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Article

Modification of Liquid Glasses Is a Key Factor in the Technology of Obtaining Hybrid Compositions and Coatings with Anticorrosive Properties

by
Pavel Razgovorov
1,
Svetlana Loginova
1,
Natalia Politaeva
2,*,
Ksenia Velmozhina
2 and
Polina Shinkevich
2
1
Institute of Civil and Transport Engineers, Yaroslavl State Technical University, Moskovsky Prosp., 88, Yaroslavl 150023, Russia
2
Institute of Civil Engineering, Peter the Great St. Petersburg Polytechnic University, Polytechnic Str., 29, Saint Petersburg 195220, Russia
*
Author to whom correspondence should be addressed.
Coatings 2023, 13(6), 974; https://doi.org/10.3390/coatings13060974
Submission received: 15 April 2023 / Revised: 3 May 2023 / Accepted: 16 May 2023 / Published: 23 May 2023
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Abstract

:
The aim of the work was to investigate the prospects of imparting valuable physical and chemical properties, such as corrosion resistance, impact and bending strength, adhesion and storage stability, to hybrid systems of potassium and sodium silicates by modification with organic compounds. Here, we present the results of worldwide activities of scientific teams studying the manufacturing technology of modified liquid glass anticorrosive coatings used in chemical, petrochemical industry and modern construction. The authors theoretically and economically justified and put into practice novel organic and inorganic compositions with increased viability. The durable and waterproof coatings with good adhesion to various substrates (non-ferrous metals, steel, plastered surface and wood) were obtained. The authors demonstrate the possibility of recycling of zinc-containing rongalite production wastes and sludge pastes of electrochemical productions containing alkali and alkaline-earth metal cations by including them into the composition instead of pigmenting solid-phase components. We propose a technological route for obtaining anticorrosion coatings to protect aluminum and its alloys operated in a zone of elevated (up to 673 K) temperatures.

