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Article

Wettability of Metals by Water

by
Laszlo Somlyai-Sipos
and
Peter Baumli
*
Institute of Physical Metallurgy, Metal Forming and Nanotechnology, University of Miskolc, 3515 Miskolc, Hungary
*
Author to whom correspondence should be addressed.
Metals 2022, 12(8), 1274; https://doi.org/10.3390/met12081274
Submission received: 27 June 2022 / Revised: 25 July 2022 / Accepted: 27 July 2022 / Published: 28 July 2022
(This article belongs to the Special Issue Nanostructured Metallic Coatings)
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Abstract

:
The wetting behavior of water on metal surfaces is important for a wide range of industries, for example, in the metallurgical industry during the preparation of metallic nanoparticles or electrochemical or electroless coating preparation from aqueous solutions, as well as in the construction industry (e.g., self-cleaning metal surfaces) and in the oil industry, in the case of water–oil separation or corrosion problems. Wettability in water/metal systems has been investigated in the literature; nevertheless, contradictions can be found in the results. Some papers have reported perfect wettability even in water/noble metal systems, while other researchers state that water cannot spread well on the surface of metals, and the contact angle is predicted at around 60°. The purpose of this paper is to resolve this contradiction and find correlations to predict the contact angle for a variety of metals. In our research, the wetting behavior of distilled water on the freshly polished surface of Ag, Au, Cu, Fe, Nb, Ni, Sn, Ti, and W substrates was investigated by the sessile drop method. The contact angle of the water on the metal was determined by KSV software. The contact angle of water is identified as being between 50° and 80°. We found that the contact angle of water on metals decreases linearly with increasing the atomic radius of the substrate. Using our new equation, the contact angle of water was identified on all of the metals in the periodic table. From the measured contact angle values, the adhesion energy of the distilled water/metal substrate interface was also determined and a correlation with the free electron density parameter of substrates was determined.

1. Introduction

The wettability of metal surfaces by water is essential information for industry and chemical technologies, especially in the corrosion processes of metals, for electrode–electrolyte contact in the case of electrochemical syntheses [1,2], or in the oil industry in the separation of water–oil systems [3,4,5,6,7,8,9,10] and other applications, e.g., metallic nanoparticle preparation or corrosion behavior [11,12,13,14,15]. Several papers report on the study of the wettability in water/metal systems [16,17,18,19,20,21]. Nevertheless, contradictions can be found in the results, as Schrader [18] pointed out. White [22] believes that the contradictory results are due to the formation of an oxide layer of unknown composition and thickness on the surfaces during the cleaning processes, resulting in perfect wetting between water and metals. White [22] and Kaptay [23] point out that water cannot spread well on the surface of oxide-free metals, as the water and metal bond types are different, i.e., we expect good wetting in metallic liquid/metallic substrates or in ionic liquid/ionic substrate systems. In contrast, in water/metal systems, the contact angle (Θ) is generally assumed to be around 60°, which is supported by the results of the experiments by Erb carried out on noble metal surfaces [24]. The contact angle of water on gold at room temperature is about 62° [25]. However, quite different contact angles have been identified in other studies. The predicted water contact angle in [17] for Au is 0°, and the same angle is measured for Ag, Pd, and Pt. Low contact angles were measured by Trevoy and Johnson examining the wettability by the water of Al, Cu, Mg, Ni, stainless steel, and Zn; they found the contact angle was in the range of 5.0–9.1° for all the studied metals [16]. Against this, Mantel and Wightman measured the water contact angle on stainless steel, and the contact angle of water was found to be 49.5° [26]. They found a contact angle of ~10° on O2-treated steel due to the formation of CrO3. The water contact angle was reported on copper (Θ = 72° at 100 °C was measured) by Boyes and Ponter [27], who used Au, Pt, Ag, Cu, and Al as substrates, and the water contact angle was measured with different parameters [28]. Knowing the exact contact angle of the water/metal system is crucial in industrial prediction and modeling, for instance, in lubricant behavior investigation or in the flow of liquids [29,30,31] or in the surface wetting effect on cavitation formation [32], where better wetting leads to lower cavity formation. Additionally, the turbulent or laminar nature of the flow is influenced by the wetting behavior of the surfaces [33,34].
As this brief review reveals, studies have obtained very different results for the contact angle of water on metal surfaces. The literature does not provide a general equation to reliably predict the wetting behavior of metals by water or adhesion energy in water/metal systems.
The aim of our work is to determine the contact angle of distilled water on the surface of a wide range of metals and then to find a correlation between the contact angle and the characteristics of the substrate based on the measured data.

2. Materials and Methods

2.1. Sample Preparation

For the experiments, Ag, Au, Cu, Fe, Nb, Ni, Sn, Ti, and W were used. The 10 mm × 10 mm × 5 mm samples were prepared from the investigated metals (purity of the metals is 99.99%); these samples were the substrates. The metals were ground and polished mechanically; the average surface roughness (Ra) of the substrates was 0.02 µm (MARSURF M 400 Surface Roughness Measuring Instrument). In all cases, the surface of the substrates was polished immediately before the measurement.

