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The amine group of the silane molecule is used to attach bioreceptors to the surface (Figure 1A); however, it can also form a weak hydrogen bond with the surface silanol group or with the silanol group of other silane molecules (Figure 1B). In addition, the silanol groups of different silane molecules can interact with each other, thereby forming polymeric structures (Figure 1B(5–7)). This procedure was repeated three times and 2% APTES in 100 ml of methanol was used to cover the NPs surfaces with silane molecules. They simply introduced 0.3 mL of APTES via an argon carrier gas (27 sccm) to a deposition chamber containing the oxide surfaces, which were hydroxylated with oxygen plasma.
Most NPs coated with APTES are used in applications such as for chemical sensors, cosmetic products (e.g., UV scattering effect in sun cream), drug delivery, magnetic resonance imaging, and bioimaging . Table 2 summarizes all the referenced solution-phase and vapor-phase processes and their monolayer characterization results. After deposition, the argon and APTES were removed, and the pressure was reduced to 75 × 10−7 Torr. Like YES CVD, there is some variation in the details of MLD processes, for example, they can be undertaken with or without high temperatures, a substrate dehydration, and nitrogen purges. This preceded the ten minute deposition of 500 L of APTES at 500 Torr, after which several nitrogen purges were used to remove excess silane. The desorption of APTES molecules from the surface was negligible in buffer solutions such as PBS compared to water.
A condensation reaction can happen between two APTES molecules and/or between the oxide surface and an APTES molecule . In the absence of water or if the water content is too low, the silanol formation could be incomplete 10,44,52,53. The water content determines the number of hydrolyzed groups during the hydrolysis step in the APTES molecule (hydrolysis of one, two, or three ethoxy groups) . The quality of the silane surface, including its morphology, strongly depends on the initial hydrolysis step, making it very critical . (A) Schematic representation of an APTES molecule, activation, and reaction with the hydroxylated oxide surface in an ideal situation. APTES has three functional reactive ethoxy groups and one amine group per one silane molecule (Figure 1).
The chemical reaction between the APTES and oxide nanoparticles’ (NP) surface is similar to the reaction with plain oxide surfaces. According to the molecular structure, an APTES monolayer should have an average chain length of ∼5–10 Å 5,44,64,65, a 0.5–0.8 nm thickness 44,53,66,67,68, an average density of 2.1–4.2 molecules per nm2 64,69 and a silanol group density of 5 per nm2 43,50. In an ideal situation, the attachment of the bioreceptors on an oxide surface via silane molecules should start with the hydrolysis of the silane molecules followed by condensation without the formation of additional bonds or different reaction routes.
List of methods used for inspecting and confirming APTES monolayer and/or multilayer formation on oxide surfaces. After the APTES grafting step, a post-deposition process (i.e., rinsing and baking) is usually performed to remove the non-covalently attached silane molecules without affecting the covalently-bonded silane molecules. As the result of the condensation reaction between silanol groups on the APTES molecule and -OH groups on a pre-treated oxide surface or between neighboring hydrolyzed APTES molecules, the formation of siloxane bonds occurs (Figure 1A). Due to this strong covalent bond, bioreceptors can be chemically attached to the silane layer via charge-to-charge interactions or bifunctional crosslinkers without disrupting the silane structure 16,17. Among all organosilanes, APTES is the most used silane molecule to functionalize oxide surfaces 5,6,7,8,9,10,11.
Amino-terminated organic layers were deposited onto silicon (Si) wafers and PS layers via 3-aminopropyltriethoxysilane (APTES) prepared in freshly hydrolysis solution. XPS results revealed the presence of Fe, O, C, and N, consistent with the development of interlinking silane molecules on a NP’s surface. Karade et al. conducted a ninhydrin colorimetric assay to monitor the monolayer formation through the quantification of the amine groups on the NPs . Additionally, APTES grafting on Fe2O3 magnetic NPs can prevent oxidative damage and play a role in the hydrophilicity or hydrophobicity of the NP surface, which is important for further drug conjugation through terminal amine groups. Moreover, the experimental grafting density was very close to the theoretically predicted APTES monolayer density. The study revealed that the equilibrium adsorption capacity was 301.2 mg/g for the highest grafting density during incubations at 70 °C using 2% APTES. The formation of more APTES monolayers on nanoparticles was proposed by Liu et al., where good quality silane layers were formed when the reaction was carried out at an elevated temperature using methanol/toluene mixed solvents .
Dissolving APTES in methanol with some water traces resulted in forming an APTES layer with 8.1 Å thickness based on spectroscopic ellipsometry measurements, which is close to the thickness of a monolayer . As previously mentioned, the amount of water in a solution and native -OH groups on an oxide substrate is critical in controlling the level of polymerization of silane molecules. XPS studies revealed that, compared to a deposition in toluene, the presence of N and C was three and two times greater, respectively, indicating more than one monolayer of APTES. Studies conducted by Pasternack et al. confirmed that lower APTES concentrations (0.1%) dissolved in toluene could create densely packed propyl chains on SiO2 when the reaction was carried out at 70 °C for less than 1 h. The deposition of APTES, in this case, was conducted on silicon wafers in a closed container (i.e., a toluene solution, and an APTES concentration range of 1–33%) backfilled with N2 gas.
Saini et al. used YES CVD to deposit monolayers of APTES onto oxide surfaces that were cleaned and hydroxylated with piranha solution without using hydration, dehydration, or N2 purges step . Another piece of research utilizing YES CVD used plasma-activated oxide surfaces, but instead of dehydrating them, they were hydrated with 500 L of water . After deposition, the non-covalently attached APTES molecules were removed using 6% acetic acid, effectively removing the multilayer and leaving the surface with an APTES monolayer, as proved by AFM and XPS surface analysis. Exposure of the oxide surfaces to a dry-cleaning process, such as oxygen plasma and UV-ozone cleaning for a certain period (5–30 min), has also been used for surface cleaning and activation 70,80.
Amino-functionalized organic films were prepared by self-assembling 3-aminopropyltriethoxysilane (APTES) on silicon wafers in either anhydrous toluene or phosphate-buffered saline (PBS) for varied deposition times. APTES films exhibit varying thicknesses and structural characteristics, with thicker films observed in anhydrous toluene (ranging from 10 Å to 144 Å) compared to thinner films produced in phosphate-buffered saline (8 Å to 13 Å). The investigation reveals that the formation and structure of APTES films on silicon substrates are significantly influenced by deposition conditions, including the choice of solvent and deposition time.
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