1. Introduction

Over the 30–40 years [1,2,3,4,5,6,7] and especially in the last 3 years [8,9,10,11,12], a considerable body of knowledge about the prospects of introducing organosilicon and organic compounds into alkali metal silicate solutions has been accumulated worldwide. There is evidence [1,2,3] that high-strength organo–inorganic compositions can be produced from liquid glasses comprising hydrolyzed siloxanes (1:1) or mixtures of the above compounds with urea-containing resins. Half a century ago, A.T. Kuznetsov [4], introducing a mixture of sodium ethyl siliconate and sulphate-alcohol bard into silicate compositions, discovered that they are water resistant and excellent for protecting metal surfaces and concrete (especially when exposed to high loads in oxidized environments). Kondo Khidetoshi and Koschii Tago [5], when identifying new physicochemical properties of systems in which aminosilanes were added and the silicon atom was conjugated to two or more hydroxyl groups, explained the achieved anticorrosive effect by the increased concentration of silicate anions in the mixture of components.
However, the most significant problem is that most liquid glass compositions, especially sodium ones, cannot be stored for more than 24 h. Exceeding this time limit causes it to turn into a solid mass in the air, making it unsuitable for creating elastic protective coatings. It would seem that William J. O’ Malley and A. Howard Vaugh [6] achieved a partial solution to the above problem by using products of controlled condensation of silanols and dispersing silica nanoparticles (10–20 nm) in them in a finely tuned ratio (25–45 wt%); however, this advantage did not provide the necessary water resistance, and unfortunately, there is no information on how these hybrid compounds can be used to form durable coatings.
A review of the worldwide literature on the development of hybrid liquid glass anticorrosive materials shows that the introduction of hydrophobic sodium alkylsiliconates provides strong and water-resistant compositions, which are suitable mainly for the protection of mineral surfaces [4,7,13,14].
The modification of liquid glasses by Japanese [15], Russian [16] and Ukrainian researchers [17] in silicone–organic media in the presence of alcohols increases the stability of silicate systems in aggressive media. However, there is no question of their stability in time, since the hydroxyl alcohol groups must be bound in order to avoid coagulation.
The study of structure formation of silicate systems containing various alkali metal atoms and kept at normal conditions (293 K, 1 atm.) shows that gelling processes actively proceed during 1 week (6–7 days) [18]. Such solutions are then stable up to τ = 180 days (Figure 1); their behavior falls within the typical provisions of the theory of anionic processes.
The straight lines obtained by the extension of two main segments on given parabolic dependence of structural viscosity of lithium, sodium and potassium silicates from holding time at 293 K (Figure 2, curves 1–3) allow us to reveal the point of jellification. It makes it possible to assess the film-forming properties of silicate systems with the inclusion of mentioned metal cations.
Potassium silicate, however, gains viscosity much faster than sodium silicate. There are three stages, each of which has a different rate of viscosity build up from the previous stage. Thus, the viscosity (μ) of lithium silicate during the first week of exposure in the presence of tetraethoxysilane changes in a gentle straight line (2.9–3.1) × 10−6 m2∙s−1. At the second stage (τ = 8–20 days), the viscosity already increases appreciably, from 3.1 to 4.5 × 10−6 m2∙s−1 (curve bend). The third stage (τ = 20–25 days) is characterized by a strong rise in viscosity to 6.5 × 10−6 m2∙s−1 Water absorption by the aggregates takes place. The microgel concentration increases most rapidly at the dynamic viscosity sections of sodium (Figure 2, Curve 2) and especially of potassium liquid glass [17] (Figure 2, Curve 3).
The formation of insoluble products involving alcohols should be considered separately. For example, amines of the general formula RmHnN are the modifiers for mixtures of silicate with polyvinyl alcohol [19]. In this case, R represents C1–3 alkyls, m = 1–3 and n = 3 − m, which do not precipitate an alcohol. The compound is formed through a hydroxyl alcohol group and a nitrogen atom:
R3N: + −CH2−CH → −CH2−CH
            |      |
        OH  R3N:OH
The formation of compound (1) is accompanied by a reduction in the viscosity of the solution. The number of intermolecular bonds involving polyvinyl alcohol also decreases, which is confirmed by infrared spectroscopy. A new absorption band in the wave number range 2280–2200 cm−1 indicates the formation of bound amino groups. In combination with the introduced silicate groups (at scientifically valid mass ratios of alcohol to amine), coagulation in such systems is theoretically improbable. In this case, an increase of strength is predicted for a film-forming system whose hybrid framework will include silicon–carbon and Si-O-C bonds at temperatures above the standard ones [19]. The achieved effect is reasonable to test in the creation of new anticorrosion materials by using a broad alcohol base.
According to V.V. Lisovskiy et al. [19], it is reasonable to mix liquid glass with phenol–formaldehyde and urea–formaldehyde resin solutions in alcohol. In addition to the phenol–formaldehyde resin (2 wt%), a synergistic effect is achieved by adding silica polymer production waste to the composition [6]. Gomi Tadasi [20] confirmed that a composition based on colloidal SiO2 and phenol–formaldehyde resin has increased hardness. However, the stabilization of phenol–formaldehyde resin molecules in alcohol–water silicate solutions [3,20] is still an actual problem. The most stable are phenol-containing systems when contain liquid glasses with a modulus of 2.7–3.0 (a distinctly alkaline agent). In contrast, a stable silicate composition with urea–formaldehyde resin can be obtained by the additional inclusion of orthophosphoric acid into the system. However, we probably need not expect this kind of reaction:
− H2O
~CH2N−CO−N−CH2OH + (HO)X SiY → ~CH2N−CO−N−CH2O SiY(OH)X−1
A.A. Kokin [21] associates the effect of increasing the water resistance of obtained materials with anticorrosion properties with a decrease in the total number of macropores (diameter up to 1.0 µm) and problems with the leaching of solution that has not entered into the reaction (2).
O.N. Primachenko [22,23] and S.S. Ishchenko et al. [24,25,26,27,28] observed the course of various competitive reactions (copolymerization, polycondensation, formation of isocyanate trimers, urethane–silicon compounds, etc.) when modifying silicate systems, depending on the nature and groups included in the additives (NH2 urea group, C-O group of epoxide, etc.). The result of the reaction between the modifier and the liquid glass solution is a hardening of the hybrid product and giving it viscoelastic properties [27,28,29]. For example, it has been found [30] that the addition of 15–25 wt% glycerol to liquid glasses provides a controlled increase in the viscosity of silicate systems without reducing their aggregative stability. It is claimed that glycerol is involved in the formation of a spatial silica–oxygen lattice, the presence of which is confirmed by infrared spectroscopy and the drop in the fluidity of hybrid compositions of this kind. European scientists [31] also tested copolymers of urea and acrylic acid. They are formed by the interaction of -COOH and -NH2-functional groups in the reaction (Figure 3).
A thorough study of the effect of additives of organic compounds including NH and NH2 groups [2,5,32,33,34,35,36,37,38,39] reveals clear prospects for giving silicate compositions increased adhesive properties and strength [5,36]. Such additives assist in the so-called “cross-linking” of silica oligomers through the action of intermolecular strength and the formation of sufficiently stable H-bonds [40]. The authors of this study specifically highlight urea among the effective additives of this kind.
In particular, application studies [37,41] showed a significant increase (up to 20%) in the adhesion to various substrates of a composite material incorporating urea-modified potassium silicate. The obtained result is in satisfactory agreement with the results obtained earlier [33,34,35] by P.B. Razgovorov (the optimum concentration of urea was set at 5–10 wt%). Reference [37] further justified the inclusion of mechanically activated Al2O3 (alumina) in such compositions. Over 30 years ago [5], in Japan, the addition of urea to silica-containing emulsions gave improved adhesion properties. This information is consistent with the results of using dextrin in combination with urea as a silicate system modifier [36]. A variety of polymer combinations with SiO2 inclusion have been found in silicate solutions. This increases the adhesive properties of the composite material. Its composition was established using infrared spectroscopy [36].
The aim of this work arising from an analysis of the literature was to create modified stable-at-storage compositions from sodium and potassium silicates. The main task when using such compositions is to obtain durable anticorrosion coatings for the chemical, oil refining and modern construction industry.

