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Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition
Accepted Manuscript Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition Chao Liu, Jiaqian Qin, Zhihao Feng, Shiliang Zhang, Mingzhen Ma, Xinyu Zhang, Riping Liu PII:
S0925-8388(17)34221-4
DOI:
10.1016/j.jallcom.2017.12.046
Reference:
JALCOM 44132
To appear in:
Journal of Alloys and Compounds
Received Date: 30 July 2017 Revised Date:
4 December 2017
Accepted Date: 5 December 2017
Please cite this article as: C. Liu, J. Qin, Z. Feng, S. Zhang, M. Ma, X. Zhang, R. Liu, Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition, Journal of Alloys and Compounds (2018), doi: 10.1016/j.jallcom.2017.12.046. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition
Zhanga,*, and Riping Liua
State Key Laboratory of Metastable Materials Science and Technology, Yanshan
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a
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Chao Liua, Jiaqian Qin b,*, Zhihao Fenga,c, Shiliang Zhanga,*, Mingzhen Maa, Xinyu
b
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University, Qinhuangdao 066004, P. R. China
Surface Coatings Technology for Metals and Materials Research Unit, Metallurgy
and Materials Science Research Institute, Chulalongkorn University, Bangkok 10330, Thailand
School of Materials Science and Engineering, Hebei University of Science and
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c
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Technology, Shijiiazhuang 050000, P. R, China
*Corresponding Author. Fax: +66 2611 7586 E-mail:
[email protected]
(J.
Qin),
[email protected] (S. Zhang) 1
[email protected]
(X.
Zhang),
ACCEPTED MANUSCRIPT Abstract The microstructure and mechanical properties of (Zr-Ti)χNi1-χ(χ=1, 3, and 5 wt.%) alloys were studied. With the addition of nickel (Ni), the phase composition of alloys
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changes from α phase to α phase + hexagonal close packed (hcp) C14 Laves-phase. The thickness of lamellar α phase decreases with increasing Ni content. Optical microscopy and transmission electron microscopy results indicated that Zr-Ti-Ni C14
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Laves-phase is formed on the boundary. The Zr-Ti-3wt.%Ni alloys exhibits better
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ultimate compressive strength and compressive plasticity (1715 MPa and 9.70%) than that of Zr-Ti alloys (1598MPa and 12.4%). The decrease of the average thickness of the lamellar α-phases (from 0.183µm to 0.065µm) leads to the improvement of the strength of the alloy. Additionally, the solid solution strengthening and the second
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phase strengthening is also important reasons for the improvement of the strength.
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Keywords: Zr-Ti alloy; nickel addition; C14 Laves-phase; mechanical properties
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ACCEPTED MANUSCRIPT 1 Introduction
Zirconium-Titanium (Zr-Ti) binary alloys are extensively studied in aviation, biological and industrial applications due to their low neutron-capture, eximious
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corrosion, thermal stability and excellent irradiation[1-6]. Physicochemical properties of Zr and Ti are similar because of there are the same primary group in the periodic
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table Zr-Ti binary phase diagram shows, those two elements can form infinite solid solutions of hexagonal close-packed structure (hcp) in α transition temperature region
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and body-centered cubic structure (bcc) in β transition temperature region[7]. Microstructure, such as phase composition, grain size, shape and composition distribution in matrix, is a critically important characteristic because of its important influence on the mechanical properties[8-14]. Pervious noted that the variety of phase
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composition strongly affects the mechanical properties of Zr alloys[15]. Feng et al.[16-19] reported that the average size of the grain and second phase particles
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compound is related to the mechanical of properties of Zr/Ti alloys. Kendig et al.[20, 21] showed that the mechanical properties increased with increasing solid solution
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strengthening and dispersion strengthening. Ni is an important alloying element that is widely used to improve the
mechanical properties of alloys effectively. The solute elements Ni leading to the decrease in the critical cooling rate[22]. Wang et al. reported that Ni addition to solders raising solder joint strength[23]. Many other studies also show that Ni can improve the mechanical properties of the matrix alloy[9, 24-26]. However, the effect of addition of Ni on the mechanical properties of Zr-Ti 3
ACCEPTED MANUSCRIPT alloys has not been reported. The present investigation mainly reveals the addition of Ni in Zr-Ti binary alloys is effective in the refinement of microstructural and promoting mechanical properties. More than this study will concentrates on the
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microstructure phase compositions, and compressive properties of as-cast Zr-Ti-Ni
2. Materials and Methods
materials
used
include
Zr-Ti
(ZTN0),
Zr-Ti-1wt.%Ni
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The
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alloys.
