Removing Pb2+ and As(V) from polluted water by highly reusable Fe-Mg metal-organic complex adsorbent
Graphical abstract
Introduction
Among the reported pollutants [[1], [2], [3], [4]], heavy metal ions such as Pb(II) and As(V) are polluting water more and more seriously [[5], [6], [7], [8], [9], [10], [11]]. A series of metal-based materials such as metal oxides, metal organic complexes, and metal hydroxides are often used as adsorbents to remove heavy metal ions [[12], [13], [14], [15]]. Thereinto, metal organic complexes have the advantages of both organics and metallic materials. This presents a synergistic effect and improves the adsorption performance, hydrophilic and chemical stability of composite materials greatly [[16], [17], [18]]. Over the past few years, the fabrication of two-dimension (2D) nanomaterials has attracted significant interests because of their outstanding performance in energy storage [[19], [20], [21], [22]], semiconductor [23], optics [24], sensing [25], biomedicines [26] and other areas [[27], [28], [29], [30], [31]]. Mechanical exfoliation method is an easy technology to prepare 2D nanosheets, and the first preparation of monolayer graphene is based on this technology [32]. Since then, many different types of 2D materials have been synthesized by this method [33]. However, mechanical exfoliation method cannot achieve a low-cost mass production. Therefore, a series of methods have been developed to prepare 2D layered materials, which can be applied in practical production, such as mechanical stripping [34], physical vapor deposition [35], liquid chemical synthesis [36], ultrasonic liquid phase stripping method [37], and epitaxial growth method [38]. 2D nanomaterials are suitable for water treatment because of their more surface active sites and high specific surface area [[39], [40], [41], [42], [43]].
The most common form of adsorption is electrostatic adsorption. Pb(II) and As(V) usually exist as positive ions (i.e., Pb2+) and negative ions (i.e., H2AsO4−, HAsO42−) in water, respectively. As a result, the adsorbent for removing Pb2+ should be negatively charged and while for removing As(V), the adsorbent should be positively charged. Another adsorption mechanism of heavy metal ions is the ion exchange. The ions with the same charges between adsorbent and heavy metal ions are exchanged during the adsorption process [44]. But the exchanged ions of the adsorbent will remain in the solution, and may lead to a secondary pollution. As a result, the metal elements in the adsorbent should be harmless to human body and the ecosystems when the ion exchange was used as the adsorption mechanism to remove heavy metal cations, such as Fe and Mg. At present, most of the cationic adsorbents based on ion exchange mechanism cannot be desorbed and recycled [45], thus post-treatment of saturated adsorption is an urgent problem to be solved. Mg2+ in metal organic nanocomposites is easy to exchange with Pb(II) in solution [46], which can effectively adsorb Pb(II) in aqueous solutions, and the adsorbed material is relatively stable. However, Fe(III) in metal organic nanocomposites has a certain affinity with As (V) in aqueous solutions [47].
In this study, we designed a kind of metal organic nanocomposites with Fe and Mg as metal active sites and terephthalic acid as organic medium using ultrasonic assisted in situ growth method. This preparation method has the characteristics of simple operation, low cost and industrialization. The adsorption capacity of the product for Pb (II) was studied, and the anion adsorption capacity of the product after saturated adsorption of Pb (II) was further explored. As (V) in the solution was adsorbed by saturated Pb (II) material. The Fe-Mg metal organic nanosheet (Fe-Mg-BDC) and The Fe-Mg metal organic nanosheets after the saturated adsorption of Pb(II) (Fe-Pb(Mg)-BDC) were characterized by SEM, TEM, EDX, XRD, FT-IR, etc. The adsorption capacity of Fe-Mg-BDC and Fe-Pb(Mg)-BDC for As(V) was tested. The adsorption isotherm and adsorption kinetic models of Fe-Mg-BDC for Pb(II) and Fe-Pb(Mg)-BDC for As(V) were studied and analyzed in details.
Section snippets
Materials
Na2HAsO4·7H2O, Pb(NO3)2, FeCl2·4H2O, MgCl2·6H2O, N,N-dimethylformamide, benzenedicarboxylic acid, triethylamine (TEA) and ethyl alcohol were obtained commercially and were used as-received without any further purification. Ultrapure water used in the experiments was prepared by a Millipore System (Millipore Q).
Synthesis of Fe-Mg metal organic nanosheets (Fe-Mg-BDC)
The Fe-Mg metal organic nanosheets (Fe-Mg-BDC) were synthesized as follows. Firstly, a mixed solution consisting of DMF (60 mL), ethanol (4 mL) and water (4 mL) was stirred to make a
Characterization of Fe-Mg-BDC complexes
In order to explore the content of different metal elements in Fe-Mg-BDC, 30 mg Fe-Mg-BDC was dissolved in 20 mL aqua regia, and then added in ultra-pure water to 1000 mL. 10 mL of the solution was taken and the concentrations of Mg and Fe elements were tested using ICP. The results are shown in Table 1. The morphologies of Fe-Mg BDC were characterized by SEM and TEM. As shown in Fig. 1a, the Fe-Mg-BDC shows a thin sheet shape with a mean diameter of 4 μm and nanoscale thickness (Fig. 1b). Fig.
Conclusions
The Fe-Mg metal organic nanosheet adsorbents had been successfully prepared by a simple room temperature ultrasonic method. Fe-Mg-BDC was found to own nano-lamella structure with a specific surface area of 33.4 m2 g−1, and had a good adsorption of Pb(II) cation. The Fe-Mg-BDC adsorbents for Pb(II) followed the Langmuir isotherm and pseudo-second order kinetics model, respectively. The adsorption mechanism of Fe-Mg-BDC for Pb(II) was proven to be the ion exchange with the Mg and Fe as residual
Declaration of Competing Interest
All the authors have agreed on this submission. There is no conflict of interest for this submission. This paper is not under consideration by other journals.
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