TY - JOUR
AU - Ahmed, Muhanad A
AB - Abstract In chemical manufactures, the corrosion inhibitors were added in order to reduce the corrosion of mild steel. Chemical molecules are often used on mild steel surfaces as portion of the latest finishing steps before painting and/or storage. Here, this work elucidated the utilization of an isatin derivative, namely, 3-((3-acetylphenyl)imino)indolin-2-one synergistic with zinc oxide nanoparticles for improving the impedance of mild steel (MS) against corrosion in 1.0 M hydrochloric acid using the weight loss method and scanning electron microscopy (SEM). Weight loss measurements demonstrated that the best 3-((3-acetylphenyl)imino)indolin-2-one concentration was 0.5 mM and the inhibition efficiency was 83% whereas the inhibition efficiency was 92% with addition of ZnO NPs. 3-((3-Acetylphenyl)imino)indolin-2-one retards the corrosion process at 300 K and demonstrates low inhibition efficiencies at 310, 320 and 330 K. 1. INTRODUCTION Nanocrystalline materials were considered to be one of the most significant materials used enormously in researches during the past years. This was as a result of these materials’ impact on various applications for this new branch of materials. These applications could be found for example in novel optical, electrical and mechanical properties of devices comprising nanocrystalline semiconductors and oxides in photo-voltaic solar cells [1], light-emitting diodes [2], varistors [3] and ceramics [4]. In addition, ion-insertion batteries and electrochromic devices are other applications of these materials. Among these semiconductor materials, zinc oxide (ZnO) has attracted considerable attention due to its extraordinary importance and a substantial number of research papers published reporting on ZnO nanocrystalline [5–7]. Mild steel corrosion [8,9] is still one of the most considerable issues when mild steel has been utilized in industries. The expenses of corrosion process were in billions per year, particularly in manufacturing in which mild steel is exposed to the hydrochloric acid medium, an extremely corroded parameter. Corrosive solutions, in particular the various concentrations of HCl medium, are broadly utilized and have a significant role in manufactures, in the oil refining, pickling, cleaning and chemical industrial stages. Previously, protections of our environment turn into a first problem. Nowadays, investigators have considerable attention about the organic molecules which could be degradable as well as eco-friendly. Natural and organic chemical inhibitors were used as corrosion inhibitor due to their significant characteristics [10]. Generally, the corrosion event for different alloys is particularly prominent in these manufactures [11–16]. There are various approaches to reduce and impede metal corrosion, among which is to utilize various inhibitors [17–21]. Hence, the use of a metal corrosion in the corrosive environment is important not only for industrial uses but also for academic research [22–28]. The objectives of this study are to synthesize a 3-((3-acetylphenyl)imino)indolin-2-one as a corrosion inhibitor and to study the synergistic effect of the 3-((3-acetylphenyl)imino)indolin-2-one and zinc oxide (ZnO) nanoparticles (NPs) to inhibit mild steel corrosion in 1 M HCl. The weight loss method and scanning electron microscopy (SEM) were employed to evaluate the inhibition efficiencies. The novelty of this work is the synergistic study of two compounds (organic and inorganic compounds) which were ZnO NPs and 3-((3-acetylphenyl)imino)indolin-2-one as corrosion inhibitors for mild steel in hydrochloric acid. This study was done for the first time. 2. EXPERIMENTAL DETAILS 2.1. Materials and chemical analyses Zinc oxide nanoparticles (ZnO NPs) have been prepared through the sol–gel technique. A solution of NaOH (20 g) in distilled water (25 mL) was poured onto the solution of Zn(CH3CO2)2·2H2O (5.0 g) in distilled water (45 mL) and then stirred for 10 min. Finally, 250 mL of the ethyl alcohol was added to the solution in order to obtain a white precipitate of zinc oxide nanoparticles. 