(ZTN1),
Zr-Ti-3wt.%Ni (ZTN3) and Zr-Ti-5wt.%Ni (ZTN5). The pure Zr (99.9 wt.%), Ti (99.9 wt.%) and Ni ( 99.9 wt.%) were used to prepare the ZTN series alloys. These
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materials were provided by ZhongNuo Advanced Material Technology Co., Ltd. The melted alloys were then flipped at least and re-melted six times using a vacuum arc melting furnace equipped with a water-cooling system under a Ti-gettered argon
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atmosphere to achieve appropriate homogeneity and minimize compositional
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segregation. The weight of four alloy samples was approximately 60g. X-ray fluorescence was used to analyze the composition of the sample and shown in Table 1. For compressive tests, the cylindrical samples with diameter of 5 mm and height
of 10 mm were prepared. The compression tests were conducted on an Instron 5982 testing machine at a strain rate of 5×10-4S-1. The phase composition of the specimens was examined using a conventional X-ray diffraction (XRD) with Cu Kα radiation. Optical microscopy (OM), scanning electron microscopy (SEM) and transmission 4
ACCEPTED MANUSCRIPT electron microscopy (TEM) were used for microstructural analysis. Hardness tests were performed on FM-ARS 9000 type Vickers hardness tester at a load of 200gf for
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10S. The final hardness value is the average of at least 10 effective tests.
Table 1. Nominal chemical composition (and analyzed chemistry) of the current alloys (wt.%). Zr
Ti
Ni
ZTN0
50 (49.97)
50 (50.46)
0
ZTN1
49.5 (49.52)
49.5 (49.50)
1(1.01)
ZTN3
48.5 (48.51)
48.5 (48.52)
3 (3.02)
ZTN5
47.5 (47.5)
47.5 (47.5)
5 (4.98)
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Alloys
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3. Results and discussion
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The XRD patterns of the as-cast alloys are shown in Fig. 1. The as-cast Zr-Ti alloy showed α phase with no other intermetallic compound or phase. This characteristic can be explained by Zr-Ti binary phase diagram[27], those two elements can form infinite solid solutions of hcp structural α phase in room temperature. Fig. 2 indicates that the crystal parameters of α phase decrease with the content of Ni increasing. Because of the small atomic radius of Ni (0.125nm) compared with Zr (0.160nm) and Ti (0.147nm), the addition of Ni results in a decrease of lattice 5
ACCEPTED MANUSCRIPT parameters “a” and “c”, but the axial ratio “c/a” increases. These distortions cause the XRD peaks shift to higher angle when the Ni content increasing. This result means that the Ni addition does lead to the formation of the solid solution with matrix.
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According to Zr-Ni and Ti-Ni binary phase diagram[27], Ni has low solid solubility in Zr-Ti matrix. Thus the C14 Laves-phase arises in the alloys. The C14 can be observed in ZTN5 sample by XRD, as shown in Fig.1, when the accession of Ni reaches to 5
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wt.%. But no peaks of C14 phase were detected in the XRD patterns ZTN1 and ZTN3
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samples because the content of C14 phase is very few with Ni content less than 5 wt.%. In order to further verify that, the TEM bright field images of the microscopic morphology and selected area electron diffraction pattern (SAED) of C14 Laves-phase were obtained and shown in Fig. 3 (a-c). Moreover, the SEM image of
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C14 Laves-phase was also presented in Fig. 3(d) to show the precipitation of C14 phase in the grain boundary. It can be seen that more compounds are produced with Ni content increasing. Similarly, the Ni addition can cause the formation of C14
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Laves-phase which has also been reported in previous literatures [28-30].
