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US-12624143-B2 - Polyamide-functionalized silicon carbide (SiC) nanoparticles-based ceramic membrane for separating an oil and water mixture

US12624143B2US 12624143 B2US12624143 B2US 12624143B2US-12624143-B2

Abstract

A ceramic membrane includes an alumina (Al 2 O 3 ) layer; and a polyamide nanocomposite layer at least partially covering a surface of the alumina layer. The polyamide nanocomposite layer contains polyamide-functionalized silicon carbide (SiC) nanoparticles having an average particle size of 0.1 to 1 micrometer (μm), an amine-functionalized SiC moiety, an acyl aryl moiety, and a piperazine moiety. The amine-functionalized SiC moiety contains a SiC core and an amine functionalized silicon dioxide (SiO 2 ) shell covering the SiC core. The amine-functionalized SiC moiety is covalently bonded to the piperazine moiety via the acyl aryl moiety; and the amine functionalized SiO 2 shell contains at least one amino group containing structural unit that is covalently bonded to the SiO 2 shell.

Inventors

  • Umair Baig
  • Abdul Waheed

Assignees

  • KING FAHD UNIVERSITY OF PETROLEUM AND MINERALS

Dates

Publication Date
20260512
Application Date
20230601

Claims (12)

  1. 1 . A method of making a ceramic membrane comprising an alumina (Al 2 O 3 ) layer, a polyamide nanocomposite layer at least partially covering a surface of the alumina layer, wherein the polyamide nanocomposite layer comprises polyamide-functionalized silicon carbide (SiC) nanoparticles having an average particle size of 0.1 to 1 micrometer (μm), wherein the polyamide-functionalized SiC nanoparticles comprise an amine-functionalized SiC moiety, an acyl aryl, and a piperazine moiety, wherein the amine-functionalized SiC moiety comprises a SiC core and an amine functionalized silicon dioxide (SiO 2 ) shell covering the SiC core, wherein the amine-functionalized SiC moiety is covalently bonded to the piperazine moiety via the acyl aryl moiety, and wherein the amine functionalized SiO 2 shell comprises at least one amino group containing structural unit that is covalently bonded to the SiO 2 shell, the method comprising: calcining silicon carbide particles at a temperature of 600 to 800 degree Celsius (° C.) in the presence of oxygen to form a first composite having a silicon carbide core surrounded by a silicon dioxide shell; dispersing the first composite in an alcohol solvent and mixing with an aminosilane compound to form a second composite; washing the second composite and drying to form an amine-functionalized silicon carbide composite; mixing the amine-functionalized silicon carbide composite and a piperazine-containing solution to form a dispersion; dipping the alumina layer into a surfactant solution to form a treated alumina layer; passing the dispersion through the treated alumina layer to from form an impregnated alumina layer containing the amine-functionalized silicon carbide composite particles and piperazine molecules; and dipping the impregnated alumina layer in an acyl aryl chloride solution and reacting to form the polyamide nanocomposite layer covering the surface of the alumina layer thereby forming the ceramic membrane.
  2. 2 . The method of claim 1 , wherein the alcohol solvent comprises at least one of isopropanol, ethanol, and methanol.
  3. 3 . The method of claim 1 , wherein the aminosilane compound comprises at least one of N-(6-aminohexyl)aminomethyltriethoxysilane, bis(3-triethoxysilylpropyl)amine, 3-aminopropyl(diethoxy)methylsilane, 3-Aminopropyltrimethoxysilane (APTMS), and 3-aminopropyltriethoxysilane (APTES).
  4. 4 . The method of claim 1 , wherein the first composite is present in the alcohol solvent at a concentration of 5 to 20 milligrams per milliliter (mg/mL).
  5. 5 . The method of claim 1 , wherein the aminosilane compound is present in the alcohol solvent at a concentration of 1 to 10 vol. % based on a total volume of the alcohol solvent.
  6. 6 . The method of claim 1 , wherein the amine-functionalized silicon carbide composite has an average particle size in a range of 20 to 600 nm.
  7. 7 . The method of claim 1 , wherein the amine-functionalized silicon carbide is present in the dispersion at a concentration of 0.01 to 0.5 g/mL based on a total volume of the dispersion.
  8. 8 . The method of claim 1 , wherein the piperazine is present in the piperazine-containing solution at a concentration of 0.5 to 5 g/mL based on a total volume of the piperazine-containing solution.
  9. 9 . The method of claim 1 , wherein the surfactant solution comprises at least one surfactant selected from the group consisting of sodium dodecyl sulfate (SDS), sorbitan monolaurate, and dodecyltrimethylammonium bromide.
  10. 10 . The method of claim 1 , wherein the treated alumina layer formed the surfactant solution is placed on a support disc in a dead end filtration cell; wherein the dead end filtration cell is in the shape of a vertical cylinder having a gas inlet, a permeate outlet, a top portion, a body portion, and a bottom portion; wherein the gas inlet is located on the outer surface of the top portion; wherein the permeate outlet is located on the outer surface of the bottom portion; wherein the top portion is in fluid communication with the bottom portion via the body portion of the dead end filtration cell; wherein the bottom portion comprises the support disc and a cell bottom; and wherein the support disc is above and adjacent to the cell bottom.
  11. 11 . The method of claim 1 , wherein the acyl aryl chloride is present in the acyl aryl chloride solution at a concentration of 0.05 to 0.5 g/mL based on a total volume of the acyl aryl chloride solution.
  12. 12 . The method of claim 1 , wherein the acyl aryl chloride comprises at least one selected from the group consisting of terephthaloyl chloride, phthaloyl dichloride, and isophthaloyl dichloride.