2. Materials and Methods

The potassium liquid glass hardened and repeatedly filtered; the initial silicate modulus is 2.9–3.2, and the density is 1.35–1.41 g∙cm−3; the total content of potassium and silicon oxides is 30.2–38.5 wt%.
Sodium liquid glass hardened and was repeatedly filtered; the initial silicate modulus is 2.7–3.3, and the density is 1.36–1.43 g∙cm−3; the total sodium and silicon oxides content is 30.2–38.5 wt%.
Urea grade “h”; melting point is 405.7 K at 1 atm. pressure; at the boiling point, it decomposes.
Butadiene styrene latex SKS 65-GP (BS-65-K-3), first quality category, non-volatile matter content is 50.0 (41.9) wt%.
Hydrophobizator GKZh-11 brand “chda”, alcohol-free sodium methylsiliconate solution, organosilicon liquid forming a polyalkylsilicone film; degree of polymerization is 2–3, pH is 13.0–14.0, nonvolatile matter content is 55 wt%.
Nonionic additive OP-10 (auxilliary substance) includes a mixture of oxyethylated alkylphenolols and polyethylene glycol; oil-like, water-soluble liquid of light yellow or light brown color; pH is 6.0–8.0 (at concentration 10 g∙L−1); basic substance content is not less than 80 wt%, and moisture content is not more than 0.3 wt%.
Calcium carbonate, the main component is CaCO3; average particle size is 20 microns; carbonate content is not less than 97.0–98.5 wt%, and mass fraction of free alkali is 0.01–0.04 wt%.
Agilite, calcined insoluble residue content is not less than 80.0 wt%, and moisture content is not more than 1.0 wt%.
Zinc flake, grades BC-0, BC-1 and BC-2, inorganic pigment white, the main component is ZnO; average particle size is 0.4–0.6 microns, and the content of zinc compounds in terms of oxide is not less than 98.0–99.7 wt%; mass fraction of water-soluble substances is not more than 0.06%–0.15%, and calcination losses is 0.2%–0.3%.
Titanium flake, grades P-02, P-03 and P-04; inorganic pigment white, rutile form, the main component is TiO2; pH is 6.5–8.0; content of titanium compounds in recalculation on titanium dioxide is not less than 90.0–98.0 wt%; content of volatile substances is not more than 0.5 wt%.
Chrome oxide (III) grades OKHP-1 and OKHP-2, a solid green powder, chrome in conversion to oxide is not less than 99.0 wt%; volatile matter is not more than 0.15 wt%.
Aluminum oxide (III), grades AOA-1, AOA-2 and AOA-3; white granules, rubbing strength is not less than 50.0–65.0 wt% and loss on ignition is not more than 5.0 wt%.
Iron (III) oxide (red iron oxide pigment), pH is 7.0–9.0; volatile matter content is not more than 3.0 wt%.
Aluminum powder PAP-1 and PAP-2 grades, powder silvery gray, floatation is not less than 80.0 wt%, the total content of impurity elements (iron, silicon, copper and manganese) is not more than 0.95–0.96 wt%, and impurity fatty additives are not more than 3.8 wt%.
Rongalit production waste (JSC “Khimprom”, Ivanovo, Russia) (calcined zinc oxide powder, gray-blue color); includes (wt%) ZnO 80.0–88.5, Zn (metal) 9.0–13.0 and Zn(OH)2 0.13–0.14; percentage on ignition is the rest.
Sludges of electrochemical production waste rongalite (Voronezh, plant “Processor”, Russia), powdery waste of yellow-brown color; includes (wt%) Ca 21.5–26.0, Fe 0.7–6.0, Cu 0.2–2.1, Ni 0.01–0.36, Zn 0.08, Pb 0.01–0.07, Cr 0.03–0.05 and water as the rest.
Kaolin (Scientific-Production Enterprise “Industrial Minerals”, Samara Region), white powder, including kaolinite, is up to 90%; SiO2 compounds is 8%–9%; impurity minerals (mica and hydromica) make up the rest.