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Addition of Ni remarkably affects the α grain size. The OM images of the as-cast Zr-Ti-Ni alloys revealing microstructural features results are given in Fig. 4. The sample of Zr-Ti binary alloy is composed of α-phase completely, with prior-β grain boundaries retained. The β phase convert to α phase is solid phase transformation. The liquid phase transform the β grain take place when the liquid-to-solid transition. And with the temperature is further reduced, the solid phase transition from β to α grain take place. The nucleation and growth of the α phase started near the prior β grain 6
ACCEPTED MANUSCRIPT boundaries[17, 31]. Also, the OM results (Fig. 4) indicate gradual changes in the microstructure with increasing Ni content. TEM and SEM experiments were performed to further observe and analyze the microscopic morphology characteristic
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of the C14 Laves-phase (Fig. 3). The C14 Laves-phase appeared on the grain boundary of the prior-β phase, as shown in Fig. 4(d), which is consistent with the TEM and SEM results. Furthermore, the thickness of the lamellar α phase gradually
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decreases with increasing of Ni content. TEM bright field image and SAED reveal
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that a large number of lamellar α phase appears inside of prior-β grain in the as-cast Zr-Ti-Ni alloy (Fig.5). It also confirms that the thickness of α lamellar is decreased with Ni content increasing from 0 to 5 wt.%. The average α grain size was measured by using Nano Measurer software[32] (Fig. 6). It gradually decreases from 0.183 µm
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to 0.065 µm when Ni content gradually increased from 0 wt.% to 5 wt.%. According to the Zr-Ni and Ti-Ni binary phase diagram, Ni had marginal solubility in Zr-Ti matrix. The nucleation and growth of α grain would be influenced by the increase of
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the Ni concentration. The site of α-phase nucleates and grows near these prior-β
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boundaries or inside the grain. In the case of Ni addition, more C14 Laves-phase particles can be formed, and the site of α-phase nucleates increases. Moreover, the increasing in the number of C14 Laves-phase particles will pin the grain boundaries, resulting in prevent in the further growth of the grain boundaries. A similar result was also observed in Cu3Sn alloys[23]. Fig.7 and Table 2 exhibits the compressive stress-strain curves and compressive test results of the as-cast samples. The compressive properties of the as-cast alloys 7
ACCEPTED MANUSCRIPT were evaluated through room temperature compressive tests. The ultimate compressive strength (UCS) and yield strength (YS) gradually increase and compressive plasticity (ε) gradually decrease when the content of Ni in the alloys
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increase from 0 wt.% to 5 wt.%. As for ZTN3 alloy exhibit better comprehensive mechanical properties. The UCS, YS and ε of the as-cast ZTN3 are 1715 MPa, 1258 MPa and 9.70%, respectively. The microhardness (Hv) of the specimens under
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different Ni content is shown in Fig. 8. The microhardness of as-cast ZTN0 alloy is
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approximately 312 Hv. Nevertheless, the highest microhardness of alloys prepared with 5 wt.% Ni addition can be obtained about 418 Hv. This result, which is consistent with the compressive properties, could be attributed to the amount of Ni
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Table 2. Compressive strength of the as-cast Zr-Ti-Ni alloys.
1598
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UCS (MPa)
ZTN0
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Alloys
ZTN1
ZTN3
ZTN5
1651
1715
1691
YS (MPa)
1117
1159
1258
1648
ε (%)
12.40
10.20
9.70
2.67
The mechanical properties of as-cast Zr-Ti-Ni alloys are greatly influenced by phase composition and microstructure. The stress-strain curve and microhardness results indicate that the addition of Ni in Zr-Ti matrix could contribute to solid 8
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strengthening[33],
grain
refinement[34]
and
the
secondary-phase
strengthening[35-37], thus the better strength of the Zr-Ti-Ni alloys can be prepared. Firstly, lattice distortion is a significant strengthening mechanism of solid solution
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strengthening. The solid solution strengthening of alloys is known to arise from dislocations pinned through interactions with the solute atoms and higher stresses. In this situation, higher stresses are required for dislocation movement through a solute
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field[38-41]. Except that, Fleischer demonstrated that YS is related to the
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concentration of solute atoms[41]. The concentration of solute atoms also plays a very important role in solid solution strengthening. It can be considered as follows: σ∝C2/3, where σ is the YS and C is the concentration of the solute atom. The values of σ as a function of the concentration of the solute atom Ni is shown in Fig. 9. It is obviously
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revealed that solid solution of Ni in the Zr-Ti matrix enhances the YS of the alloys with containing Ni contents from 0 wt.% to 5 wt.%. Secondly, C14 Laves-phase particles on the grain boundaries prevent the growth of α lamellar, resulting in the
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thinner of the α grain size. As we known, the strength of alloys is related to the α grain
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size. Utilizing the Hall-Petch formula (i.e. σ=σ0+kd-1/2, Where σ0 is the yield strength of the matrix alloy, σ is the yield strength (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%). k is the slope of Hall-Petch and d the thickness of the lamellar α phase as shown in Fig. 5). The formula illustrates that the strength of the alloys increases with the grain size decreasing [42, 43]. In the others, the yield strength improvement originates from dislocation pile-up at the grain boundary. The smaller size of α lamellar causes the increase in the number of grain boundary of the unit volume. And more grain 9
ACCEPTED MANUSCRIPT boundaries are act as the obstacle to hinder the motion of dislocation. As we can see from the Table 2 and Fig.6, the yield strength of (Zr-Ti)χNi1-χ alloys increase as lamella thickness d decrease. Above all, the YS of alloys can be improved[18]. In
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addition to the effect of grain refinement strengthen; the second phase particles also play an important role on the increase strength of the alloy. Generally speaking, the hard C14 Laves-phase plays the role of obstruction when dislocations are movement.
