Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content

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CERAMICS INTERNATIONAL

Ceramics International ] (]]]]) ]]]–]]] www.elsevier.com/locate/ceramint

Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content Fei Caia, Chuanhai Jianga,n, Zhongquan Zhanga, Vincent Jib a

School of Materials Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, PR China b ICMMO/LEMHE, UMR 8182, Université Paris-Sud 11, Orsay Cedex 91405, France Received 28 May 2014; received in revised form 27 June 2014; accepted 27 June 2014

Abstract In this work, Ni–Al–Y2O3 composite coatings with different contents of Y2O3 nanoparticles were prepared from a conventional Watt bath containing different Y2O3 particle loadings (1 g/L, 2 g/L, 5 g/L, 10 g/L). The influences of Y2O3 particle loadings in the bath on the composition, texture, grain size, microstrain, residual stress and hardness of the composite coatings were investigated. The anti-corrosion of the composite coating in NaCl and NaOH solutions were also evaluated in detail. The results showed that the Y2O3 particle content in the composite coatings increased with increasing the particle loadings. The (2 0 0) preferred orientation of the composite coating evolved to (1 1 1) preferred orientation with increasing Y2O3 particle loadings. The composite coating deposited at 5 g/L showed the smaller grain size, lower tensile residual stress and the maximum hardness value. Corrosion experiment showed that the composite coating deposited at 5 g/L exhibited the best corrosion resistance both in NaCl and NaOH solutions. & 2014 Published by Elsevier Ltd and Techna Group S.r.l.

Keywords: Ni–Al–Y2O3 composite coating; Electrodeposition; Texture; Residual stress; Corrosion resistance

1. Introduction Recently, electrodeposited composite coatings reinforced with rare earth oxide (REO, Y2O3, CeO2 and La2O3) have been extensively studied due to their higher microhardness, better wear resistance, improved corrosion resistance and enhanced high temperature oxidation resistance [1–13]. The incorporated rare earth oxide (REO) can hinder the movement of the dislocation or result in finer nickel grains, leading to higher hardness [1,4,6,10–12]. The higher hardness could increase the load carrying capacity and the resistance for plastic deformation, and result in higher wear resistance of the composite coatings [1,4,6,10,12]. The improved corrosion resistance could be ascribed to the incorporated inert particles acted as “physical barriers” in corrosive environments or the formation of many “corrosion micro-cells” in which the inert particles acted as cathode and nickel matrix acted as anode n

Corresponding author. Tel.: þ86 21 34203096. E-mail address: [email protected] (C. Jiang).

[6,11,12]. The grain refining caused by incorporating particles also contributed to the improvement of corrosion resistance of the composite coating [6,11]. The REO reinforced composite coatings also exhibited higher oxidation resistance [5–9]. The incorporated reactive elements (such as Y, Ce, La) or their oxides particles could block the outward diffusion of nickel and change the oxidation mechanism of the coating [6–9]. The oxidation resistance of the composite coatings was improved by decreasing the growth rate of the oxide and increasing the adherence of the oxide scale to the underlying alloys [6,8,9]. Ni–Al composite coatings, another important composite coating reinforced with Al metal particles, have also been extensively studied because of their excellent resistances to high-temperature oxidation and corrosion, [14–20]. Ni–Al coatings exhibited excellent oxidation resistance at high temperature even with low Al content due to the formation of continuous, dense, adherent and protective oxide film on the coating surfaces [14– 18]. The addition of metal Al particle in the coating also improved the anti-corrosion of Ni–Al composite coating due to the formation of Al-oxide-containing-passive-film on the coating

http://dx.doi.org/10.1016/j.ceramint.2014.06.123 0272-8842/& 2014 Published by Elsevier Ltd and Techna Group S.r.l.

Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123

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surface, which prevented further corrosion of the Ni matrix [19,20]. Similar result was also found for Ni–Cr coating [21]. The addition of a reactive element or its oxide could further improve the oxidation resistance of the Ni–Al coatings [22– 26]. The Ni–Al composite coatings with addition of CeO2 exhibited slower oxidation than its counterpart Ni–Al composite coatings, which was ascribed to that the CeO2 profoundly prevented the intergranular cracking [22]. When the β-NiAl phase was dispersed with a small amount of Y2O3 nanoparticles, the formed alumina scale became adherent which could inhibit the further oxidation of the coating [23]. However, the microstructure and property, such as texture, residual stress, hardness and corrosion resistance of the Ni–Al–Y2O3 coatings were few reported and needed further research. In our previous work, Ni–Al composite coatings with different Al particle content were investigated [20]. In this work, the Ni–Al–Y2O3 composite coating with different Y2O3 particle contents were fabricated and the effect of the Y2O3 particle content on the texture, grain size, microstrain, residual stress were investigated. The corrosion resistance of the composite coating was also discussed in detail. 2. Experimental details 2.1. Electrodeposition of Ni–Al–Y2O3 composite coatings Ni–Al–Y2O3 composite coatings were prepared by electrodeposition from Watt baths. The Watt baths were consisted of NiSO4  6H2O (240 g/L), NiCl2  6H2O (40 g/L), H3BO3 (30 g/L) and C12H25NaSO4 (0.2 g/L). The solution temperature was maintained at 50 1C by an automatic controller. The current density was 4 A/cm2, the pH was 4.2 and the stirring rate was 200 rpm. The Al particles content was maintained at 100 g/L and different amounts of Y2O3 particles (1 g/L, 2 g/L, 5 g/L, and 10 g/L) were added to the solution in order to obtain Ni–Al–Y2O3 composite coatings. The diameters of Al and Y2O3 particles were 1 mm and 50 nm, respectively. For all the electrodeposition experiments, the electrolyte was magnetically stirred for 4 h to suspend the particles in the electrolyte. Stainless steel plate with an area of 1 cm2 was used as the cathode, a pure nickel plate was used as the anode. Before the electrodeposition, the stainless steel specimens were grounded by using grade 400, 600 and 1000 emery paper, degreased in acid (10% HCl) and finally washed with distilled water. All the composite coatings were prepared with DC electrodeposition method with deposition time of 60 min. 2.2. Characterization of Ni–Al–Y2O3 composite coatings The surface morphologies of the coatings were examined by a field emission scanning electron microscope (FSEM, JSM7600F) and the chemical composition of coatings was checked with Energy Dispersive X-ray Spectroscopy (EDX) method. The weight fraction of Y2O3 was determined by using the Y to O ratio of 2:3 determined by the chemical formula Y2O3. A Rigaku Ultima IV X-ray diffractometer (XRD, Cu Kα radiation, λ ¼ 1.54056 Å) was used to characterize the phases of the coatings. The voltage and current were 40 kV and

30 mA, respectively. To quantify the relative crystallographic textures of the coatings, the texture coefficients (TC) for predominant (h k l) peaks in XRD patterns were calculated according to the following formula [27],   Iðh k lÞ 1 Iðh k lÞ  1 ∑ TCðh k lÞ ¼ I 0 ðh k lÞ n I 0 ðh k lÞ where I(h k l) is measured intensity of (h k l) reflection, I0(h k l) is powder diffraction intensity of nickel, and n is the number of reflections used in the calculations. In this case, (1 1 1), (2 0 0) and (2 2 0) peaks are used for texture coefficient calculation (n ¼ 3). The grain size and micro-strain of the coatings were obtained by using Voigt method according to the integral breadth of (2 0 0) peak. The relationship of integral breadth could be shown in the following formula [28]: 2

βhC ¼ βfC þ βgC ;

2

2

βhG ¼ βfG þ βgG

where subscript C and G denote the Cauchy and Gaussian components, and superscripts h, f, g denote the measured line profile, the structural broadened profile and the instrumental profile, respectively. Then, the domain size (D) and microstrain (ε) can be calculated by formula: D¼

λ βfC cos θ

;

ε¼

βfG 4 tan θ

where λ, β, θ represent the wavelength of Cu-Kα, integral breath and Bragg angle, respectively. The residual stress of the as-deposited Ni–Al composite coatings was determined by the classical sin2ψ method [29]. The sin2ψ method was made on a Proto LXRD Residual Stress Analyser, the voltage and current were 30 kV and 25 mA, respectively. The peaks of (4 2 0)α of Ni were used to calculate the residual stress. The Vickers microhardness measurements were carried out with loads of 200 g and indentation time of 15 s. The corresponding final values were determined as the average of 8 measurements. Potentiodynamic polarization measurements were conducted both in 0.6 M NaCl and 1 M NaOH solutions at the ambient temperature using an electrochemical apparatus (CHI660E, Shanghai Chenhua, China), respectively. A standard three electrode system was used, with a Ag/AgCl electrode [þ 207 mV (SHE)] as the reference electrode, a platinum sheet as the auxiliary electrode (AE) and the sample as the working electrode (WE). The scan rate was 1 mV/s. The polarization potentiodynamic curves were recorded after 30 min of immersion. The corrosion current density Icorr for the particular specimens was determined by extrapolating the anode and cathode Tafel curves. 3. Results and discussions 3.1. Y2O3 particle content analysis Fig. 1(a) and (b) shows the surface morphology and the corresponding EDX of the Ni–Al–Y2O3 composite coating

Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123

Y2O3 particle content in deposits, wt %

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3

12 10 8 6 4 2 0 0

2

4

6

8

10

Y2O3 particle loading in bath, g/L Fig. 2. Y2O3 particle content in the deposits as a function of the Y2O3 loadings in the bath.