2.1. Obtaining of Chemically Modified Liquid Glass

We filled potassium or sodium liquid glass into 250 mL three-necked flask with reflux condenser, thermometer and paddle stirrer and placed it in a water bath. The modulus and density of the liquid glasses corresponded to the above values. We added urea in an amount of 5 (potassium liquid glass) to 10 wt% (sodium at 1.0–1.5 s−1 liquid glass) during stirring. We heated the mixture to 333–343 K, with the stirrer rotating at 1.0–1.5 s−1 and kept it at this temperature until the viscosity reached 25–30 s according to the funnel VZ-4. Funnel VZ-4 is a cone-shaped tank with a volume of 100 ± 1 cm3 (diameter is 87 mm; height is 73 mm), and it is used to determine the relative viscosity of Newtonian liquids by fixing the time of outflow through the nozzle.
When liquid glasses were modified with other modifiers, sodium liquid glass was placed in the reaction apparatus described above. Nonionic additives (0.2–1.0 wt%) at room temperature and hydrophobizing additives (10 wt%) at a temperature of 353 K were introduced. The mixture was kept at this temperature and rotated at a speed of 1.0–1.5 s−1 for 1 h (nonionic additive) or 3 h (hydrophobizator), respectively.

2.2. Testing of Silicate Compositions and Cured Coatings

The obtained modified liquid glasses were cooled down to room temperature. Then, we evaluated their rheological and other physical and chemical properties and used them as a basis for the production and analysis of protective compositions. The relative viscosity of the systems was measured using a VZ-4 funnel with a nozzle diameter of (4.000 ± 0.015) mm. Part of the experimental data was obtained using an Ubbelohde viscometer (Technoglas, Moscow region, Odintsovo, Russia) with liquid flowing through a capillary with a diameter of 1.47 mm. We used a cell described in [42] to estimate the electrophoretic mobility and to calculate the ζ-potential of the systems.
When mixing modified liquid glasses with solid-phase components (chalk, talc, metal oxides, kaolin, wastes from various industries, etc.), the total mass ratio was w:t = 1:1 [38]; the amount of butadiene styrene latex in the composition did not exceed 20 wt%. The prepared compositions are classified as low-hazard substances. Immediately before the test, they were stirred with a paddle stirrer at 1 s−1 for 1 min and diluted with water to a relative viscosity of 20–25 s, using a VZ-4 funnel. These compositions were applied on the concrete tiles and glass plates of 90 × 120 mm in size with a brush or air compressor. The anticorrosion compositions were applied on the aluminum and steel plates via the pouring technique. The coatings were dried at temperature (293 ± 2) K for 8 h. The thickness of the cured one-layer coatings was 25–30 µm.
The elasticity, water absorption, weathering resistance and resistance of the cured coatings to detergents and under marine (tropical) conditions were assessed by using both theoretical and empirical [43] techniques. The resistance of the coatings to static effects of water at temperature (293 ± 2) K was identified as follows. The one-layer coating applied on the aluminum or glass plate was dried for 24 h in a desiccator. The plate was then immersed into distilled water at room temperature for 6 h, and then it was removed from the water and air dried for 2 h. A coating was considered water-resistant if, after wiping with a soft dark tissue, there was no or very weak chalk bleaching on its surface (≥6 on an eight-point scale).
In order to determine the silicate composition consumption (in terms of dry film), a two-layer coating was applied to the glass plate. At the same drying temperature (293 ± 2) K, the first layer was dried for 2 h, and the second one for 8 h. The plate with the dried first layer was placed on top of a chessboard with dark and light areas (squares). A second coat was brushed on until the light and dark areas of the chessboard (squares) underneath the plate were indistinguishable for viewing. After the drying of the second coat, the application area, the total mass of the coating (by deducting the mass of the glass plate) and the quantity applied per 1 m2 of surface area to be covered were determined.
The curing time (silicification period) of coatings incorporating conventional additives and industrial wastes (rongalite production, electrochemical sludge, etc.) was assessed by using carbon paper in black (for light-colored coatings) and red (for dark-colored coatings). Tests were carried out after 4, 6 and 8 h, respectively, from the time of coating on heavy white paper. The result is considered to correspond to the time interval (as mentioned above) if no silicate composite prints were left on the carbon paper.

