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The Stöber method for forming spherical silica colloids is well-established as one of the pillars of colloidal synthesis. In a modified form, it has been extensively used to deposit both porous and protective shells over metal nanomaterials. Current best-practice techniques require that the vitreophobic surface of metal nanoparticles be primed with a surface ligand to promote silica deposition. Although such techniques have proved highly successful in forming core-shell configurations, the site-selective deposition of silica onto preselected areas of faceted metal nanostructures has proved far more challenging. Herein, a primer-free TEOS-based synthesis is demonstrated that is capable of forming architecturally complex nanoframes and nanocages on the pristine surfaces of faceted gold nanostructures. The devised synthesis overcomes vitreophobicity using elevated TEOS concentrations that trigger silica nucleation along the low-coordination sites where gold facets meet. Continued deposition sees the emergence of a well-connected frame followed by the lateral infilling of the openings formed over gold facets. With growth readily terminated at any point in this sequence, the synthesis distinguishes itself in being able to achieve patterned and tunable silica depositions expressing interfaces that are uncorrupted by primers. The so-formed structures are demonstrated as template materials capable of asserting high-level control over synthesis and assembly processes by using the deposited silica as a mask that deactivates selected areas against these processes while allowing them to proceed elsewhere. The work, hence, extends the capabilities and versatility of TEOS-based syntheses and provides pathways for forming multicomponent nanostructures and nanoassemblies with structurally engineered properties.
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Avian influenza virus subtype H9N2 has the ability to infect birds and humans, further causing significant losses to the poultry industry and even posing a great threat to human health. Oral vaccine received particular interest for preventing majority infection due to its ability to elicit both mucosal and systemic immune responses, but their development is limited by the bad gastrointestinal (GI) environment, compact epithelium and mucus barrier, and the lack of effective mucosal adjuvants. Herein, we developed the dendritic fibrous nano-silica (DFNS) grafted with Cistanche deserticola polysaccharide (CDP) nanoparticles (CDP-DFNS) as an adjuvant for H9N2 vaccine. Encouragingly, CDP-DFNS facilitated the proliferation of T and B cells, and further induced the activation of T lymphocytes in vitro. Moreover, CDP-DFNS/H9N2 significantly promoted the antigen-specific antibodies levels in serum and intestinal mucosal of chickens, indicating the good ability to elicit both systemic and mucosal immunity. Additional, CDP-DFNS facilitate the activation of CD4 + and CD8 + T cells both in spleen and intestinal mucosal, and the indexes of immune organs. This study suggested that CDP-DFNS may be a new avenue for development of oral vaccine against pathogens that are transmitted via mucosal route.
Asunto(s)
Adyuvantes Inmunológicos , Pollos , Inmunidad Mucosa , Subtipo H9N2 del Virus de la Influenza A , Vacunas contra la Influenza , Gripe Aviar , Nanopartículas , Polisacáridos , Dióxido de Silicio , Animales , Subtipo H9N2 del Virus de la Influenza A/inmunología , Subtipo H9N2 del Virus de la Influenza A/efectos de los fármacos , Polisacáridos/administración & dosificación , Polisacáridos/farmacología , Polisacáridos/química , Polisacáridos/inmunología , Dióxido de Silicio/administración & dosificación , Dióxido de Silicio/química , Nanopartículas/administración & dosificación , Vacunas contra la Influenza/administración & dosificación , Vacunas contra la Influenza/inmunología , Inmunidad Mucosa/efectos de los fármacos , Gripe Aviar/prevención & control , Gripe Aviar/inmunología , Adyuvantes Inmunológicos/administración & dosificación , Adyuvantes Inmunológicos/farmacología , Administración Oral , Mucosa Intestinal/inmunología , Mucosa Intestinal/efectos de los fármacos , Anticuerpos Antivirales/sangre , Anticuerpos Antivirales/inmunologíaRESUMEN
This research focuses on the surface modification of Nd-Fe-B magnetic powder to enhance its thermal and oxidation resistance without compromising magnetic properties and to improve adhesion to the polymer binder for enhanced mechanical properties. A three-step surface modification process involving phosphatization treatment, tetraethyl orthosilicate (TEOS) application, and 3-aminopropyltriethoxysilane (APTES) grafting, was applied to the powder, which was then compounded with polyamide 12 and injection-moulded into cylinders and dog-bone-shaped tubes. The resulting magnets exhibited remanence (Br) of 487.6 mT, coercivity (Hci) of 727.7 kA/m, and energy product (BHmax) of 39.3 kJ/m3. The modified magnets demonstrated exceptional corrosion resistance and thermal stability, with less than 5% irreversible flux loss after exposure to hot water, temperature shock, and pressurised steam. Furthermore, the modified magnets displayed significantly higher tensile strength, elongation at break, and elastic modulus with improvements of 62%, 16.7%, and 19.9%, respectively, compared to the non-modified batch. Additionally, the modified batch showed a notable 52% increase in flexural stress during flexural testing. These findings underscore the potential of silane surface modifications in producing injection-moulded permanent magnets based on Nd-Fe-B alloy, extending their shelf life and enhancing their overall performance.
