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Environ Sci Technol ; 2020 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-32182042


Surface functional groups play a dominating role in determining the adsorption performance of metal oxide particles. The ability to manipulate the surface functional groups is vital in designing an effective adsorbent for water decontamination. In this study, a facile method is proposed for tuning the amount of the surface hydroxyl groups of CeO2 particles. The volume of water added during the ethylene glycol-mediated solvothermal synthesis of CeO2 particles can be used to adjust the amount of surface hydroxyl groups. By simple reduction in the volume of water, the number of surface hydroxyl groups of CeO2 particles can be increased and the phosphate adsorption capacity can be greatly improved. Our results show that the obtained CeO2 particles have high phosphate adsorption capacity at low phosphate concentrations, fast adsorption kinetics, and the ability to achieve an ultralow phosphate concentration in the real sewage effluent. This study provides an effective strategy for designing highly effective metal oxide adsorbents through surface functional group engineering.

Environ Sci Technol ; 2019 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-31804806


Eutrophication of water bodies is a serious and widespread environmental problem. Achieving low levels of phosphate concentration to prevent eutrophication is one of the important goals of the wastewater engineering and surface water management. Meeting the increasingly stringent standards is feasible in using a phosphate-selective sorption system. This critical review discusses the most fundamental aspects of selective phosphate removal processes and highlights gains from the latest developments of phosphate-selective sorbents. Selective sorption of phosphate over other competing anions can be achieved based on their differences in acid-base properties, geometric shapes, and metal complexing abilities. Correspondingly, interaction mechanisms between the phosphate and sorbent are categorized as hydrogen bonding, shape complementarity, and inner-sphere complexation, and their representative sorbents are organic-functionalized materials, molecularly imprinted polymers, and metal-based materials, respectively. Dominating factors affecting the phosphate sorption performance of these sorbents are critically examined, along with a discussion of some overlooked facts regarding the development of high-performance sorbents for selective phosphate removal from water and wastewater.

Chemosphere ; 192: 209-216, 2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-29102865


Lanthanum-based adsorbents are ideal candidates for phosphate removal because of their excellent affinity to phosphate. However, their application in the removal of trace-levels of phosphate from sewage is still unsatisfactory due to the limited adsorption capacity and inadequate optimization of the operational parameters. To overcome these drawbacks, we have developed a novel lanthanum hydroxide (LH), using a facile precipitation and hydrothermal process that involves a nanorod-like structure with the lengths ranging from 124 to 1700 nm, depending on the La/OH molar ratio. The phosphate adsorption capacity of the developed LH is up to 170.1 mg-P g-1 in synthetic water, while a slightly lower adsorption capacity of 111.1 mg-P g-1 is observed in a sewage sample. A polynominal model consisting of three variables (i.e. dosage, reaction time and initial phosphate concentration) for predicting efficiency of phosphate removal has been successfully developed using a face-centred central composite design (CCD)-based methodology. The results also suggest a strong interactive effect of the dosage with the phosphate concentration, and reaction time, which can significantly affect the optimization of the phosphate removal by LH. Both X-ray photoelectron spectroscopy and X-ray diffraction studies indicate that the inner sphere complexation of phosphate with LH is probably the major mechanism governing phosphate removal.

Lantânio/química , Fosfatos/química , Esgotos/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Adsorção , Nanotubos , Espectroscopia Fotoeletrônica , Água/química , Difração de Raios X
Environ Sci Technol ; 51(21): 12377-12384, 2017 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-29035555


Lanthanum-based materials are effective for sequestering phosphate in water, however, their removal mechanisms remain unclear, and the effects of environmentally relevant factors have not yet been studied. Hereby, this study explored the mechanisms of phosphate removal using La(OH)3 by employing extended X-ray absorption spectroscopy (EXAFS), attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), density functional theory (DFT) and chemical equilibrium modeling. The results showed that surface complexation was the primary mechanism for phosphate removal and in binary phosphate configurations, namely diprotonated bidentate mononuclear (BM-H2) and bidentate binuclear (BB-H2), coexisting on La(OH)3 in acidic conditions. By increasing the pH to 7, BM-H1 and BB-H2 were the two major configurations governing phosphate adsorption on La(OH)3, whereas BB-H1 was the dominant configuration of phosphate adsorption at pH 9. With increasing phosphate loading, the phosphate configuration of on La(OH)3 transforms from binary BM-H1 and BB-H2 to BB-H1. Amorphous Ca3(PO4)2 forms in the presence of Ca, leading to enhanced phosphate removal at alkaline conditions. The contributions of different mechanisms to the overall phosphate removal were successfully simulated by a chemical equilibrium model that was consistent with the spectroscopic results. This study provides new insights into the molecular-level mechanism of phosphate removal by La(OH)3.

Lantânio , Nanotubos , Adsorção , Fosfatos , Espectroscopia de Infravermelho com Transformada de Fourier
Water Res ; 126: 179-188, 2017 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-28950228


The use of lanthanum (La)-based materials for phosphate removal from water and wastewater has received increasing attention. However, challenges remain to enhance phosphate sorption capacities and recover La-based sorbents. In this study, magnetic La(OH)3/Fe3O4 nanocomposites with varied La-to-Fe mass ratios were synthesized through a precipitation and hydrothermal method. Based upon preliminary screening of synthesized La(OH)3/Fe3O4 nanocomposites in terms of phosphate sorption capacity and La content, La(OH)3/Fe3O4 nanocomposite with a La-to-Fe mass ratio of 4:1 was chosen for further characterization and evaluation. Specifically, for these materials, magnetic separation efficiency, phosphate sorption kinetics and isotherm behavior, and solution matrix effects (e.g., coexisting ions, solution pH, and ionic strength) are reported. The developed La(OH)3/Fe3O4 (4:1) nanocomposite has an excellent magnetic separation efficiency of >98%, fast sorption kinetics of 30 min, high sorption capacity of 83.5 mg P/g, and strong selectivity for phosphate in presence of competing ions. Phosphate uptake by La(OH)3/Fe3O4 (4:1) was pH-dependent with the highest sorption capacities observed over a pH range of 4-6. The ionic strength of the solution had little interference with phosphate sorption. Sorption-desorption cyclic experiments demonstrated the good reusability of the La(OH)3/Fe3O4 (4:1) nanocomposite. In a real treated wastewater effluent with phosphate concentration of 1.1 mg P/L, 0.1 g/L of La(OH)3/Fe3O4 (4:1) efficiently reduced the phosphate concentration to below 0.05 mg P/L. Electrostatic attraction and inner-sphere complexation between La(OH)3 and P via ligand exchange were identified as the sorption mechanisms of phosphate by La(OH)3/Fe3O4 (4:1).

Nanocompostos/química , Fosfatos/isolamento & purificação , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/isolamento & purificação , Adsorção , Precipitação Química , Compostos Férricos/química , Concentração de Íons de Hidrogênio , Cinética , Lantânio/química , Magnetismo , Concentração Osmolar , Fosfatos/química , Espectroscopia Fotoeletrônica , Espectroscopia de Infravermelho com Transformada de Fourier , Águas Residuárias/química , Poluentes Químicos da Água/química