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. 2020 Jul 29;21(1):524-539.
doi: 10.1080/14686996.2020.1782714.

As(V) and As(III) sequestration by starch functionalized magnetite nanoparticles: influence of the synthesis route onto the trapping efficiency

Mbolantenaina Rakotomalala Robinson  1 , Romain Coustel  1 , Mustapha Abdelmoula  1 , Martine Mallet  1
Affiliations

As(V) and As(III) sequestration by starch functionalized magnetite nanoparticles: influence of the synthesis route onto the trapping efficiency

Mbolantenaina Rakotomalala Robinson et al. Sci Technol Adv Mater. .

Abstract

We report the effect of the synthesis route of starch-functionalized magnetite nanoparticles (NPs) on their adsorption properties of As(V) and As(III) from aqueous solutions. NP synthesis was achieved by two different routes implying the alkaline precipitation of either a mixed Fe2+/Fe3+ salt solution (MC samples) or a Fe2+ salt solution in oxidative conditions (MOP samples). Syntheses were carried out with starch to Fe mass ratio (R) ranging from 0 to 10. The crystallites of starch-free MC NPs (14 nm) are smaller than the corresponding MOP (67 nm), which leads to higher As(V) sorption capacity of 0.3 mmol gFe -1 to compare with respect to 0.1 mmol gFe -1 for MOP at pH = 6. MC and MOP starch-functionalized NPs exhibit higher sorption capacities than a pristine one and the difference in sorption capacities between MOP and MC samples decreases with increasing R values. Functionalization tends to reduce the size of the magnetite crystallites and to prevent their agglomeration. Size reduction is more pronounced for MOP samples (67 nm (R0) to 12 nm (R10)) than for MC samples (14 nm (R0) to 9 nm (R10)). Therefore, due to close crystallite size, both MC and MOP samples, when prepared at R = 10, display similar As(V) (respectively, As(III)) sorption capacities close to 1.3 mmol gFe -1 (respectively, 1.0 mmol gFe -1). Additionally, according to the effect of pH on arsenic trapping, the electrostatic interactions appear as a major factor controlling As(V) adsorption while surface complexation may control As(III) adsorption.

Keywords: 212 Surface and interfaces; 301 Chemical syntheses / processing; 308 Materials resources / recycling; 501 Chemical analyses; 502 Electron spectroscopy; Magnetite; XPS; arsenic; polysaccharide; sorption capacity; zeta potential.

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Conflict of interest statement

No potential conflict of interest was reported by the authors.

Figures

None
Graphical abstract
Figure 1.
Figure 1.
XPS high-resolution spectra of O 1s and C 1s core level for MC (a) and MOP (b) samples prepared at different R = mstarch/mFe ratios. In each figure the O 1s and C 1s spectra of starch (St.) are also displayed.
Figure 2.
Figure 2.
Zeta potential as a function of pH for (a) MC (b) MOP nanoparticles synthesized with different R = mstarch/mFe ratios. In each figure the zeta potential curve of gelatinized starch (St.) is also displayed for comparison.
Figure 3.
Figure 3.
Comparison of As(V) adsorption percentage as a function of sorbent dose for (a) MC and (b) MOP samples synthesized with different R = mstarch/mFe ratios and corresponding As(V) sorption capacities for (c) MC and (d) MOP samples. Experimental conditions: 0.1 M KCl; pH = 6; initial concentration of As(V) is 0.1 mM.
Figure 4.
Figure 4.
Effect of contact time and R ratio on adsorption of As(V) on (a) MC and (b) MOP samples. The curves (c) and (d) displayed pseudo-second-order linear kinetic modeling of As(V) on MC and MOP samples respectively. Experimental conditions: 0.1 M KCl; pH = 6; initial concentration of As(V) is 0.1 mM.; adsorbent dose = 1.5 g L−1.
Figure 5.
Figure 5.
Adsorption isotherms of As(V) onto (a) MC (b) MOP samples synthesized at R = 0, 2 and 10; representation of the corresponding linear Langmuir relationship onto MC (c) and MOP (d) samples; representation of the corresponding linear Freundlich relationship onto MC (e) and MOP (f). Experimental conditions: 0.1 M KCl; pH = 6; adsorbent dose = 1.5 g L−1.
Figure 6.
Figure 6.
Adsorption isotherms of As(III) onto (a) MC (b) MOP samples synthesized at R = 0 and 10; representation of the corresponding linear Langmuir relationship onto MC (c) and MOP (d) samples; representation of the corresponding linear Freundlich relationship onto MC (e) and MOP (f). Experimental conditions: 0.1 M KCl; pH = 6; adsorbent dose = 1.5 g L−1.
Figure 7.
Figure 7.
pH influence on adsorption of As(V) and As(III) by (a) MC (b) MOP samples synthesized at R = 0; pH influence on adsorption of As(V) and As(III) by (c) MC (d) MOP samples synthesized at R = 10. Experimental conditions: 0.1 M KCl; pH = 6; adsorbent dose = 1.5 g L−1; [As]initial = 0,1 mM.
Figure 8.
Figure 8.
Effect of coexisting sulfate or phosphate anions on As(V) and As(III) adsorption percentage by MC and MOP samples synthesized with R = 0 and R = 10.
Figure 9.
Figure 9.
Room temperature Mössbauer spectrum of MC R0 magnetite before (black) and after (grey) As(V) adsorption.
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