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Sol-gel production of hybrid materials has, to some extent, revolutionised materials' engineering and the way science and technology perceive the creation of new materials. Despite that, the method presents some limitations that are circumvented by radiation processing. Electron beam irradiation was used to promote synthesis of hybrid structures while using silanol-terminated PDMS, TEOS and TPOZ as precursors. Evaluation of the method's performance was executed by gel fraction determination, WDXRF and FTIR-ATR. Results showed that, although there is some pre-irradiation reactivity between precursors, radiolysis induces scission on multiple sites of precursor's structures, which induces hybrid network formation to a greater extent. Characterisation allowed determining electron beam irradiation to be effective in the creation of Si-O-Zr bonds, resulting in the production of a Class II hybrid material.
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The extensive utilization of nanoparticles in cancer therapies has inspired a new field of study called cancer nanomedicine. In contrast to traditional anticancer medications, nanomedicines offer a targeted strategy that eliminates side effects and has high efficacy. With its vast surface area, variable pore size, high pore volume, abundant surface chemistry and specific binding affinity, mesoporous silica nanoparticles (MPSNPs) are a potential candidate for cancer diagnosis and treatment. However, there are several bottlenecks associated with nanoparticles, including specific toxicity or affinity towards particular body fluid, which can cater by architecting core-shell nanosystems. The core-shell chemistries, synergistic effects, and interfacial heterojunctions in core-shell nanosystems enhance their stability, catalytic and physicochemical attributes, which possess high performance in cancer therapeutics. This review article summarizes research and development dedicated to engineering mesoporous core-shell nanosystems, especially silica nanoparticles and Fe3O4@Au nanoparticles, owing to their unique physicochemical characteristics. Moreover, it highlights state-of-the-art magnetic and optical attributes of Fe3O4@Au and MPSNP-based cancer therapy strategies. It details the designing of Fe3O4@Au and MPSN to bind with drugs, receptors, ligands, and destroy tumour cells and targeted drug delivery. This review serves as a fundamental comprehensive structure to guide future research towards prospects of core-shell nanosystems based on Fe3O4@Au and MPSNP for cancer theranostics.
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The search for new materials with improved properties for advanced applications is, nowadays, one of the most relevant and booming fields for scientists due to the environmental and technological needs of our society. Within this demand, hybrid siliceous materials, made out of organic and inorganic species (ORMOSILs), have emerged as an alternative with endless chemical and textural possibilities by incorporating in their structure the properties of inorganic compounds (i.e., mechanical, thermal, and structural stability) in synergy with those of organic compounds (functionality and flexibility), and thus, bestowing the material with unique properties, which allow access to multiple applications. In this work, synthesis using the sol-gel method of a series of new hybrid materials prepared by the co-condensation of tetraethoxysilane (TEOS) and 4-chlorophenyltriethoxysilane (ClPhTEOS) in different molar ratios is described. The aim of the study is not only the preparation of new materials but also their characterization by means of different techniques (FT-IR, 29Si NMR, X-ray Diffraction, and N2/CO2 adsorption, among others) to obtain information on their chemical behavior and porous structure. Understanding how the chemical and textural properties of these materials are modulated with respect to the molar percentage of organic precursor will help to envisage their possible applications: From the most conventional such as catalysis, adsorption, or separation, to the most advanced in nanotechnology such as microelectronics, photoluminescence, non-linear optics, or sensorics.