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The resistance increases as C14 Laves-phase content from 0 wt.% to 5 wt.%, at the
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same time, greater forces are required to move dislocations. So, it can be concluded that the YS of (Zr-Ti)χNi1-χ alloys could be strengthen by adding Ni element. In Fig. 7 and Table 2, the UCS slightly decreases when the Ni content from 3 wt.% increased to 5 wt.%. The materials fracture before the higher strength due to the bad plasticity of
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However, the ε of the as-cast (Zr-Ti)χNi1-χ alloys reduces with the Ni addition. With the Ni content increasing, the poor ε could be caused by the dislocation density
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increasing and the different sizes between the solute atoms Ni and the elements of the
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matrix. The phase segregation of C14 Laves can be detected on the prior-β grain boundaries, which obstructs dislocation migration and reduces plasticity[44]. Chen et al. [9] also reported that the Ni-containing compounds can decrease plasticity. The fracture morphology of the compressive tested specimens of as-cast Zr-Ti-Ni
alloys with different Ni contents is shown in Fig. 10. ZTN0 alloy (Fig. 10(a)) reveals typical characteristic of ductile fracture, the dimples appear on the fracture surface. The fracture morphology of the ZTN1 alloy exhibits different size dimples and 10
ACCEPTED MANUSCRIPT river-shaped pattern (Fig. 10(b)), which is responsible for the fracture behavior from ductile to brittle. Fig. 10(c) shows typical characteristic features of brittle fracture, including a fracture morphology crystal sugar pattern. While the macroscopic crack
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generate on the fracture morphology of ZTN5 (Fig. 10(d)), which would attribute to
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the poor compressive plasticity for ZTN5.
4 Conclusion
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In the present study, the mechanical properties and microstructure of as-cast Zr-Ti-Ni alloys were studied. The following generalized conclusions can be drawn from this study.
The as-cast Zr-Ti-Ni alloys samples are confirmed to consist of the α-phase and
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the C14 Laves-phase after Ni addition.
The thickness of α lamellar gradually decreases with increasing of Ni content in the alloys.
Zr-Ti-3wt.%Ni alloy has a better mechanical properties. The ultimate
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compressive strength, yield strength and compressive plasticity are 1715 MPa, 1258 MPa and 9.70%, respectively.
The fracture behavior could be turned by the addition of Ni content in the as-cast Zr-Ti-Ni alloys.
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ACCEPTED MANUSCRIPT Acknowledgment This research is funded by NSFC (grant 51571174), National Science Foundation for Distinguished Young Scholars for Hebei Province of China (grant E2016203376), and
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Hundred Excellent Innovative Talents Support Program in Hebei Province (grant SLRC2017056). J.Q would like to acknowledge the support from Thai Government Budget (2017), Chulalongkorn University (GB_B_60_114_62_03), Ratchadapisek
Technology
for
Metals
and
Materials
Research
Unit
(GRU
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Coatings
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Sompoch Endowment Fund, Chulalongkorn University, granted to the Surface
60-001-62-001-1), and State Key Laboratory of Metastable Materials Science and Technology, Yanshan University. Reference
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Figure Captions
Fig.1 XRD patterns of the as-cast ZTN0, ZTN1, ZTN3 and ZTN5 alloys. Fig.2 α phase crystal lattice parameter of (Zr-Ti)χNi1-χ alloys.
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Fig.3 Bright field TEM and SEM micrographs of C14 Laves-phase, (a) as-cast ZTN1, (b) as-cast ZTN3, (c) as-cast ZTN5, (d) as-cast ZTN5. Fig.4 Optical micrographs, (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and
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(d) as-cast ZTN5.
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Fig.5 Bright field TEM micrographs of α lamellar of as-cast (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%), alloy, (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and (d) as-cast ZTN5
Fig.6 The thickness of α lamellar distribution of as-cast (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%), (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and (d) as-cast ZTN5. Fig.7 Engineering compressive stress-strain at room temperature for the vary amount of add Ni into the Zr-Ti alloys. 18
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The effect of Ni addition on the microstructural of Zr-Ti alloys is studied. The mechanism of microstructural evolution is discussed. C14 Laves-phase is formed on the grain boundary. Strength mechanism is proposed from different aspects.
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1. 2. 3. 4.