Description

STATEMENT REGARDING PRIOR DISCLOSURE BY THE INVENTORS Aspects of this technology are described in “Facile fabrication of ceramic-polymeric nanocomposite membrane with special surface wettability using amino decorated NH2—SiO2@SiC nanopowder for production of clean water from oily wastewater,” Process Safety and Environmental Protection, Volume 171, 694-704, which is incorporated herein by reference in its entirety. STATEMENT OF ACKNOWLEDGEMENT This research was supported by the Interdisciplinary Research Center for Membranes and Water Security under the project INMW2207 at King Fahd University of Petroleum and Minerals (KFUPM), Saudi Arabia. BACKGROUND Technical Field The present disclosure is directed to a ceramic membrane, particularly a polyamide-functionalized silicon carbide (SiC) nanoparticles-based ceramic membrane for separating an oil and water mixture. Description of Related Art The “background” description provided herein is to present the context of the disclosure generally. Work of the presently named inventors, to the extent it is described in this background section, as well as aspects of the description that may not otherwise qualify as prior art at the time of filing, are neither expressly nor impliedly admitted as prior art against the present invention. Oily wastewaters from industrial processes contain oil in three forms: floated and dispersed oil (which accounts for approximately 90% of the oil content by weight), emulsified oil (about 10% by weight), and dissolved oil (only 0.5% by weight). The removal of floated and dispersed oil droplets is easier as their larger size (>10 μm) allows for mechanical removal. On the other hand, separating emulsified oil from oily wastewaters is extremely difficult due to the presence of emulsifiers that reduce the surface tension between the oil and water interface, making separation challenging. Emulsified oil, also known as oil-in-water (O/W) emulsion, is produced by several industries, including oil and gas, oil transportation and refining, cosmetics, and textiles. Conventional treatment methods for O/W emulsions include dissolved air flotation, coalescence separation, and gravity separation. However, these methods are often inefficient, particularly when the emulsifiers completely emulsify the oil droplets. Membrane-based technologies have been developed to tackle the challenge of treating the large volume of oily wastewater generated by the oil and gas industry. Ultrafiltration polymeric membranes have been developed for oil/water separation. However, polymeric membranes are susceptible to fouling, as oil can deposit on their surfaces. Superhydrophilic/superoleophilic membranes have been developed with fine-tuned wettability features. A chitosan-based membrane prepared by incorporating UiO-66-NH2 in the membrane is known. The membrane, after incorporation of UiO-66-NH2, showed improved performance compared to the unmodified membrane. Polymeric membranes, however, often exhibit reduced chemical and thermal stability when used in real-world industrial processes for separating oil form oil-in-water (O/W) emulsion. Due to the stability of ceramic membranes under experimental and real-world oil-in-water (O/W) emulsion separation conditions, ceramic membranes, such as silica (SiO2), alumina (Al2O3), Zirconia (ZrO2), and titania (TiO2), have emerged as an attractive alternative to polymeric membranes. Despite their stability, ceramic membranes are prone to two types of fouling: reversible and irreversible. The reversible fouling is due to the deposition of foulants on the membrane surface followed by penetration of foulants in the membrane's pores, which results in blockage of the pore, leading to blockage of membrane pores. The blockage of the pores leads to a considerable decline in permeate flux. The reversible fouling can be removed by hydraulic washing, such as a back flush or cross flush. Conversely, irreversible fouling is challenging to be removed by simple hydraulic washing because the foulants are tightly bound to the membrane surface. Hence, chemical cleaning is carried out to restore the membrane performance, which may damage the membrane integrity and reduces the life span of the ceramic membranes. A combination of humic acid and Bovine serum albumin (BSA) model foulants caused irreversible fouling of the ZrO2@TiO2 membrane (Munla, L., Peldszus, S., Huck, P. M., 2012. Reversible and irreversible fouling of ultrafiltration ceramic membranes by model solutions. J. Am. Water Works Assoc. 104, E540-E554). In addition to the oil present in O/W emulsions, the other components also contribute to membrane fouling. Emulsion-stabilizing surfactants, for instance, have been found to affect the fouling profile of the membranes. The surfactant charge was found to play a crucial role in controlling membrane fouling. It was found that the surfactant with an opposite charge to the membrane surface reduces the membrane fouling. This may be attributed to the