2.2. Contact Angle Measurement

The experiments were carried out by the sessile drop method in equipment designed by Sunplant Ltd. (Miskolc, Hungary) (Figure 1).
In the contact angle measurement, a 5 µL distilled water droplet was placed on the surface of a polished substrate using an automatic pipette. The silhouettes of the formed droplet were photographed with a CCD camera, and the contact angle values were determined using KSV software (CAM2008, KSV Instruments Ltd., Helsinki, Finland). The contact angle values are shown as an average of 10 repeated measured data. The experiments were performed in an air atmosphere.

2.3. Validation of the Estimated Contact Angle

The estimation of the contact angles was validated in the cases of the Al, Si, Mo, and Hg. Al, Si, and Mo substrates, which were prepared according to Section 2.1, while Hg, for the substrate preparation, was poured into a Petri dish to minimize the curvature of the Hg surface. The contact angle measurement in all cases was performed according to Section 2.2.
Figure 2 shows a flowchart of the measurement process and analysis of the water contact angle on metal surfaces.

3. Results and Discussion

3.1. Relationship between Measured Contact Angles and Atomic Radii

The measured contact angle values of distilled water on the metal substrates are shown in Table 1.
In accordance with the results of White [22] and Kaptay [23], the contact angle of water on metal surfaces was found to be between 57° and 73° depending on the type of metal. Our results—that the contact angle on metal surfaces is not 0°—is also supported by the fact that microgrooves and micro-textures can improve the lubrication effect during water lubrication tests [30]. In the case of Θ = 0–5°, the liquid spreads perfectly on the surface, and there is no effect of microgrooving on the behavior of the liquid. If the contact angle is around 60°, the water spreads better due to the microgrooves.
The contact angle of the distilled water on metals as a function of the atomic number provides the periodic function shown in Figure 3. It can be seen that the contact angle follows the periodicity according to the periodic number of the substrate; opposite to this trend, the radius of the atoms of the substrate shows the periodicity.
From the opposite periodicity of contact angle and the atom radius of the substrate observed in Figure 3, it can be concluded that the atomic radius of the substrate affects the contact angle value measured on the surface of the substrate. Figure 4 shows the contact angle values as a function of the atomic radius of the substrate. The linear trend of the contact angle as a function of the atomic radius of the substrate is clearly shown.
Considering Figure 4, the contact angle of distilled water on different substrates, taking into account the atomic radius of the substrate, can be described for metallic substrates with the following relation:
Θ = −0.582rA + 148,
where Θ is the contact angle of the distilled water (°) and rA is the atomic radius of the substrate (pm) [35,36].
Since water was used as the liquid phase, the question arises whether a chemical reaction may have occurred between the water and the substrate at room temperature, and the formed reaction product, an oxide, may possibly have affected the contact angle of water. In Figure 5, the free enthalpy of the formation of the possible oxides of the substrates is shown as a function of the atomic radius of the substrate. It can be seen that there is no mathematically descriptive relationship between the free enthalpy of formation and atomic radius (correlation coefficient r = −0.3991 and R2 = 0.1593). This means that the observed wetting behavior is not affected by oxide formation. This is also supported by the fact that carbon fits well in the contact angle–atomic radius diagram (Figure 4) (Θ waterCarbon = 80 ± 5°), while there is no chemical reaction between C and H2O at room temperature.

3.2. Estimation of the Contact Angle of the Distilled Water for the Metals of the Periodic Table

Using Equation (1), it is possible to estimate the contact angle of the distilled water on the surface of the metallic and semi-metallic elements of the periodic table. The estimated contact angles on the metallic and semi-metallic elements are depicted in Figure 6. The estimated contact angles were validated with the contact angle measurement of distilled water on liquid Hg and polished surfaces of Al, Si, and Mo. The results of the measured and validated contact angle can be seen in Table 2. A good correlation can be seen between the measured and estimated data; they overlap within the uncertainty of measurement with an r = 0.8311 correlation coefficient.

3.3. Water/Metal Adhesion Energy

The adhesion energy of the water/metal system can be identified using the contact angle of the water by using the Young–Dupré Equation (2):
W = σlv.(1+cosΘ)
where W is the adhesion energy (J/m2), σlv. is the surface tension of the liquid phase (J/m2), and Θ is the contact angle (°). The wettability of metals and thus the adhesion energy of the water/metal system must also depend on the charged particles located on the surface of the substrate. The metallic substrates have different free electron densities [38], which affect the wetting behavior. The calculated adhesion energy values of the water/metal system (based on Equation (2)) are depicted as a function of the free electron density parameter (Figure 7) according to the W~ f(rS−4) correlation. The rS−4 was established in the work of Wojciechowski [39]; the values of the free electron density (rS) are from Perrott and Rasolt [40]. In Figure 7, a good correlation can be seen between the adhesion energy of the water/metal system and the free electron density parameter (rS−4) of the metals. We can say that the free electron density of the metal substrate determines the adhesion energy of the water/metal system. The correlation is
W = π.rS0.62
The calculated adhesion energy values are checked against Equation (3) in Figure 7. A good correlation can be seen with the semi-empirical coefficient of Equation (3): π ≈ 58 mJ/m2. The correlation coefficient between the free electron density parameter and the calculated adhesion energy is −0.8648, which means that there is a strong correlation between the data.

