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. 2022 Jul 13;12(1):11865.
doi: 10.1038/s41598-022-16038-0.

Facile fabrication of amino-functionalized MIL-68(Al) metal-organic framework for effective adsorption of arsenate (As(V))

Alireza Rahmani  1 , Amir Shabanloo  2 , Solmaz Zabihollahi  3 , Mehdi Salari  4 , Mostafa Leili  1 , Mohammad Khazaei  1 , Saber Alizadeh  5 , Davood Nematollahi  5
Affiliations

Facile fabrication of amino-functionalized MIL-68(Al) metal-organic framework for effective adsorption of arsenate (As(V))

Alireza Rahmani et al. Sci Rep. .

Abstract

An amino-functionalized MIL-68(Al) metal-organic framework (amino-MIL-68(Al) MOF) was synthesized by solvothermal method and then characterized by FESEM, XRD, FTIR, EDX-mapping, and BET-BJH techniques. In order to predict arsenate (As(V)) removal, a robust quadratic model (R2 > 0.99, F-value = 2389.17 and p value < 0.0001) was developed by the central composite design (CCD) method and then the genetic algorithm (GA) was utilized to optimize the system response and four independent variables. The results showed that As(V) adsorption on MOF was affected by solution pH, adsorbent dose, As(V) concentration and reaction time, respectively. Predicted and experimental As(V) removal efficiencies under optimal conditions were 99.45 and 99.87%, respectively. The fitting of experimental data showed that As(V) adsorption on MOF is well described by the nonlinear form of the Langmuir isotherm and pseudo-second-order kinetic. At optimum pH 3, the maximum As(V) adsorption capacity was 74.29 mg/g. Thermodynamic studies in the temperature range of 25 to 50 °C showed that As(V) adsorption is a spontaneous endothermic process. The reusability of MOF in ten adsorption/regeneration cycles was studied and the results showed high reusability of this adsorbent. The highest interventional effect in inhibiting As(V) adsorption was related to phosphate anion. The results of this study showed that amino-MIL-68(Al) can be used as an effective MOF with a high surface area (> 1000 m2/g) and high reusability for As(V)-contaminated water.

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Conflict of interest statement

The authors declare no competing interests.

Figures

Figure 1
Figure 1
FESEM images of amino-MIL-68(Al) with different magnifications (a–f).
Figure 2
Figure 2
Experimental and simulated XRD patterns of amino-MIL-68(Al) (a); FTIR spectra of amino-MIL-68(Al) (b).
Figure 3
Figure 3
EDX-mapping analysis of amino-MIL-68(Al) (a). The ADS/DES isotherm of N2 on amino-MIL-68(Al) (b), BJH pore size of amino-MIL-68(Al) (c).
Figure 4
Figure 4
FESEM images of MIL-68(Al) with different magnifications (a–d); The ADS/DES isotherm of N2 on MIL-68(Al) (e), BJH pore size of MIL-68(Al) (f).
Figure 5
Figure 5
Output of GA method for optimization of independent variables in As(V) adsorption process on amino-MIL-68(Al). MATLAB R2013a software was used to create this figure (https://www.mathworks.com/products/matlab.html).
Figure 6
Figure 6
Interaction of pH and MOF dose on system response (As(V) = 2.5 mg/L, Time = 80 min). Design-Expert v13 software was used to create this figure (https://www.statease.com/docs/v13/).
Figure 7
Figure 7
Interaction of reaction time and As(V) concentration on system response (pH = 3, MOF dose = 0.4 g/L). Design-Expert v13 software was used to create this figure (https://www.statease.com/docs/v13/).
Figure 8
Figure 8
Nonlinear isotherm models (pH = 3) (a), and nonlinear adsorption kinetic models (pH = 3, As(V) = 50 mg/L) (b) for As(V) adsorption on amino-MIL-68(Al).
Figure 9
Figure 9
As(V) removal efficiency by amino-MIL-68(Al) and MIL-68(Al) for ten consecutive reuse cycles under optimal conditions (a). Interventional effect of anions on As(V) removal efficiency by amino-MIL-68(Al) (The oncentration of anions = 1 mM) (b).
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