3. Results

The theoretical basis of the interaction of liquid glasses with urea was described in more detail by one of the authors of this paper in [33,38]. The appearance of the flow curve of sodium liquid glass with an initial modulus of 3.2 and a density of 1.41 g∙cm−3 (Figure 4, Curve 1) indicates that this system belongs to the Newtonian type. When stored for 1 week, the flow is typical for Bingham systems (Figure 4, Curve 1′). In order to destroy the structure and organize the flow, a load of 18 mm Hg (Θ) must be applied to the system.
The natural behavior of the structure-forming processes in sodium liquid glass explains the low storage stability of the systems based on it. When 5 wt% urea is injected (Figure 4, Curve 2) the picture changes: Θ increases slightly compared with the initial value and remains practically unchanged for 1 week (168 h) of storage (Figure 4, Curve 2′). The Newtonian viscosity parameter (corresponding to the slope tangent of Curves 2 and 2′ in Figure 4) for original silicate systems and those treated with urea modifier is also characterized by constancy.
Our results correlate with the results of a study of the electrokinetic potential (ζ-potential) of investigated silicate systems in the presence of 5 wt% urea and auxiliary substance OP-10 at 5 g∙L−1 (Table 1).
The hypothesis of a close relationship between this parameter and the value of the high hydrogen index of the medium [39] due to the presence of an alkali metal cation (in this case, sodium) in the liquid glass has not been fully confirmed. On the other hand, it was found that spontaneous processes of structure formation in a silicate system are capable of proceeding even when its ζ-potential is sufficiently low (3.2–4.4 mV << 30.0 mV). The increase in electrokinetic potential of the modified solution achieved already at room temperature (for a 5 mas% urea additive 2–3 times; for an additive 5 g∙L−1 (0.4 wt%) auxiliary substance OP-10 to 40.9 > 30.0 mV) is explained by the formation of silazane bonds Si-N involving urea amino groups and/or the adsorption of nonionic molecules in the internal liquid glass structure.
The particles in our initial sodium silicate solution (modulus, 2.7; density, 1.41 g∙cm−3) are negatively charged, which promotes anionic polymerization processes when a modifier is added. They contain a core and an adsorption layer, while the micelle additionally has a Gouy diffuse layer (Figure 5). We discovered that in order to obtain a high-quality modified product in the presence of a nonionic additive (auxiliary substance OP-10, neonol), the concentration of the additive in the silicate system should not be higher than 0.5 wt%; otherwise, an additional antidote defoamer will be needed.
An analysis of the obtained results shows that the introduction of urea and auxiliary substance OP-10 in a scientifically justified ratio to the sodium liquid glass solution (stated above) ensures the equality of the rates of destruction and recovery of coagulation structures. The hysteresis loops (Figure 6) and the thixotropic properties of the resulting systems provide strong indications that the individual operations (diluting with water, mixing components) will be easier when carrying out the technological route of obtaining the corrosion-protection material directly at the industrial site.
Thus, on the basis of our research, mass media contain reliable information about the possibility of reducing energy costs in the production of composite material directly at the site of the construction project in preparation for the application of protective coatings with improved corrosion-protection properties.
However, BASF (Germany) has produced conservation resistant silicate materials for more than 30 years [45,46]. In addition to liquid glasses (≤24 wt%), they contain a 50% aqueous dispersion based on a styrene–acrylate–butadiene copolymer (butadiene–styrene or acrylate latex) [47]. O.M. Andrutskaya [48] mentions that with a volume concentration of pigments and fillers of ≈35%, there is practically no disintegration and delamination of prepared dispersions’ latex molecules. They act as a surface-active agent and stabilize the system [49], adsorbing on the surface of the solid-phase particles.
The result of mixing vinyl chloride butadiene latex (140 nm particle diameter) with hydroxyethyl cellulose and a nonionic substance [50] has drawn public attention. The obtained hybrid materials (2) are resistant to precipitation and wind and are characterized by pronounced anticorrosion properties compared to silicate compositions produced in the absence of latex (1) (Table 2).
As is known [50,51,52], surfactants are added to liquid glass solutions in order to give the resulting organic–inorganic materials well-controlled rheological properties. For example, it was found [51] that sulphonol (nonionic substance) in small amounts (0.5 wt%) acts similarly to the previously described auxiliary substance OP-10, inhibiting the coagulation–condensation process and ensuring stability during storage of the prepared hybrid material. In both cases, the effect achieved is due to the formation of solvate shells around the silicic acid particles incorporating silica micelles, surfactant molecules and water, which prevent these particles from coalescing. Nowadays, researchers are of the general opinion that the stability of corrosion protection hybrid inorganic–organic materials with sodium and potassium silicates is guaranteed by the low dilution of the latter and the low (≤1–2 wt%) concentration of the surfactant additive [52].