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Composite membranes consisting of microporous tantalum-doped silica layers supported on mesoporous alumina substrates were fabricated using chemical vapor deposition (CVD) in both thermal decomposition and counter-flow oxidative deposition modes. Tetraethyl orthosilicate (TEOS) was used as the silica precursor and tantalum (V) ethoxide (TaEO) as the tantalum source. Amounts of TaEO from 0 mol% to 40 mol% were used in the CVD gas mixture and high H2 permeances above 10-7 mol m-2 s-1 Pa-1 were obtained for all conditions. Close examination was made of the H2/CH4 and O2/CH4 selectivities due to the potential use of these membranes in methane reforming or partial oxidation of methane applications. Increasing deposition temperature correlated with increasing H2/CH4 selectivity at the expense of O2/CH4 selectivity, suggesting a need to optimize membrane synthesis for a specific selectivity. Measured at 400 °C, the highest H2/CH4 selectivity of 530 resulted from thermal CVD at 650 °C, whereas the highest O2/CH4 selectivity of 6 resulted from thermal CVD at 600 °C. The analysis of the membranes attempted by elemental analysis, X-ray photoelectron spectroscopy, and X-ray absorption near-edge spectroscopy revealed that Ta was undetectable because of instrumental limitations. However, the physical properties of the membranes indicated that the Ta must have been present at least at dopant levels. It was found that the pore size of the resultant membranes increased from 0.35 nm for pure Si to 0.37 nm for a membrane prepared with 40 mol% Ta. Similarly, an increase in Ta in the feed resulted in an increase in O2/CH4 selectivity at the expense of H2/CH4 selectivity. Additionally, it resulted in a decrease in hydrothermal stability, with the membranes prepared with higher Ta suffering greater permeance and selectivity declines during 96 h of exposure to 16 mol% H2O in Ar at 650 °C.
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It is a novel idea to fabricate wood-inorganic composites by utilizing the transpiration of bionic trees to realize the self-assembly of inorganic precursors in wood formation. We selected a 10-year-old poplar and diffused the solvent or sol containing SiO2 precursor into the xylem via the slow-release drip method. In combination with the moisture in xylem, reactions such as hydrolysis, polycondensation and self-assembly were induced in order to form wood inorganic composites. It was found, through microscopic observation, that such inorganic substances were yellowish brown and widely existed in vessels, wood fibers and ray cells. For the new grown wood, the fiber-tissue ratio and cell wall thickness underwent an increase, while the vessel diameter and tissue ratio experienced a decline. Moreover, such change was related to the concentration of precursors. EDS analysis proved that the elemental composition of sediments in wood cells was C, O, Si, K and Ca. XPS confirmed that the newly formed wood contained silicon oxide, illustrating that the standing tree slow-release drip technology could induce wood to fabricate inorganic composites.
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In this work, new adsorbent composites from the silica precursor tetraethyl orthosilicate (TEOS) and chitosan have been successfully synthesized, denominated 20%Chi, 30%Chi and 40%Chi. The composites presented enhanced chemical and physical characteristics, with emphasis on the high surface areas between 374.94 m2/g to 886.31 m2/g. The application of the composites in the model system (TY - Tartrazine yellow dye), presented adsorption capacities dependent on the amount of chitosan in the composite (40%Chi > 30%Chi > 20%Chi). However, from the experimental data of the constituent materials, 30%Chi provided the greatest increase in the adsorption capacity in the monolayer, with values of 36%. This demonstrates that the amount of chitosan in the compound alters the arrangement of adsorption sites. The 30%Chi composite presented life cycle superior to 10 reuse cycles.
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In the microscale, bacteria with helical body shapes have been reported to yield advantages in many bio-processes. In the human society, there are also wisdoms in knowing how to recognize and make use of helical shapes with multi-functionality. Herein, we designed atypical chiral mesoporous silica nano-screws (CMSWs) with ideal topological structures (e.g., small section area, relative rough surface, screw-like body with three-dimension chirality) and demonstrated that CMSWs displayed enhanced bio-adhesion, mucus-penetration and cellular uptake (contributed by the macropinocytosis and caveolae-mediated endocytosis pathways) abilities compared to the chiral mesoporous silica nanospheres (CMSSs) and chiral mesoporous silica nanorods (CMSRs), achieving extended retention duration in the gastrointestinal (GI) tract and superior adsorption in the blood circulation (up to 2.61- and 5.65-times in AUC). After doxorubicin (DOX) loading into CMSs, DOX@CMSWs exhibited controlled drug release manners with pH responsiveness in vitro. Orally administered DOX@CMSWs could efficiently overcome the intestinal epithelium barrier (IEB), and resulted in satisfactory oral bioavailability of DOX (up to 348%). CMSWs were also proved to exhibit good biocompatibility and unique biodegradability. These findings displayed superior ability of CMSWs in crossing IEB through multiple topological mechanisms and would provide useful information on the rational design of nano-drug delivery systems.