S0925-8388(17)34221-4
DOI:
10.1016/j.jallcom.2017.12.046
Reference:
JALCOM 44132
To appear in:
Journal of Alloys and Compounds
Received Date: 30 July 2017 Revised Date:
4 December 2017
Accepted Date: 5 December 2017
Please cite this article as: C. Liu, J. Qin, Z. Feng, S. Zhang, M. Ma, X. Zhang, R. Liu, Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition, Journal of Alloys and Compounds (2018), doi: 10.1016/j.jallcom.2017.12.046. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT Improving the microstructure and mechanical properties of Zr-Ti alloy by nickel addition
Zhanga,*, and Riping Liua
State Key Laboratory of Metastable Materials Science and Technology, Yanshan
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a
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Chao Liua, Jiaqian Qin b,*, Zhihao Fenga,c, Shiliang Zhanga,*, Mingzhen Maa, Xinyu
b
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University, Qinhuangdao 066004, P. R. China
Surface Coatings Technology for Metals and Materials Research Unit, Metallurgy
and Materials Science Research Institute, Chulalongkorn University, Bangkok 10330, Thailand
School of Materials Science and Engineering, Hebei University of Science and
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c
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Technology, Shijiiazhuang 050000, P. R, China
*Corresponding Author. Fax: +66 2611 7586 E-mail:
[email protected]
(J.
Qin),
[email protected] (S. Zhang) 1
[email protected]
(X.
Zhang),
ACCEPTED MANUSCRIPT Abstract The microstructure and mechanical properties of (Zr-Ti)χNi1-χ(χ=1, 3, and 5 wt.%) alloys were studied. With the addition of nickel (Ni), the phase composition of alloys
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changes from α phase to α phase + hexagonal close packed (hcp) C14 Laves-phase. The thickness of lamellar α phase decreases with increasing Ni content. Optical microscopy and transmission electron microscopy results indicated that Zr-Ti-Ni C14
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Laves-phase is formed on the boundary. The Zr-Ti-3wt.%Ni alloys exhibits better
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ultimate compressive strength and compressive plasticity (1715 MPa and 9.70%) than that of Zr-Ti alloys (1598MPa and 12.4%). The decrease of the average thickness of the lamellar α-phases (from 0.183µm to 0.065µm) leads to the improvement of the strength of the alloy. Additionally, the solid solution strengthening and the second
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phase strengthening is also important reasons for the improvement of the strength.
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Keywords: Zr-Ti alloy; nickel addition; C14 Laves-phase; mechanical properties
2
ACCEPTED MANUSCRIPT 1 Introduction
Zirconium-Titanium (Zr-Ti) binary alloys are extensively studied in aviation, biological and industrial applications due to their low neutron-capture, eximious
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corrosion, thermal stability and excellent irradiation[1-6]. Physicochemical properties of Zr and Ti are similar because of there are the same primary group in the periodic
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table Zr-Ti binary phase diagram shows, those two elements can form infinite solid solutions of hexagonal close-packed structure (hcp) in α transition temperature region
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and body-centered cubic structure (bcc) in β transition temperature region[7]. Microstructure, such as phase composition, grain size, shape and composition distribution in matrix, is a critically important characteristic because of its important influence on the mechanical properties[8-14]. Pervious noted that the variety of phase
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composition strongly affects the mechanical properties of Zr alloys[15]. Feng et al.[16-19] reported that the average size of the grain and second phase particles
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compound is related to the mechanical of properties of Zr/Ti alloys. Kendig et al.[20, 21] showed that the mechanical properties increased with increasing solid solution
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strengthening and dispersion strengthening. Ni is an important alloying element that is widely used to improve the
mechanical properties of alloys effectively. The solute elements Ni leading to the decrease in the critical cooling rate[22]. Wang et al. reported that Ni addition to solders raising solder joint strength[23]. Many other studies also show that Ni can improve the mechanical properties of the matrix alloy[9, 24-26]. However, the effect of addition of Ni on the mechanical properties of Zr-Ti 3
ACCEPTED MANUSCRIPT alloys has not been reported. The present investigation mainly reveals the addition of Ni in Zr-Ti binary alloys is effective in the refinement of microstructural and promoting mechanical properties. More than this study will concentrates on the
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microstructure phase compositions, and compressive properties of as-cast Zr-Ti-Ni
2. Materials and Methods
materials
used
include
Zr-Ti
(ZTN0),
Zr-Ti-1wt.%Ni
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The
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alloys.