2.2. Preparation of 3-((3-acetylphenyl)imino)indolin-2-one The inhibitor 3-((3-acetylphenyl)imino)indolin-2-one was synthesized according to the approach cited in [29]. The light brown product with the yield of 51% has a melting point of 263–265°C. The data of the FT-IR spectra were 3391.5 cm−1 for the amino group, 1510.7 cm−1 for the C=C aromatic group and 1717.3 cm−1 for the carbonyl group. 1H NMR data (ppm), (CDCL3): 8.35 ppm (s, N-H), 7.18–7.84 ppm (m, 8 aromatic protons) and 2.55 ppm (s, 3H, CH3). The analysis of C16H12N2O2 was C, 72.72; H, 4.58; N, 10.60% and that for found C, 73.51; H, 4.41; N, 11.21%. 2.3. Weight loss method Hydrochloric acid solution with a concentration of 1.0 M has been produced by adding distilled water to 37% HCl solution. Various concentrations of 0 × 10−3 to 10 × 10−3 M of 3-((3-acetylphenyl)imino)indolin-2-one have been used and tested for corrosion inhibition. The mild steel (MS) specimen (with a volume area of 3.5 × 3 × 0.3 cm3) was initially washed with double-distilled water and acetone and then dried. The composition of the tested mild steel (MS) specimen was carbon, silicon, manganese, phosphorous, sulfur and copper at concentrations of 0.13, 0.18, 0.39, 0.40, 0.04 and 0.025, respectively, in addition to iron, which represents the rest of the concentration. The mild steel specimen was then immersed in a hydrochloric acid solution of ~100 mL in the absence and presence of the 3-((3-acetylphenyl)imino)indolin-2-one inhibitor. The synergistic effects were studied through the addition of 1.0 × 10−3 g of zinc oxide (ZnO) nanoparticles. The testes were performed at room temperature (RT) for a period of 4, 8 and 16 h. The specimens were washed, dried and then weighed before and after each immersion in the HCl solution. The calculations were performed in triplicate, and the mean value was used gravimetric measurements. Equations 1–3 were used to calculate the corrosion rate, inhibition efficiency and surface coverage, respectively. $$\begin{equation}{C}_{\mathrm{R}}=\frac{87.6\times W}{d\ a\ t}\end{equation}$$(1) where CR is the corrosion rate in mmp, W is the weight loss in mg, d is the density, a is the area in cm2 and t is the time in h. $$\begin{equation}\mathrm{IE}\%=\frac{W_o-{W}_1}{W_o}\times 100\end{equation}$$(2) where IE % is the inhibition efficiency, Wo is without inhibitor and W1 is with inhibitor. $$\begin{equation}\theta =\frac{IE}{100}\end{equation}$$(3) where θ is the surface coverage. 2.4. Surface morphologies The surface morphology of the studied specimens without and with the addition of 3-((3-acetylphenyl)imino)indolin-2-one was investigated to evaluate the surface nature such as smoothness and roughness. These have been conducted using SEM. SEM was carried out utilizing SEM, JEOL Japan model SM-7600F, and was utilized to test the metal surface in acidic solution in the presence and absence of an inhibitor. The latter is an effective instrument which generates photographs of the tested surfaces of films or powders through scanning the surface of the sample by the electron beam (e-beam). The interactions of electrons with the target atoms in the surface of the sample generate different signals which have data about the topography of the tested surface and the composition of the tested samples. 3. RESULTS AND DISCUSSION 3.1. ZnO NP characterization The powder of zinc oxide (ZnO) nanoparticles has been characterized by the x-ray powder diffraction (XRD) technique. This is a powerful technique which has been used to analyze the crystalline structure of a variety of solid materials [30, 31]. The XRD technique consists of the source, sample holder and detector. The source is built of a copper block, on which high-energy electrons impinge upon ~40 kV. When the electrons enter the copper block, they are decelerated emitting a continuous spectrum of electromagnetic radiation, which is called Bremsstrahlung. In addition, the emission of discrete lines also takes place by means of the excitations within the copper atoms, i.e. Cu Kα1 radiation with a distinct wavelength (λ) of 1.54062 Å. This monochromatic radiation is used for the XRD experiments. Figure 1 shows the XRD patterns of ZnO NPs which was synthesized via the chemical method, namely, sol gel technique, and obtained at the calcining temperature of 500°C. It is obvious from this figure that no impurities are