Author’s Contribution to the Development of Anticorrosion Coatings on the Surface of Aluminum and Non-Ferrous Metals

The adsorption of OH-ions from silicate systems on steel requires the presence of defects in a thin passivation film with a lack of saturation valence which act as active centers [53]. SiO44- silicate ions act as donors by binding to iron oxide. The structurally imperfect areas of the passivation film become more stable, and the condensation of the polymer forms of the silicate ions takes place on the resulting compound.
E.P. Katsanis et al. [54] found that liquid glasses with modulus n (ratio of silicon dioxide moles to alkali metal oxide moles in solution) of at least 3.2 enhanced corrosion protection properties when protecting non-ferrous metals. In this case, a thin, invisible double-layer film is formed on the non-ferrous metal, which prevents the corrosion process from occurring. The outer layer is an amorphous silicate compound phase.
Actual problems of creating anticorrosion protective materials and coatings on aluminum products were considered in the Russian Federation in the 1980s to the 1990s [55,56]. The mechanism of the processes, especially in the presence of phosphates, has now been well studied [57,58,59], also by the authors of the study [57].
The silicate composites are applied by pouring or auto-deposition for protecting aluminum products against corrosion. When chromium, magnesium and zirconium oxides are added to compositions as pigments and fillers, the adhesion properties of the obtained coatings at the tearing off are high enough and increase in proportion to the heating temperature of the protected surface (4.0 MPa at 313–323 K to 5.0 MPa at 573 K [40]). This way, the higher electrical resistance liquid glass solutions act as a dielectric and provide the necessary bonding to the aluminum surface (positive charge), with the excellent conductivity of the metal preventing the formation of a double layer.
The maximum filling (up to 75%–80% of the total mass of the composition) of high-modulus solutions of sodium liquid glass (n = 3.6–4.5) with zinc powder [60] also manages to provide the necessary electrochemical contact between aluminum and zinc particles and achieve the required anticorrosion effect during priming. Otherwise, (an insufficient concentration of zinc dust) zinc leaching leads to the formation of air bubbles on the primed surface. Nevertheless, the creation of such corrosion-protection materials has started a new age of protection for metal structures in the oil, gas and petroleum industries, especially in areas of periodic environmental impact.
The effective combination of liquid glass solutions in composition with natural aluminosilicates for giving the anticorrosion properties to the finished materials, fire resistance and weatherability is discussed in [61,62]. Thus, the introduction of asbestos into liquid glass in a scientifically proven ratio (1:2) produces an anticorrosive material that protects any metal when exposed to ultra-high temperatures (≥1273 K).
The authors of the present work took part in developing varnish compositions to which were added triglycerides of fatty acids, zinc and titanium whiting, iron oxide (III) as an analogue of the material described in [63]. Kaolin (Samara region) is an additional component. The material is corrosion-resistant; suitable for the protection of metals, wood and plastered surfaces; and has thermal and water resistance.
As for compositions containing liquid glass, the most important task is to increase their stability when stored mixed with metal oxides (zinc, titanium, iron, magnesium and aluminum). These metal oxides act as solid phases—pigments and fillers that provide the material with the necessary hiding power and appropriate coloration. The modification of potassium and sodium silicates with urea (5–10 wt%) at 333–343 K [35,36,37] and further stirring of cooled film-forming compound under normal conditions with butadiene styrene latex [36,37,40] give water resistant dispersion silicate materials with bending strength in the range of 10–15 mm (Table 2) and stability during storage ≥180 days. These single-package silicate materials are stored as a paste and diluted with water to the required consistency (conditional viscosity of 20 s, according to the VZ-4 funnel) when used at the coating site. The optimum combination of zinc, iron and magnesium compounds (10 wt%) in the solid phase makes these compositions the effective inhibitors of the corrosion fracture of iron, steel and its alloy substrates [40].
The author’s approach to solving the problem of single-package silicate materials with anticorrosion properties deals with the study of the prospects of making them cheaper and, at the same time, creating new possibilities for solving modern environmental problems. Thus, we identified the option of replacing the solid components—zinc and/or titanium oxides with basic sulphate white lead (a zinc-containing waste from the production of rongalite) [64]. The economic effect of such one-pack compositions (180 days) is up to €300–320/ton. The consumption of such silicate compositions is within 250 g∙m−2 (in terms of dry film). It can even be reduced to 120–150 g∙m−2 in the case of using sludge of electrochemical production as a solid phase. These slurries are pastes including copper, calcium, chromium (III), iron and aluminum cations [39,64]. The curing time of the coatings obtained does not exceed 6 h, while maintaining water resistance, elasticity (bending test; 10 mm) and stability of the composition during storage (at least 120 days) [65]. The issue also deals with the recycling of industrial wastes. The developed anticorrosion compositions and coatings protect the surfaces of structural elements made of aluminum and its alloys in the zone of temperatures up to 573–673 K well, at consistent compliance with operations on the process route (Table 3).
A dynamic analysis of physical and chemical characteristics of compositions and the obtained coatings involves the possibility of mathematical modelling and the prediction of their protective effect in conditions of multifactorial experiment (degree of dilution of the composition, temperature of modification and coating, intensity of mixing, concentration of modifying additives, etc.). This trend is highly relevant in terms of the perspective of predicting the course of individual stages of corrosion processes.