(ZTN1),
Zr-Ti-3wt.%Ni (ZTN3) and Zr-Ti-5wt.%Ni (ZTN5). The pure Zr (99.9 wt.%), Ti (99.9 wt.%) and Ni ( 99.9 wt.%) were used to prepare the ZTN series alloys. These
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materials were provided by ZhongNuo Advanced Material Technology Co., Ltd. The melted alloys were then flipped at least and re-melted six times using a vacuum arc melting furnace equipped with a water-cooling system under a Ti-gettered argon
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atmosphere to achieve appropriate homogeneity and minimize compositional
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segregation. The weight of four alloy samples was approximately 60g. X-ray fluorescence was used to analyze the composition of the sample and shown in Table 1. For compressive tests, the cylindrical samples with diameter of 5 mm and height
of 10 mm were prepared. The compression tests were conducted on an Instron 5982 testing machine at a strain rate of 5×10-4S-1. The phase composition of the specimens was examined using a conventional X-ray diffraction (XRD) with Cu Kα radiation. Optical microscopy (OM), scanning electron microscopy (SEM) and transmission 4
ACCEPTED MANUSCRIPT electron microscopy (TEM) were used for microstructural analysis. Hardness tests were performed on FM-ARS 9000 type Vickers hardness tester at a load of 200gf for
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10S. The final hardness value is the average of at least 10 effective tests.
Table 1. Nominal chemical composition (and analyzed chemistry) of the current alloys (wt.%). Zr
Ti
Ni
ZTN0
50 (49.97)
50 (50.46)
0
ZTN1
49.5 (49.52)
49.5 (49.50)
1(1.01)
ZTN3
48.5 (48.51)
48.5 (48.52)
3 (3.02)
ZTN5
47.5 (47.5)
47.5 (47.5)
5 (4.98)
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Alloys
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3. Results and discussion
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The XRD patterns of the as-cast alloys are shown in Fig. 1. The as-cast Zr-Ti alloy showed α phase with no other intermetallic compound or phase. This characteristic can be explained by Zr-Ti binary phase diagram[27], those two elements can form infinite solid solutions of hcp structural α phase in room temperature. Fig. 2 indicates that the crystal parameters of α phase decrease with the content of Ni increasing. Because of the small atomic radius of Ni (0.125nm) compared with Zr (0.160nm) and Ti (0.147nm), the addition of Ni results in a decrease of lattice 5
ACCEPTED MANUSCRIPT parameters “a” and “c”, but the axial ratio “c/a” increases. These distortions cause the XRD peaks shift to higher angle when the Ni content increasing. This result means that the Ni addition does lead to the formation of the solid solution with matrix.
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According to Zr-Ni and Ti-Ni binary phase diagram[27], Ni has low solid solubility in Zr-Ti matrix. Thus the C14 Laves-phase arises in the alloys. The C14 can be observed in ZTN5 sample by XRD, as shown in Fig.1, when the accession of Ni reaches to 5
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wt.%. But no peaks of C14 phase were detected in the XRD patterns ZTN1 and ZTN3
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samples because the content of C14 phase is very few with Ni content less than 5 wt.%. In order to further verify that, the TEM bright field images of the microscopic morphology and selected area electron diffraction pattern (SAED) of C14 Laves-phase were obtained and shown in Fig. 3 (a-c). Moreover, the SEM image of
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C14 Laves-phase was also presented in Fig. 3(d) to show the precipitation of C14 phase in the grain boundary. It can be seen that more compounds are produced with Ni content increasing. Similarly, the Ni addition can cause the formation of C14
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Laves-phase which has also been reported in previous literatures [28-30].