there, proposing that the synthesized ZnO NPs are of a high purity due to the high-temperature treatment and also of a high crystallinity [30]. It is also shown that the peak is expanded, revealing that the size of the ZnO nanoparticles was quite small regarding the Debye–Scherrer equation [32]. $$\begin{equation}D=\frac{0.9\ \lambda}{\beta \cos \theta }\end{equation}$$(4) where D, λ, β, θ and 0.9 are the particle size in nm, the wavelength of the X-ray, the full width at half maximum, the peak position and the Scherrer constant, respectively. Figure 1 Open in new tabDownload slide X-ray diffraction data of the ZnO NPs. Figure 1 Open in new tabDownload slide X-ray diffraction data of the ZnO NPs. 3.2. The effect of inhibitor concentration The mild steel corrosion in 1.0 M of hydrochloric acid medium without and with the addition of different concentrations of 0 × 10−3 to 10 × 10−3 M of 3-((3-acetylphenyl)imino)indolin-2-one as corrosion inhibitor for the immersion times of 4, 8 and 16 h at 300 K was measured by weight loss methods. From the data of weight loss measurements, corrosion rates versus concentration in the presence and absence of ZnO NP plots at various immersion times are displayed in Figures 2 and 3, respectively. Figure 2, on the one hand, confirms that the corrosion rates of the tested inhibitor decrease with the increase in the inhibitor concentration. Figure 3, on the other hand, confirms that the corrosion rates of the tested inhibitor decrease with the increase in the inhibitor concentration in the presence of 1 × 10−3 g of zinc oxide. The addition of 1 × 10−3 g of zinc oxide NPs has synergistic effects with the inhibitor and decreased the corrosion rates. The use of the inhibitor 3-((3-acetylphenyl)imino)indolin-2-one molecules to corrode the metal in the acid solution at times of exposure <24 h increases the inhibition efficiency gradually until it reaches excellent efficiency, but its inhibition efficiency decreases after 24 h. Hour and thus the corrosion rate increases. The rate of corrosion gradually increased with the immersion time of 3-((3-acetylphenyl)imino)indolin-2-one molecules, as a result of the decrease in the number of inhibitor molecules available in the acid solution that work to protect the metal surface and thus increase the corrosion rate and decrease the inhibition efficiency. Figure 2 Open in new tabDownload slide Variation of corrosion rates with various inhibitor concentrations for mild steel in 1 N HCl4 at 300 K for the immersion times of 4, 8 and 16 h. Figure 2 Open in new tabDownload slide Variation of corrosion rates with various inhibitor concentrations for mild steel in 1 N HCl4 at 300 K for the immersion times of 4, 8 and 16 h. Figure 3 Open in new tabDownload slide Variation of corrosion rates with various inhibitor concentrations and 1 × 10–3 g of zinc oxide nanoparticles for mild steel in 1 N HCl at 300 K for the immersion times of 4, 8 and 16 h. Figure 3 Open in new tabDownload slide Variation of corrosion rates with various inhibitor concentrations and 1 × 10–3 g of zinc oxide nanoparticles for mild steel in 1 N HCl at 300 K for the immersion times of 4, 8 and 16 h. Figures 4 and 5 represent the inhibition efficiencies of the studied inhibitor versus the various concentrations of the studied inhibitor in the absence and presence of 1 × 10−3 g of zinc oxide NPs, respectively. Figure 4 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations for mild steel in 1 N HCl at 300 K for the immersion time of 4, 8 and 16 h. Figure 4 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations for mild steel in 1 N HCl at 300 K for the immersion time of 4, 8 and 16 h. Figure 5 Open in new tabDownload slide Variation of IE% with various inhibitor concentrations and 1.0 × 10–3 g of zinc oxide nanoparticles for mild steel in 1 N HCl at 300 K for the immersion time of 4, 8 and 16 h. Figure 5 Open in new tabDownload slide Variation of IE% with various inhibitor concentrations and 1.0 × 10–3 g of zinc oxide nanoparticles for mild steel in 1 N HCl at 300 K for the immersion time of 4, 8 and 16 h. Figures 4 and 5 confirm that the inhibitive performance of the tested inhibitor increases with the increase in the concentration of the studied inhibitor, and