Y2O3 particle content in the deposits attained the maximum value of 9.71 wt% at 10 g/L. 3.2. Coating microstructures and texture

Fig. 1. (a) Surface morphology image and (b) the corresponding EDX of Ni– Al–Y2O3 composite coatings deposited at 10 g/L.

deposited at Y2O3 particle loadings of 10 g/L. As seen in Fig. 1(a), the coating deposited at 10 g/L showed some colonized structure typical for composite coating [6,7,20]. The EDX results confirmed the detection of Ni, Al and Y elements as shown in Fig. 1(b). The Y2O3 particle content in the deposits as a function of Y2O3 particle loadings is ploted in Fig. 2. It was found that the Y2O3 particle content increased with increasing the Y2O3 particle loadings in bath. The average Y2O3 content for the composite coatings determined from the EDX results were 1.06 wt%, 3.75 wt%, 7.86 wt% and 9.71 wt% for the coatings deposited at Y2O3 particle loadings of 1 g/L, 2 g/L, 5 g/L and 10 g/L, respectively. The electro-codeposition mechanism of the particles has been well studied in the past several decades and several models have been developed [30–32]. The co-deposition process of the Y2O3 particles could be explained by the Guglielmi’s two-step adsorption model [30]. First, the Y2O3 particles with adsorbed ions were physically and loosely adsorbed on the cathode surface. Second, the metal ions adsorbed on the Y2O3 particles were reduced, making the Y2O3 particles strongly absorb on the growing surface and to be embedded in the coating. In this study, with increase of the Y2O3 particle loadings, the probability of the Y2O3 particles absorbing on the growing coating surface increased. Thus, the

The XRD patterns of the Ni–Al–Y2O3 composite coating deposited at different Y2O3 particle loadings are shown in Fig. 3(a). All the Ni peaks exhibited the face-centered cubic (FCC) crystal structure (JCPDS card no. 04-0850). The coating deposited at 1 g/L exhibited (2 0 0) preferred orientation. As the Y2O3 particle loadings increased, the (2 0 0) preferred orientation was suppressed and random orientation occurred. With further increase in the Y2O3 particle loading up to 10 g/L, the Ni–Al coating exhibited (1 1 1) preferred orientation. In addition, the peaks of Al and Y2O3 particles were also observed as shown in Fig. 3(b) for coating deposited at 5 g/L. Fig. 4 presents the calculated texture coefficient results of coating with different Y2O3 particle content. The (2 0 0) texture coefficients decreased while the (1 1 1) texture coefficients increased with the increasing Y2O3 particle loadings. The results above showed that incorporation of Y2O3 particles could change the preferred orientations of the electrodeposited coating. In the electrodeposition process, some chemical species such as nickel hydroxide and hydrogen were formed and partially adsorbed on the surface of cathode or the growing coating, which inhibited the (2 0 0) texture model [6]. As the Y2O3 content increased to a critical value 3.75 wt% in this instance, renucleation occurred on both (1 1 1) and (2 2 0) planes, which led to random grains growth. The addition of Y2O3 particles also had an effect on the grain size and microstrain of the coatings. Fig. 5(a) and (b) demonstrate the grain size and microstrain of the Ni–Al–Y2O3 composite coatings deposited at different Y2O3 particle loadings, respectively. As seen in Fig. 5(a), the grain size of the coating decreased with increasing the Y2O3 particle loadings and obtained the minimum value of 57 nm at 5 g/L beyond which the grain size increased again. During the electroplating process, the incorporated Y2O3 particles could act as new nucleus and promote the grain nucleation rather than the grain

Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123

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Y2O3 particles. It could be also found in Fig. 5(b) that the microstrain of the composite coating increased with increasing the Y2O3 particle loadings.