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Addition of Ni remarkably affects the α grain size. The OM images of the as-cast Zr-Ti-Ni alloys revealing microstructural features results are given in Fig. 4. The sample of Zr-Ti binary alloy is composed of α-phase completely, with prior-β grain boundaries retained. The β phase convert to α phase is solid phase transformation. The liquid phase transform the β grain take place when the liquid-to-solid transition. And with the temperature is further reduced, the solid phase transition from β to α grain take place. The nucleation and growth of the α phase started near the prior β grain 6
ACCEPTED MANUSCRIPT boundaries[17, 31]. Also, the OM results (Fig. 4) indicate gradual changes in the microstructure with increasing Ni content. TEM and SEM experiments were performed to further observe and analyze the microscopic morphology characteristic
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of the C14 Laves-phase (Fig. 3). The C14 Laves-phase appeared on the grain boundary of the prior-β phase, as shown in Fig. 4(d), which is consistent with the TEM and SEM results. Furthermore, the thickness of the lamellar α phase gradually
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decreases with increasing of Ni content. TEM bright field image and SAED reveal
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that a large number of lamellar α phase appears inside of prior-β grain in the as-cast Zr-Ti-Ni alloy (Fig.5). It also confirms that the thickness of α lamellar is decreased with Ni content increasing from 0 to 5 wt.%. The average α grain size was measured by using Nano Measurer software[32] (Fig. 6). It gradually decreases from 0.183 µm
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to 0.065 µm when Ni content gradually increased from 0 wt.% to 5 wt.%. According to the Zr-Ni and Ti-Ni binary phase diagram, Ni had marginal solubility in Zr-Ti matrix. The nucleation and growth of α grain would be influenced by the increase of
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the Ni concentration. The site of α-phase nucleates and grows near these prior-β
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boundaries or inside the grain. In the case of Ni addition, more C14 Laves-phase particles can be formed, and the site of α-phase nucleates increases. Moreover, the increasing in the number of C14 Laves-phase particles will pin the grain boundaries, resulting in prevent in the further growth of the grain boundaries. A similar result was also observed in Cu3Sn alloys[23]. Fig.7 and Table 2 exhibits the compressive stress-strain curves and compressive test results of the as-cast samples. The compressive properties of the as-cast alloys 7
ACCEPTED MANUSCRIPT were evaluated through room temperature compressive tests. The ultimate compressive strength (UCS) and yield strength (YS) gradually increase and compressive plasticity (ε) gradually decrease when the content of Ni in the alloys
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increase from 0 wt.% to 5 wt.%. As for ZTN3 alloy exhibit better comprehensive mechanical properties. The UCS, YS and ε of the as-cast ZTN3 are 1715 MPa, 1258 MPa and 9.70%, respectively. The microhardness (Hv) of the specimens under
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different Ni content is shown in Fig. 8. The microhardness of as-cast ZTN0 alloy is
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approximately 312 Hv. Nevertheless, the highest microhardness of alloys prepared with 5 wt.% Ni addition can be obtained about 418 Hv. This result, which is consistent with the compressive properties, could be attributed to the amount of Ni
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Table 2. Compressive strength of the as-cast Zr-Ti-Ni alloys.
1598
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UCS (MPa)
ZTN0
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Alloys
ZTN1
ZTN3
ZTN5
1651
1715
1691
YS (MPa)
1117
1159
1258
1648
ε (%)
12.40
10.20
9.70
2.67
The mechanical properties of as-cast Zr-Ti-Ni alloys are greatly influenced by phase composition and microstructure. The stress-strain curve and microhardness results indicate that the addition of Ni in Zr-Ti matrix could contribute to solid 8
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strengthening[33],
grain
refinement[34]
and
the
secondary-phase
strengthening[35-37], thus the better strength of the Zr-Ti-Ni alloys can be prepared. Firstly, lattice distortion is a significant strengthening mechanism of solid solution
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strengthening. The solid solution strengthening of alloys is known to arise from dislocations pinned through interactions with the solute atoms and higher stresses. In this situation, higher stresses are required for dislocation movement through a solute
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field[38-41]. Except that, Fleischer demonstrated that YS is related to the
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concentration of solute atoms[41]. The concentration of solute atoms also plays a very important role in solid solution strengthening. It can be considered as follows: σ∝C2/3, where σ is the YS and C is the concentration of the solute atom. The values of σ as a function of the concentration of the solute atom Ni is shown in Fig. 9. It is obviously
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revealed that solid solution of Ni in the Zr-Ti matrix enhances the YS of the alloys with containing Ni contents from 0 wt.% to 5 wt.%. Secondly, C14 Laves-phase particles on the grain boundaries prevent the growth of α lamellar, resulting in the
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thinner of the α grain size. As we known, the strength of alloys is related to the α grain
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size. Utilizing the Hall-Petch formula (i.e. σ=σ0+kd-1/2, Where σ0 is the yield strength of the matrix alloy, σ is the yield strength (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%). k is the slope of Hall-Petch and d the thickness of the lamellar α phase as shown in Fig. 5). The formula illustrates that the strength of the alloys increases with the grain size decreasing [42, 43]. In the others, the yield strength improvement originates from dislocation pile-up at the grain boundary. The smaller size of α lamellar causes the increase in the number of grain boundary of the unit volume. And more grain 9
ACCEPTED MANUSCRIPT boundaries are act as the obstacle to hinder the motion of dislocation. As we can see from the Table 2 and Fig.6, the yield strength of (Zr-Ti)χNi1-χ alloys increase as lamella thickness d decrease. Above all, the YS of alloys can be improved[18]. In
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addition to the effect of grain refinement strengthen; the second phase particles also play an important role on the increase strength of the alloy. Generally speaking, the hard C14 Laves-phase plays the role of obstruction when dislocations are movement.
