Synthesis of granulated hydrophobic magnetic sorbents and composite sponges based on Fe3O4/Zn-Al-LDH for oil pollution removal

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Abstract

In this study, we present a novel surface modification approach for magnetic composite materials based on Fe3O4/Zn-Al layered double hydroxides (LDH) to enhance their hydrophobic properties. We have systematically investigated the interaction mechanisms between various surfactants (stearate, oleate, and sodium dodecyl sulfate) and the Fe3O4/Zn-Al-LDH surface. Our research examined how ethanol-mediated hydrophobization affects the material's porous and crystalline structure. We developed innovative synthesis routes for both granulated and sponge-like magnetic sorbents utilizing melamine-formaldehyde resin as a binding matrix. Under optimized conditions, the resulting Fe3O4-LDH-ST granulated sorbents and MEL-Fe3O4/LDH-ST sponge-like materials demonstrated exceptional oil sorption capacities of 0.60 and 21.36 g/g, respectively, combined with significant magnetic susceptibility, enhanced hydrophobicity, and excellent regeneration potential. These engineered materials show promise for marine oil spill remediation and environmental monitoring applications.

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About the authors

N. P. Ivanov

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

O. O. Shichalin

Sakhalin State University

Author for correspondence.
Email: ivanov.np@dvfu.ru
Russian Federation, Yuzhno-Sakhalinsk

V. L. Rastorguev

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

V. M. Zakharenko

Elyakov Pacific Institute of Bioorganic Chemistry, Far Eastern Branch of the Russian Academy of Sciences

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

A. L. Myagchilov

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

P. A. Marmaza

Sakhalin State University

Email: ivanov.np@dvfu.ru
Russian Federation, Yuzhno-Sakhalinsk

Ya. G. Zernov

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

S. M. Pisarev

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

I. Yu. Buravlev

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

E. K. Papynov

Far Eastern Federal University

Email: ivanov.np@dvfu.ru
Russian Federation, Vladivostok

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Supplementary files

Supplementary Files
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2. Fig. 1. Diffraction patterns of the original and modified granulated sorption materials based on Fe3O4/Zn-Al-LDH.

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3. Fig. 2. Differential curves of pore size distribution in the original and modified granular sorption materials based on Fe3O4/Zn-Al-LDH.

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4. Fig. 3. SEM images and EDS maps of the elemental distribution over the surface of the original and modified granular sorption materials: a – Fe3O4/SDG, b – Fe3O4/SDG-OL-0.01, Fe3O4/SDG-ST-0.01, Fe3O4/SDG-DOD-0.01.

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5. Fig. 4. Sorption capacity in relation to oil, motor oil and water for the original and modified granulated sorption materials based on Fe3O4/Zn-Al-LDH.

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6. Fig. 5. Water contact angles for spongy hydrophobic magnetic composites: a – MEL-Fe3O4/SDG-OL-0.01, b – MEL-Fe3O4/SDG-OL-0.05.

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7. Fig. 6. Sorption capacity in relation to oil, motor oil and water for the original and modified spongy sorption materials MEL-Fe3O4/SDG.

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8. Fig. 7. Sorption indices in relation to oil in multiple adsorption–desorption cycles for modified granular sorption materials MEL-Fe3O4/SDG-OL-0.01 and -0.05.

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9. Fig. 8. Sorption indices in relation to oil in multiple adsorption–desorption cycles for modified spongy sorption materials MEL-Fe3O4/SDG-OL-0.01: a – sorption capacity, b – water contact angle after five cycles.

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10. Fig. 9. Proposed mechanism of surface hydrophobization of LDH using the example of interaction with sodium stearate.

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