also the inhibition efficiency increases with the addition of 1.0 × 10−3 g of zinc oxide nanoparticles. The range of the inhibitor depends upon the chemical structure of the inhibitor. At the minimum studied concentrations, the inhibitive efficiency increases progressively and nearly reached saturation over the concentration of 10 × 10−3 M. The inhibition efficiencies of the same inhibitor concentration at 300 K were increased with the addition of ZnO NPs. The inhibition efficiency analysis of the studied inhibitor reveals that the inhibition efficiencies increase when adding ZnO NPs, and this trend can be demonstrated according to the synergistic effect of ZnO NPs and the studied inhibitor molecules. As shown in Figure 6, the compound 3-((3-acetylphenyl)imino)indolin-2-one can be in two forms, namely keto and oxo forms. The two conformations help us to understand the stabilization of the studied inhibitor. Figure 6 Open in new tabDownload slide The conformations of the studied inhibitor. Figure 6 Open in new tabDownload slide The conformations of the studied inhibitor. The inhibition efficiency that tested the inhibitor in the presence of ZnO NPs was achieved even at quite a low concentration of the tested inhibitor, while it was achieved at a much higher concentration in the case of ZnO NP absence. 3.3. Effect of temperature The effect of the inhibitive achievement of the tested inhibitor in 1 M hydrochloric acid solution on the surface of mild steel has been studied by the weight loss technique in the temperature extent from 300 to 330 K in the absence and presence of ZnO NPs. Figure 7 demonstrates the inhibition efficiency values that are obtained from the weight loss technique at various temperatures of 300–330 K. It was obvious from Figure 7 that the tested inhibitor adsorbed on the surface of the tested mild steel at all studied temperatures and the inhibition efficiency decrease with the increase in temperature in the absence and presence of the studied inhibitor. The inhibition efficiency diminishes with the rise in temperature, which is the indication of physisorption adsorption [33, 34], and this was imputed to dissolve the protective film that formed on the surface of mild steel by tested inhibitor molecules. As the temperature rises, the adsorbed number of the inhibitor molecules decreases, and this refers to the decrease in the inhibition efficiency. Figure 7 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations for mild steel in 1 N HCl at various temperatures of 300, 310, 320 and 330 K for the immersion time of 8 h. Figure 7 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations for mild steel in 1 N HCl at various temperatures of 300, 310, 320 and 330 K for the immersion time of 8 h. Figure 8 displays the inhibition efficiency values that are obtained from the weight loss technique at various temperatures of 300–330 K in the presence of ZnO NPs. It was obvious from this figure that the tested inhibitor adsorbed on the surface of the tested mild steel at all studied temperatures and the inhibition efficiency decrease with the increase in temperature in the absence and presence of the studied inhibitor, but still better than without the addition of ZnO NPs. Figure 8 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations with the addition of ZnO NPs for mild steel in 1 N HCl at various temperatures of 300, 310, 320 and 330 K for the immersion time of 8 h. Figure 8 Open in new tabDownload slide Variation of IE % with various inhibitor concentrations with the addition of ZnO NPs for mild steel in 1 N HCl at various temperatures of 300, 310, 320 and 330 K for the immersion time of 8 h. 3.4. Adsorption isotherm Natural and synthetic organic compounds were exploited for the purpose of retarding the corrosion in the corrosive solution due to the adsorption of these molecules on the surface of the tested alloy. The adsorption depends upon the chemical structure of the inhibitor, the stable conformation in the solution, the surface of the tested alloy and the solution temperature. Different adsorption isotherms namely Langmuir, Frumkin and Temkin were applied for the tested inhibitor on the surface of the tested alloy in the HCl solution. The correlation coefficient (R2) was utilized to evaluate the better fit. For the tested inhibitor, the better fit acquired was with the Langmuir adsorption isotherm as shown in Equation 5 below: $$\begin{equation}\frac{C}{\theta }=\frac{1}{K}+C\end{equation}$$(5) where C is the concentration and K is the equilibrium constant. The C/θ vs C in Figure 9 gives a straight line. Generally, the coefficient (R2) is approximately equal to unity, and the slope was found to deviate from unity. The slope deviation from unity might be due to the interactions between the adsorbed molecules on the mild steel’s surface [35] or the adsorbate might occupy further than one adsorption site on the surface of mild steel. Furthermore, a comparable attitude was seen by many investigators [36], and the Langmuir adsorption isotherm was proposed. Figure 9 Open in new tabDownload slide Langmuir isotherm plot for the adsorption of the tested inhibitor on mild steel in 1 M HCl. Figure 9 Open in new tabDownload slide Langmuir isotherm plot for the adsorption of the tested inhibitor on mild steel in 1 M HCl. 3.5. SEM The SEM micrographs of the surface of the tested mild steel have been obtained in the absence and presence of 3-((3-acetylphenyl)imino)indolin-2-one, which immersed in 1 M hydrochloric acid (HCl) medium. These micrographs are displayed in Figures 10 and 11. Figure 10 Open in new tabDownload slide SEM image of mild steel in the absence of the corrosion inhibitor after immersion in 1 M HCl solution. Figure 10 Open in new tabDownload slide SEM image of mild steel in the absence of the corrosion inhibitor after immersion in 1 M HCl solution. Figure 11 Open in new tabDownload slide SEM image of mild steel in the presence of the corrosion inhibitor after immersion in 1 M HCl solution. Figure 11 Open in new tabDownload slide SEM image of mild steel in the presence of the corrosion inhibitor after immersion in 1 M HCl solution. Figure 10 shows the influence of 1 M HCl medium on the surface of mild steel after 4 h as immersion time without the addition of 3-((3-acetylphenyl)imino)indolin-2-one. It is obvious that the surface has pits, which were obtained by the corrosive medium. Figure 11 represents the mild steel immersion in the corrosive solution in the presence of 0.01 M of 3-((3-acetylphenyl)imino)indolin-2-one as a corrosion inhibitor. It is obvious that the surface is smooth due to the formation of a protected layer from the inhibitor molecules as adsorbed layer on the surface of mild steel. 4. CONCLUSION A new corrosion inhibitor namely 3-((3-acetylphenyl)imino)indolin-2-one showed excellent inhibition efficiency towards the hydrochloric acid solution. The optimum inhibition efficiency of 3-((3-acetylphenyl)imino)indolin-2-one was accomplished at low and high concentrations, and the highest inhibition efficiency was 83.99% at the concentration of the inhibitor of 0.01 M. Thus, 3-((3-acetylphenyl)imino)indolin-2-one acts as a considerable corrosion inhibitor. The corrosion rate was decreased in the presence of the corrosion inhibitor even at a higher solution temperature. 3-((3-Acetylphenyl)imino)indolin-2-one have four hetero atoms and double bonds that give the chemical structure of this inhibitor the stability and the capability to be adsorbed on the surface of mild steel. The addition of ZnO NPs to the corrosive solution, on the other hand, increases the inhibition efficiency from 83% (without ZnO NPs) to 92% (with ZnO NPs), and therefore, ZnO NPs have synergistic effects when added to the corrosive solution with 3-((3-acetylphenyl)imino)indolin-2-one. The SEM technique is powerful and supports the formation of a protected layer on the surface of mild steel. The adsorption of 3-((3-acetylphenyl)imino)indolin-2-one on the surface of mild steel in the corrosive solution followed the Langmuir adsorption isotherm. 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TI - Synergistic effect of ZnO nanoparticles with organic compound as corrosion inhibition
JO - International Journal of Low-Carbon Technologies
DO - 10.1093/ijlct/ctaa076
DA - 2020-10-20
UR - https://www.deepdyve.com/lp/oxford-university-press/synergistic-effect-of-zno-nanoparticles-with-organic-compound-as-Lax10Nzcs1
SP - 1
EP - 1
VL - Advance Article
IS - 
DP - DeepDyve
ER -