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The resistance increases as C14 Laves-phase content from 0 wt.% to 5 wt.%, at the
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same time, greater forces are required to move dislocations. So, it can be concluded that the YS of (Zr-Ti)χNi1-χ alloys could be strengthen by adding Ni element. In Fig. 7 and Table 2, the UCS slightly decreases when the Ni content from 3 wt.% increased to 5 wt.%. The materials fracture before the higher strength due to the bad plasticity of
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alloy.
However, the ε of the as-cast (Zr-Ti)χNi1-χ alloys reduces with the Ni addition. With the Ni content increasing, the poor ε could be caused by the dislocation density
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increasing and the different sizes between the solute atoms Ni and the elements of the
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matrix. The phase segregation of C14 Laves can be detected on the prior-β grain boundaries, which obstructs dislocation migration and reduces plasticity[44]. Chen et al. [9] also reported that the Ni-containing compounds can decrease plasticity. The fracture morphology of the compressive tested specimens of as-cast Zr-Ti-Ni
alloys with different Ni contents is shown in Fig. 10. ZTN0 alloy (Fig. 10(a)) reveals typical characteristic of ductile fracture, the dimples appear on the fracture surface. The fracture morphology of the ZTN1 alloy exhibits different size dimples and 10
ACCEPTED MANUSCRIPT river-shaped pattern (Fig. 10(b)), which is responsible for the fracture behavior from ductile to brittle. Fig. 10(c) shows typical characteristic features of brittle fracture, including a fracture morphology crystal sugar pattern. While the macroscopic crack
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generate on the fracture morphology of ZTN5 (Fig. 10(d)), which would attribute to
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the poor compressive plasticity for ZTN5.
4 Conclusion
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In the present study, the mechanical properties and microstructure of as-cast Zr-Ti-Ni alloys were studied. The following generalized conclusions can be drawn from this study.
The as-cast Zr-Ti-Ni alloys samples are confirmed to consist of the α-phase and
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the C14 Laves-phase after Ni addition.
The thickness of α lamellar gradually decreases with increasing of Ni content in the alloys.
Zr-Ti-3wt.%Ni alloy has a better mechanical properties. The ultimate
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compressive strength, yield strength and compressive plasticity are 1715 MPa, 1258 MPa and 9.70%, respectively.
The fracture behavior could be turned by the addition of Ni content in the as-cast Zr-Ti-Ni alloys.
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ACCEPTED MANUSCRIPT Acknowledgment This research is funded by NSFC (grant 51571174), National Science Foundation for Distinguished Young Scholars for Hebei Province of China (grant E2016203376), and
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Hundred Excellent Innovative Talents Support Program in Hebei Province (grant SLRC2017056). J.Q would like to acknowledge the support from Thai Government Budget (2017), Chulalongkorn University (GB_B_60_114_62_03), Ratchadapisek
Technology
for
Metals
and
Materials
Research
Unit
(GRU
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Coatings
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Sompoch Endowment Fund, Chulalongkorn University, granted to the Surface
60-001-62-001-1), and State Key Laboratory of Metastable Materials Science and Technology, Yanshan University. Reference
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Figure Captions
Fig.1 XRD patterns of the as-cast ZTN0, ZTN1, ZTN3 and ZTN5 alloys. Fig.2 α phase crystal lattice parameter of (Zr-Ti)χNi1-χ alloys.
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Fig.3 Bright field TEM and SEM micrographs of C14 Laves-phase, (a) as-cast ZTN1, (b) as-cast ZTN3, (c) as-cast ZTN5, (d) as-cast ZTN5. Fig.4 Optical micrographs, (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and
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(d) as-cast ZTN5.
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Fig.5 Bright field TEM micrographs of α lamellar of as-cast (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%), alloy, (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and (d) as-cast ZTN5
Fig.6 The thickness of α lamellar distribution of as-cast (Zr-Ti)χNi1-χ (χ=0,1,3 and 5 wt.%), (a) as-cast ZTN0, (b) as-cast ZTN1 (c) as-cast ZTN3 and (d) as-cast ZTN5. Fig.7 Engineering compressive stress-strain at room temperature for the vary amount of add Ni into the Zr-Ti alloys. 18
ACCEPTED MANUSCRIPT Fig.8 Microhardness of ZTN0, ZTN1, ZTN3 and ZTN5. Fig.9 Value of σ as a function of the concentration of the solute atom Ni. Fig.10 Compressive fracture surfaces of as-cast ZTN0, ZTN1, ZTN3 and ZTN5
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alloys at room temperature.
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The effect of Ni addition on the microstructural of Zr-Ti alloys is studied. The mechanism of microstructural evolution is discussed. C14 Laves-phase is formed on the grain boundary. Strength mechanism is proposed from different aspects.
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