(200) •

• Ni 4

×10

(111)

3.3. Residual stress analysis

Intensity, CPS

•

6 (220) (311)(222) •

4

• •

1 g/L

2 g/L 2

5 g/L 10 g/L

0

20

40

60

80

100

120

Diffraction angle 2θ , deg •

•

• • Ni ♦ Al ♣ Y2O3

Intensity, CPS

3.4. Hardness measurements

0.2

The microhardness of Ni–Al–Y2O3 coatings deposited at different Y2O3 particle loadings are indicated in Fig. 7. It was found that the hardness values of the composite coatings increased with increasing the Y2O3 particle loadings and attained the maximum at 5 g/L beyond which the hardness value decreased slightly. The hardness enhancement for the Ni–Y2O3 composite coatings was related to the grain refinement strengthening from the Ni matrix and the dispersion strengthening caused by the Y2O3 particles. First, the variation of the hardness values was consistent with that of grain size of the composite coating that the maximum hardness was observed for coating with smaller grain size. Thus, grain refinement strengthening might be the main strengthening mechanism for the composite coating [12]. Second, the enhancement in the hardness of the composite coatings was also related to the dispersion strengthening caused by the Y2O3 particles, which hindered the motion of dislocations [1,6,10]. As the Y2O3 particle loadings increased, the hardness of the composite coatings increased. However, the hardness of the composite coating decreased with further increasing the Y2O3 particle loadings to 10 g/L, which might be due to the aggregation of the Y2O3 particles.

0.1

3.5. Potentiodynamic polarization

• ♣

20

•

♦ ♣

♣ 40

♣ 60

♦

♦ 80

100

120

Diffraction angle 2θ , deg Fig. 3. The XRD patterns of the Ni–Al–Y2O3 composite coating deposited at different Y2O3 particle loadings (a) and the typical XRD pattern of coating deposited at 5 g/L.

0.7

Texture Coefficient (TC)

Fig. 6 shows the residual stresses of Ni–Al–Y2O3 coatings deposited at different Y2O3 particle loadings and all the coatings had low tensile residual stresses. The tensile residual stresses of 35 MPa, 26 MPa, 14 MPa and 30 MPa were obtained for coatings deposited at Y2O3 particle loadings of 1 g/L, 2 g/L, 5 g/L and 10 g/L, respectively. The generation of tensile residual stresses could be ascribed to the decreasing structural mismatch and the grain coalescence [35]. It was found that the variation of the residual stress of the coatings agreed with the variation of grain size that coating with smaller grain exhibited lower residual stress, which was due to that the residual stress cannot accumulate as much as with larger grains [36].

(111) (200)

0.6 0.5 0.4 0.3

0

2

4

6

8

10

Y2O3 particle loading in bath, g/L Fig. 4. Texture coefficients (TC) of the Ni–Al–Y2O3 composite coatings deposited at different Y2O3 particle loadings.

growth, which was also found for TiO2 [33,34]. Thus, the grain size decreased with increasing the Y2O3 particle contents. However, as the Y2O3 particle loading increased up to 10 g /L, the grain size increased due to the aggregation of the

The potentiodynamic polarization curves of composite coatings with different Y2O3 particle in 0.6 M NaCl and 1 M NaOH solution are shown in Figs. 8 and 9, respectively. The corrosion potential Ecorr and corrosion current Icorr obtained from the polarization curves were summarized in Table 1. As the Y2O3 content increased, the corrosion potential Ecorr increased for coatings both in NaCl and NaOH solutions and the corrosion current Icorr decreased and obtained the minimum value at 5 g/L, indicating the best corrosion resistance for coating deposited at 5 g/L. Then, the corrosion current Icorr increased slightly with

Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123

120

0.19

110

0.18

100

0.17

Microstrain, %

Grain Size, nm

F. Cai et al. / Ceramics International ] (]]]]) ]]]–]]]

90 80 70 60

5

0.16 0.15 0.14 0.13 0.12

50

0.11

40 0

2

4

6

8

10

0.10 0

2

Y2O3 particle loading in bath, g/L

4

6

8

10

Y2O3 particle loading in bath, g/L

Fig. 5. (a) Grain size and (b) microstrain of the coating as a function of particle loadings.