4. Discussion

The analysis of worldwide research in the field of chemical modification of liquid glasses presents the technological aspects of obtaining anticorrosive compositions with increased vitality and elasticity.

5. Conclusions

Based on the results of the world and author’s study in the field of modification of liquid glasses, the main technological aspects on the preparation of time-stable (180 days) one-pack compositions with increased elasticity were presented.
It is found that compounds including amino groups such as urea, butadiene-styrene latexes and nonionic surfactants form hybrid thixotropic and storage-stable organo-inorganic structures when using a reasonable proportion of additives (0.5–20.0 wt%) to liquid glasses (modulus, 2.9–3.2; density, 1.35–1.42 g∙cm−3). The formation of these structures prevents the cohesion of solid-phase particles in the system and improves (1.5–2.0 times) the most important physical and mechanical characteristics (water resistance, adhesion to the substrate and strength) of new coatings used for the corrosion protection of aluminum and its alloys, iron and steel, as well as plastered surfaces.

Author Contributions

Conceptualization, P.R. and S.L.; methodology, N.P.; writing—original draft preparation, K.V.; writing—review and editing, P.S. All authors have read and agreed to the published version of the manuscript.

Funding

This research was performed by Peter the Great St. Petersburg Polytechnic University and supported under the strategic academic leadership program ‘Priority 2030′ of the Russian Federation (Agreement No. 075-15-2021-380, dated 20 February 2023).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Detailed results of the author’s research are presented in the sources given in the References section.

Acknowledgments

The authors would like to express their gratitude to the staff of the Centre for Collective Use of Scientific Equipment of Ivanovo State University of Chemistry and Technology for their assistance in testing the physical and chemical properties of the coatings obtained from modified organo–inorganic systems with the inclusion of liquid glass.

Conflicts of Interest

The authors declare no conflict of interest.

