the adsorption of MO was attributed to multilayer adsorption, while the coverage adsorption of Pb(II) on the g-C3N4/beta-CD was monolayer adsorption. The thermodynamic parameters showed that the adsorption of both MO and Pb(II) was spontaneous and endothermic. The DFT calculations further evidenced the surface complexation and electrostatic interaction of Pb(II) on the g-C3N4 and g-C3N4/beta-CD, whereas, the interaction of MO with g-C3N4 and g-C3N4/beta-CD was mainly attributed to hydrogen bonds and strong pi-pi interactions. The results demonstrated that g-C3N4/beta-CD is a promising material for the efficient removal of organic and inorganic pollutants in environmental pollution remediation.
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3. |
- Zou, Yidong, et al.
(författare)
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Coagulation Behavior of Graphene Oxide on Nanocrystallined Mg/AI Layered Double Hydroxides : Batch Experimental and Theoretical Calculation Study
- 2016
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 50:7, s. 3658-3667
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Tidskriftsartikel (refereegranskat)abstract
- Graphene oxide (GO) has attracted considerable attention because of its remarkable enhanced adsorption and multifunctional properties. However, the toxic properties of GO nanosheets released into the environment could lead to the instability of biological system. In aqueous phase, GO may interact with fine mineral particles, such as chloridion intercalated nanocrystallined Mg/Al layered double hydroxides (LDH-Cl) and nanocrystallined Mg/Al LDHs (LDH CO3), which are considered as coagulant molecules for the coagulation and removal of GO from aqueous solutions. Herein the coagulation of GO on LDHs were studied as a function of solution pH, ionic strength, contact time, temperature and coagulant concentration. The presence of LDH Cl and LDH-CO3 improved the coagulation of GO in solution efficiently, which was mainly attributed to the surface oxygen-containing functional groups of LDH Cl and LDH-CO3 occupying the binding sites of GO. The coagulation of GO by LDH-CI and LDH-CO3 was strongly dependent on pH and ionic strength. Results of coagulation of GO on LDHs was energetically favored by electrostatic interactions and hydrogen bonds, which was further evidenced by FTIR and XPS analysis. By integrating the experimental results, it was clear that LDH Cl could be potentially used as a cost-effective coagulant for the elimination of GO from aqueous solutions, which could efficiently decrease the potential toxicity of GO in the natural environment.
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