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Orthopedic implants account for 99% of orthopedic surgeries, however, orthopedic implant-related infection is one of the most serious complications owing to the potential for limb-threatening sequelae and mortality. Current antibiotic treatments still lack the capacity to target bone infection sites, thereby resulting in unsatisfactory therapeutic effects. Here, the bone infection site targeting efficacy of D6 and UBI29-41 peptides was investigated, and bone-and-bacteria dual-targeted nanoparticles (NPs) with D6 and UBI29-41 peptides were first fabricated to target bone infection site and control the release of vancomycin in bone infection site. The results of this study demonstrated that the bone-and-bacteria dual-targeted mesoporous silica NPs exhibit excellent bone and bacteria targeting efficacy, excellent biocompatibility and effective antibacterial properties in vitro. Furthermore, in a rat model of orthopedic implant-related infection with methicillin-resistant Staphylococcus aureus, the growth of bacteria was evidently inhibited without cytotoxicity, thus realizing the early treatment of implant-related infection. Hence, the bone-and-bacteria dual-targeted molecule-modified NPs may target bacteria-infected bone sites and act as ideal candidates for the therapy of orthopedic implant-related infections.
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This study aimed at evaluating the effect of hydroxyapatite (HAp) nanosized structures and nanoparticles of hydrophilic silica as modifiers of both acid- and alkaline-catalysed tetraethoxysilane (TEOS)-based products for the consolidation of carbonate stones. Their initial effectiveness and some compatibility aspects were assessed in a porous limestone (sound and artificially aged Ançã stone samples) and two types of treatment (capillary absorption and brushing). The studied products were examined by scanning electron microscopy (SEM) and micro-Raman spectroscopy. Their depth of penetration and strengthening effect were evaluated through drilling resistance. Their action on the substrate was also further assessed by non-destructive methods based on colour variation and Shore-D hardness. Treated stone samples were dissimilarly affected by the tested treatments and exhibited a significant increase in strength with a low risk of over-strengthening. Adequate in-depth penetration patterns, as well as colour compatibility with the substrate were obtained with some of the prepared formulations through two types of treatment, both in sound and aged stone samples. The potential most effective treatments with the lowest colour change were obtained with the acid-catalysed TEOS-based products modified with HAp nanosized structures.
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The objective of this study was to investigate the spatial variation of volatile organic compounds and antioxidant activity of turmeric essential oils (TEOs) harvested from four provinces of China. The major chemical components of these TEOs were analyzed using headspace solid-phase micro-extraction gas chromatography-mass spectrometry. More than forty volatile organic compounds in TEOs were identified, which accounted for 82.09-93.64% of the oil components. The relative abundances of the main volatile organic compounds in TEOs at the genus level were visualized by a heat map. The antioxidant activity of the TEOs of five different origins was characterized by the DPPH free radical scavenging activity, in which the antioxidant activity of the TEOs from Guangxi was superior to those of other sources. Furthermore, the IC50 values of the antioxidants TEOs collected from Guangxi, Sichuan, Yunnan, Changting, and Liancheng were 33.30, 42.5, 35.22, 63.27, and 39.96 mg/mL, respectively, which indicated the excellent free radical scavenging activity of those TEOs. Therefore, the TEOs might be considered as a natural antioxidant with potential applications in food and pharmaceutical industries.