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Coatings 13 00974 g001 550
Figure 1. Time dynamics (τ) of the structural viscosity (η) of liquid glasses at 293 K [18]. Liquid glass: 1—sodium–potassium Na2O K2O n SiO2; 2—sodium Na2O n SiO2; 3—potassium K2O n SiO2.
Figure 1. Time dynamics (τ) of the structural viscosity (η) of liquid glasses at 293 K [18]. Liquid glass: 1—sodium–potassium Na2O K2O n SiO2; 2—sodium Na2O n SiO2; 3—potassium K2O n SiO2.
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Figure 2. Dynamic viscosity change (μ) of liquid glass solutions and time course (τ) of the jellification process with tetraethoxysilane. The type of liquid glass: 1—Li+; 2—Na+; and 3—K+ [17].
Figure 2. Dynamic viscosity change (μ) of liquid glass solutions and time course (τ) of the jellification process with tetraethoxysilane. The type of liquid glass: 1—Li+; 2—Na+; and 3—K+ [17].
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Figure 3. Functional groups in the reaction.
Figure 3. Functional groups in the reaction.
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Figure 4. Flow of sodium liquid glass solutions freshly prepared (1, 2) and taken after 7 days storage under regular conditions (1′, 2′). The 1, 1′ is sodium liquid glass; the 2, 2′ is sodium liquid glass modified with urea.
Figure 4. Flow of sodium liquid glass solutions freshly prepared (1, 2) and taken after 7 days storage under regular conditions (1′, 2′). The 1, 1′ is sodium liquid glass; the 2, 2′ is sodium liquid glass modified with urea.
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Figure 5. Particle structure and layer formation in sodium liquid glass micelle [44].
Figure 5. Particle structure and layer formation in sodium liquid glass micelle [44].
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Figure 6. Thixotropy in sodium liquid glass solution (a) and systems: sodium liquid glass—urea (b); sodium liquid glass—auxiliary substance OP-10 (c). The 1 is the freshly prepared liquid glass solution, and the 1′ is the liquid glass solution after 7 days storage.
Figure 6. Thixotropy in sodium liquid glass solution (a) and systems: sodium liquid glass—urea (b); sodium liquid glass—auxiliary substance OP-10 (c). The 1 is the freshly prepared liquid glass solution, and the 1′ is the liquid glass solution after 7 days storage.
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Table
Table 1. ζ-potentials of sodium liquid glass solutions in the absence and during incubation with urea modifier and auxiliary substance OP-10 introduced.
Table 1. ζ-potentials of sodium liquid glass solutions in the absence and during incubation with urea modifier and auxiliary substance OP-10 introduced.
Type of SolutionUnstored Solution, mVSolution after 7 Days of Ageing with Modifier, mV
Sodium liquid glass solution3.2 ± 0.14.4 ± 0.1
Liquid sodium glass—urea6.2 ± 0.214.6 ± 0.4
Liquid sodium glass—
auxiliary substance OP-10		26.0 ± 0.840.9 ± 1.1
Table
Table 2. Comparative characteristics of coatings based on liquid glass compositions and those incorporating SKS-65-GP latex.
Table 2. Comparative characteristics of coatings based on liquid glass compositions and those incorporating SKS-65-GP latex.
Parameter/CharacteristicSodium and Potassium Based Liquid Glass
Coatings		Liquid Glass Coatings Containing Urea and Butadiene Styrene Latex
Atmosphere resistanceSatisfactoryGood
Resistance in marine and tropical climatesHydrophobization is requiredSatisfactory
Water infiltrationFrom limited to highSmall
Water absorption WW = 0.3–0.8 kg/m2 c0.5W = 0.2–0.5 kg/m2 c0.5
Elasticity (bend test)50 mm≤15 mm
Resistant to detergents and abrasivesRelatively limitedUp to good
Application conditionsDo not apply in the rainResistant in the rain
CostMore expensiveLess expensive
Table
Table 3. Process route for protecting aluminum at 673 K by silicate coating.
Table 3. Process route for protecting aluminum at 673 K by silicate coating.
RouteOperation MaterialViscosity on Funnel VZ-4, sDrying Mode
Air Sprayer KR-10Brush
Application		Time Duration, HoursTemperature, K
DegreasingWhite spirit solvent----
SandblastingSand----
PrimingPrimer14–2540–453291–296
CoatingSodium liquid glass—aluminum powder20–2525–307–8291–296
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Razgovorov, P.; Loginova, S.; Politaeva, N.; Velmozhina, K.; Shinkevich, P. Modification of Liquid Glasses Is a Key Factor in the Technology of Obtaining Hybrid Compositions and Coatings with Anticorrosive Properties. Coatings 2023, 13, 974. https://doi.org/10.3390/coatings13060974

AMA Style

Razgovorov P, Loginova S, Politaeva N, Velmozhina K, Shinkevich P. Modification of Liquid Glasses Is a Key Factor in the Technology of Obtaining Hybrid Compositions and Coatings with Anticorrosive Properties. Coatings. 2023; 13(6):974. https://doi.org/10.3390/coatings13060974

Chicago/Turabian Style

Razgovorov, Pavel, Svetlana Loginova, Natalia Politaeva, Ksenia Velmozhina, and Polina Shinkevich. 2023. "Modification of Liquid Glasses Is a Key Factor in the Technology of Obtaining Hybrid Compositions and Coatings with Anticorrosive Properties" Coatings 13, no. 6: 974. https://doi.org/10.3390/coatings13060974

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