4. Conclusions

The aim of this investigation was to determine the wetting behavior of the metals and the adhesion energy values in water/metal systems. Furthermore, our goal was to establish new semi-empirical models for the prediction of the contact angle and adhesion energy in water/metal pairs. Our results are summarized in the following points.
−
Using Ag, Au, Cu, Fe, Nb, Ni, Sn, Ti, and W as substrates, the contact angle of the distilled water on the polished surface of the substrates was determined.
−
A new linear relationship was identified between the atomic radius of the substrate element and the contact angle of distilled water.
−
An equation was created (Equation (1)) to estimate the contact angle of distilled water on the surface of the metals and semi-metals of the periodic table. The estimated values were validated with contact angle measurement on Al, Si, Hg, and Mo.
−
The calculated adhesion energy of water/metal systems correlated well with rS−4 (the free electron density parameter) according to Equation (3).
−
These new observations can be used in the preparation of metallic nanoparticles and in water–oil separation.

Author Contributions

Measurement and calculation, L.S.-S. and P.B.; writing, review, and editing, L.S.-S. and P.B. All authors have read and agreed to the published version of the manuscript.

Funding

This research received no external funding.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

All data are in this paper.

Acknowledgments

Prepared with the professional support of the doctoral student scholarship program of the co-operative doctoral program of the Ministry of Innovation and Technology, Hungary, Financed from the national research, development and innovation fund. This work was supported by National Research, Development, and Innovation Fund (2019-1.3.1-KK-2019-00001).

Conflicts of Interest

The authors declare no conflict of interest.

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Metals 12 01274 g001 550
Figure 1. Equipment for the contact angle measurement.
Figure 1. Equipment for the contact angle measurement.
Metals 12 01274 g001
Metals 12 01274 g002 550
Figure 2. Flow chart of the measurement.
Figure 2. Flow chart of the measurement.
Metals 12 01274 g002
Metals 12 01274 g003 550
Figure 3. The measured contact angle of distilled water and radius of the substrate atoms as a function of the substrate atomic number.
Figure 3. The measured contact angle of distilled water and radius of the substrate atoms as a function of the substrate atomic number.
Metals 12 01274 g003
Metals 12 01274 g004 550
Figure 4. The contact angle of distilled water as a function of the atomic radius of the substrate.
Figure 4. The contact angle of distilled water as a function of the atomic radius of the substrate.
Metals 12 01274 g004
Metals 12 01274 g005 550
Figure 5. Free enthalpy of the formation of oxides [37] as a function of the atomic radius of the substrate.
Figure 5. Free enthalpy of the formation of oxides [37] as a function of the atomic radius of the substrate.
Metals 12 01274 g005
Metals 12 01274 g006 550
Figure 6. Contact angle values determined by Equation (1) as a function of the atomic number.
Figure 6. Contact angle values determined by Equation (1) as a function of the atomic number.
Metals 12 01274 g006
Metals 12 01274 g007 550
Figure 7. Adhesion energy (W) as a function of the free electron density parameter following the W~f(rS−4) correlation.
Figure 7. Adhesion energy (W) as a function of the free electron density parameter following the W~f(rS−4) correlation.
Metals 12 01274 g007
Table
Table 1. The measured contact angle on the surface of pure metals.
Table 1. The measured contact angle on the surface of pure metals.
SubstrateAgAuCuFeNbNiSnTiW
Contact angle, ±5°646272725773656263
Table
Table 2. Comparison of the estimated and measured contact angle of water on Al, Si and Mo surfaces.
Table 2. Comparison of the estimated and measured contact angle of water on Al, Si and Mo surfaces.
ElementEstimated Contact Angle
(Figure 6)		Measured Contact Angle
Al66 ± 5°71 ± 5°
Si81 ± 5°76 ± 5°
Hg59 ± 5°58 ± 5°
Mo70 ± 5°76 ± 5°
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Somlyai-Sipos, L.; Baumli, P. Wettability of Metals by Water. Metals 2022, 12, 1274. https://doi.org/10.3390/met12081274

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Somlyai-Sipos L, Baumli P. Wettability of Metals by Water. Metals. 2022; 12(8):1274. https://doi.org/10.3390/met12081274

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Somlyai-Sipos, Laszlo, and Peter Baumli. 2022. "Wettability of Metals by Water" Metals 12, no. 8: 1274. https://doi.org/10.3390/met12081274

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