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Diffusion dialysis (DD) using anion exchange membranes (AEM) is an effective process for acid recovery and requires the preparation of suitable materials for AEMs, characterized by unique ions transport properties. In this work, novel AEMs composed of quaternized diaminobutane (QDAB) and poly(vinyl alcohol) (PVA) were cross-linked by tetraethoxysilane (TEOS) via the sol-gel process. The prepared AEMs were systematically characterized by Fourier-transform infrared (FTIR) spectroscopy, ion-exchange capacity (IEC) analysis, thermo gravimetric analysis (TGA), water uptake, linear expansion ratio (LER), and mechanical strength determination, scanning electron microscopy (SEM), and DD performance analysis for acid recovery using a hydrochloric acid/iron chloride (HCl/FeCl2) aqueous mixture and varying the QDAB content. The prepared AEMs exhibited IEC values between 0.86 and 1.46 mmol/g, water uptake values within 71.3 and 47.8%, moderate thermal stability, tensile strength values in the range of 26.1 to 41.7 MPa, and elongation from 68.2 to 204.6%. The dialysis coefficient values were between 0.0186 and 0.0295 m/h, whereas the separation factors range was 24.7-44.1 at 25 °C. The prepared membranes have great potential for acid recovery via diffusion dialysis.
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The boron difluoride complex is known as an extraordinary class of fluorescent dyes, which has attracted research interest because of its excellent properties. This article reports the optical properties such as absorption, fluorescence, molar absorptivity, and photo-physical parameters like dipole moment, and oscillator strength of new fluorescent organic dye based on boron difluoride complex 2-(1-(difluoroboraneyl)-1,2-dihydroquinolin-2-yl)-2-(1-methylquinoxalin-2-ylidene) acetonitrile (DBDMA). The spectral characterization of the dye was measured in sol-gel glass, photosol-gel, and organic-inorganic matrices. The absorption and fluorescence properties of DBDMA in sol-gel glass matrices were compared with each other. Compared with the classical sol-gel, it was noticed that the photosol-gel matrix is the best one with immobilized DBDMA. In the latter, a large stokes shift was obtained (97 nm) and a high fluorescence quantum yield of 0.5. Special attention was paid to the addition of gold NPs into the hybrid material. The fluorescence emission intensity of the DBDMA with and without gold nanoparticles in different solid media is described, and that displayed organic-inorganic matrix behavior is the best host.
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Chitosan-based films have a diverse range of potential applications but are currently limited in terms of commercial use due to a lack of methods specifically designed to produce thin films in high volumes. To address this limitation directly, hydrogels prepared from chitosan, chitosan-tetraethoxy silane, also known as tetraethyl orthosilicate (TEOS) and chitosan-glutaraldehyde have been used to prepare continuous thin films using a slot-die technique which is described in detail. By way of preliminary analysis of the resulting films for comparison purposes with films made by other methods, the mechanical strength of the films produced was assessed. It was found that as expected, the hybrid films made with TEOS and glutaraldehyde both show a higher yield strength than the films made with chitosan alone. In all cases, the mechanical properties of the films were found to compare very favorably with similar measurements reported in the literature. In order to assess the possible influence of the direction in which the hydrogel passes through the slot-die on the mechanical properties of the films, testing was performed on plain chitosan samples cut in a direction parallel to the direction of travel and perpendicular to this direction. It was found that there was no evidence of any mechanical anisotropy induced by the slot die process. The examples presented here serve to illustrate how the slot-die approach may be used to create high-volume, high-area chitosan-based films cheaply and rapidly. It is suggested that an approach of the type described here may facilitate the use of chitosan-based films for a wide range of important applications.
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We immobilized a fungal laccase with only two spatially close lysines available for functionalization into macrocellular Si(HIPE) monoliths for the purpose of continuous flow catalysis. Immobilization (30-45 % protein immobilization yields) was obtained using a covalent bond forming reaction between the enzyme and low glutaraldehyde (0.625 % (w/w)) functionalized foams. Testing primarily HBT-mediated RB5 dye decolorization in continuous flow reactors, we show that the activity of the heterogeneous catalyst is comparable to its homogeneous counterpart. More, its operational activity remains as high as 60 % after twelve consecutive decolorization cycles as well as after one-year storage, performances remarkable for such a material. We further immobilized two variants of the laccase containing a unique lysine: one located in the vicinity of the substrate oxidation site (K157) and one at the opposite side of this oxidation site (K71) to study the effect of the proximity of the Si(HIPE) surface on enzyme activity. Comparing activities on different substrates for monoliths with differentially oriented catalysts, we show a twofold discrimination for ABTS relative to ascorbate. This study provides ground for the development of neo-functionalized materials that beyond allowing stability and reusability will become synergic partners in the catalytic process.