45

380

Microhardness, Hv

Residual Stress, MPa

40 35 30 25 20

360 340 320 300

15 280

10 260

5 0

2

4

6

8

10

0

Y2O3 particle loading in bath, g/L Fig. 6. Residual stresses of coatings deposited at different Y2O3 particle loadings.

further increasing Y2O3 particle up to 10 g/L. The corrosion current Icorr for coating in NaOH solution were two magnitudes more than that in NaCl solution. The passivation process was also observed for coatings in NaOH solution as shown in Fig. 9. The corrosion resistance of the coating was related with the grain size and the higher anti-corrosion was observed for coating with smaller grain, which facilitated the rapid formation of continuous Ni(OH)2 passive films and the smaller grain possessed longer circuitous length to substrate [12,37]. From this view, the corrosion resistance of the Ni–Al–Y2O3 composite coating agreed with the variation of grain size with increasing Y2O3 particle loadings. The coating deposited at 5 g/L showed the smaller grain size, thus the better corrosion resistance. In view of that the corrosion current Icorr of coating deposited at 10 g/L were very close to that deposited at 5 g/L, therefore, the corrosion resistance of the coatings could be considered to increase with increasing the Y2O3 particle content. The improvement of corrosion resistance of Ni–Al– Y2O3 coating were also related with the increasing Y2O3 particle content in the coating and the texture evolution from (2 0 0) planes to (1 1 1) planes. It was believed that these

2

4

6

8

10

Y2O3 particle loading in bath, g/L Fig. 7. The microhardness of Ni–Al–Y2O3 coatings deposited at different Y2O3 particle loadings.

incorporated neutral particles could act as “physical barriers” in corrosive environments, which improved the anti-corrosion of the composite [12,37]. The second factor was related with the texture evolution. The close packed planes or the low index planes are known to be more resistant to dissolution because of the higher binding energy of the surface atoms [38,39]. In this case, the (1 1 1) plane was the close packed plane and it possessed higher corrosion resistance than the (2 0 0) plane. As the Y2O3 content increased, the crystallographic planes of the Ni–Al composite coating evolved from (2 0 0) plane to (1 1 1) plane. Thus, the corrosion resistance of the Ni–Al–Y2O3 coatings improved. 4. Conclusions Ni–Al–Y2O3 composite coatings with different Y2O3 particle contents were deposited from a conventional Watt bath and the microstructures and properties were examined by different characterization methods. The Y2O3 particle content in the composite coating increased with increasing the Y2O3 particle loadings and attained the maximum value of 9.71 wt% at 10 g/L. The increasing Y2O3 particles content had an effect on the

Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123

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Log (current density), Log (Acm-2)

6

Y2O3 particle contents possessed low tensile residual stress and the coating deposited at 5 g/L showed the minimum residual stress. The composite coating deposited at 5 g/L also exhibited the maximum hardness value due to the grain strengthening. The corrosion experiment showed the composite coating deposited at 5 g/L exhibited the best corrosion resistance both in NaCl and NaOH solutions, which was due to the decreasing grain size with increasing the Y2O3 content.

-2 1 g/L

-3 -4 2 g/L

-5 -6 -7

5 g/L

10 g/L

-8

References

-9 -10 -0.4

-0.2

0.0

0.2

0.4

0.6

Potential, V Fig. 8. Potentiodynamic polarization curves for Ni–Al–Y2O3 coatings with different Y2O3 particle contents in 0.6 M NaCl solution.

Log (current density), Log (Acm-2)

0 -1 -2

1 g/L

-3

2 g/L

5 g/L

-4 -5 -6

10 g/L

-7 -8

-1.5

-1.0

-0.5

0.0

0.5

1.0

1.5

Potential, V Fig. 9. Potentiodynamic polarization curves for Ni–Al–Y2O3 coatings with different Y2O3 particle contents in 1 M NaOH solution.

Table 1 Corrosion potential Ecorr and corrosion current Icorr of coating deposited at different Y2O3 particle loadings. Solution

Y2O3 particle loadings (g/L)

Ecorr (mV)

Icorr (mA/cm2)

NaCl

1 2 5 10 1 2 5 10

129.2 111.2 88.2 60.2 776.4 753.6 727.3 711.7

0.916 0.543 0.120 0.154 0.423  102 0.233  102 0.193  102 0.207  102

NaOH

microstructures and properties of the coatings. As the Y2O3 particle content increased, the (2 0 0) preferred orientation was suppressed and the coatings showed (1 1 1) orientations with further increasing Y2O3 up to 10 g/L. The grain size decreased and the microstrain increased as the Y2O3 particles increases. The grain size obtained the minimum value of 57 nm at particle loading of 5 g/L. All the Ni–Al–Y2O3 coatings with different

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Please cite this article as: F. Cai, et al., Synthesis and characterization of Ni–Al–Y2O3 composite coatings with different Y2O3 particle content, Ceramics International (2014), http://dx.doi.org/10.1016/j.ceramint.2014.06.123