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Coronavirus disease 2019 (COVID-19) is largely threatening global public health, social stability, and economy. Efforts of the scientific community are turning to this global crisis and should present future preventative measures. With recent trends in polymer science that use plasma to activate and enhance the functionalities of polymer surfaces by surface etching, surface grafting, coating and activation combined with recent advances in understanding polymer-virus interactions at the nanoscale, it is promising to employ advanced plasma processing for smart antiviral applications. This trend article highlights the innovative and emerging directions and approaches in plasma-based surface engineering to create antiviral polymers. After introducing the unique features of plasma processing of polymers, novel plasma strategies that can be applied to engineer polymers with antiviral properties are presented and critically evaluated. The challenges and future perspectives of exploiting the unique plasma-specific effects to engineer smart polymers with virus-capture, virus-detection, virus-repelling, and/or virus-inactivation functionalities for biomedical applications are analysed and discussed.
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Hybrid silica xerogels combine the properties of organic and inorganic components in the same material, making them highly promising and versatile candidates for multiple applications. They can be tailored for specific purposes through chemical modifications, and the consequent changes in their structures warrant in-depth investigation. We describe the synthesis of three new series of organochlorinated xerogels prepared by co-condensation of tetraethyl orthosilicate (TEOS) and chloroalkyltriethoxysilane (ClRTEOS; R = methyl [M], ethyl [E], or propyl [P]) at different molar ratios. The influence of the precursors on the morphological and textural properties of the xerogels was studied using 29Si NMR (Nuclear Magnetic Resonance), FTIR (Fourier-Transform Infrared Spectroscopy), N2, and CO2 adsorption, XRD (X-ray Diffraction), and FE-SEM (Field-Emission Scanning Electron Microscopy). The structure and morphology of these materials are closely related to the nature and amount of the precursor, and their microporosity increases proportionally to the molar percentage of ClRTEOS. In addition, the influence of the chlorine atom was investigated through comparison with their non-chlorinated analogues (RTEOS, R = M, E, or P) prepared in previous studies. The results showed that a smaller amount of precursor was needed to detect ordered domains (ladders and T8 cages) in the local structure. The possibility of coupling self-organization with tailored porosity opens the way to novel applications for this type of organically modified silicates.
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This study presents an innovative approach for the preparation of Fe3O4 nanoparticles covered with SiO2 shell (denoted as Fe-Si-MNP), which were used to recover oil recovery from oil-in-water emulsion (O/W-emul). The Fe-Si-MNP were prepared with differing silica layer thicknesses (5 nm [Fe-Si-1], 8 nm [Fe-Si-2], 10 nm [Fe-Si-3], and 15 nm [Fe-Si-4]) and tested for the percentage of oil separation (%Soil) under different dosages (DMNP), oil concentration (Doil), surfactant dosages (Dsur), and pH. The Fe-Si-MNP exhibited excellent %Soil, reliable stability, and high magnetization values ranging between 46.1 and 80.2 emu/g. adding a 5 nm silica layer on the surface of the Fe-Si-MNP (i.e., Fe-Si-1) protected them from oxidation conditions, extended their service life, and achieved a %Soil of â¼96.3%. The %Soil slightly decreased to â¼92% with an alkaline pH or when the thickness of the silica layer increased to ≥10 nm. The %Soil was 90.5%, 89.5%, and 87.5% for Fe-Si-2, Fe-Si-3, and Fe-Si-4, respectively. Increasing the water salinity from 0.1 to 0.5 M slightly improved the %Soil for the tests carried out with a Doil of 100 mg/L to 93.3%, 90.3%, and 86.3% for Fe-Si-2, Fe-Si-3, and FeSi-4, respectively. The highest %Soil achieved with Fe- Si-1 Fe-Si-2 and Fe-Si-3 was >95%, 95% and 92%, respectively. The Fe-Si-MNP exhibited a high recyclability for 9 cycles with the lowest %Soil â¼80%. The results suggest that the structure and properties of the Fe-Si-MNP can be manipulated to achieve a high oil recovery, easy separation, and extended service life.