Optimization Design of a Bulk Metallic Glass Zr55Cu30Al10Ni5 and its Crystallization Behavior

doi:10.11901/1005.3093.2022.090

Chinese Journal of Materials Research

2023, Vol. 37

Issue (4): 281-290 DOI: 10.11901/1005.3093.2022.090

ARTICLES

Current Issue | Archive | Adv Search

Optimization Design of a Bulk Metallic Glass Zr₅₅Cu₃₀Al₁₀Ni₅ and its Crystallization Behavior

ZHU Xuedong¹, ZHANG Shuang¹(

), ZOU Cunlei¹, LIU Lingen², ZHU Zhihao², WAN Peng³, DONG Chuang¹^,²

^1.School of Materials Science and Engineering, Dalian Jiaotong University, Dalian 116028, China
^2.Key Laboratory of Materials Modification by Laser, Ion and Electron Beams of Ministry of Education, Dalian University of Technology, Dalian 116024, China
^3.Foshan Shunde Midea Electric Heating Appliance Manufacturing Co. Ltd., Foshan 528300, China

Cite this article:

ZHU Xuedong, ZHANG Shuang, ZOU Cunlei, LIU Lingen, ZHU Zhihao, WAN Peng, DONG Chuang. Optimization Design of a Bulk Metallic Glass Zr₅₅Cu₃₀Al₁₀Ni₅ and its Crystallization Behavior. Chinese Journal of Materials Research, 2023, 37(4): 281-290.

Download:

HTML

PDF(8920KB)
Export: BibTeX | EndNote (RIS)

Abstract

According to the principle of cluster-plus-glue-atom model, the composition of a novel Zr-Cu-Al-Ni alloy with glass formation ability was designed by taking the alloy Zr₅₅Cu₃₀Al₁₀Ni₅ as reference. In the quaternary Zr-Cu-Al-Ni system, two crystallization phases CuZr₂ and CuZr related with amorphous formation were firstly identified, the local structures of these two clusters can be expressed as [Cu-Zr₈Cu₄] and [Cu-Zr₈Cu₆] respectively; then, by combining these two clusters in equal proportion while coupling with the number of glue atoms 2, 4, or 6, the dual-cluster formulas for total atom number of 30, 32, or 34 respectively may be constructed by means of the dual-cluster model. Furthermore, according to dual- cluster formula of the total number of atoms of 32, a quaternary alloy with composition Zr₁₇Cu₁₀Al₃Ni₂≈Zr_53.1Cu_31.3Al_9.4Ni_6.3was tentatively designed, which is closest to the reference Zr₅₅Cu₃₀Al₁₀Ni₅. The glass formation ability of this alloy was tested experimentally. The results show that its T_rg reaches 0.6 and its crystallization activation energy is 334.138 kJ/mol, which are all slightly higher than that of the reference alloy, indicating that the designed alloy has a higher glass formation ability.

Key words: metallic materials composition optimization cluster-plus-glue-atom model glass formation ability bulk metallic glasses crystallization behavior

Received: 07 February 2022

ZTFLH:

TG139.8

Fund: National Natural Science Foundation of China(52101127);National Natural Science Foundation of China(51901033);Natural Science Foundation of Liaoning Province(2020-BS-208);Natural Science Foundation of Liaoning Province(2020-BS-207);Open Project of Key Laboratory of Materials Modification by Laser, Ion and Electron Beams of Ministry of Education, Dalian University of Technology(KF2006);Shunde District Science and Technology Project(201911220001)

	Service

	E-mail this article
	Add to citation manager
	E-mail Alert
	RSS
	（）
	Articles by authors
	ZHU Xuedong
	ZHANG Shuang
	ZOU Cunlei
	LIU Lingen
	ZHU Zhihao
	WAN Peng
	DONG Chuang

URL:

https://www.cjmr.org/EN/10.11901/1005.3093.2022.090 OR https://www.cjmr.org/EN/Y2023/V37/I4/281

Table 1 Structure information of CuZr₂ phase^[22]

Fig.1 Two kinds of clusters in CuZr₂phase (a) [Cu-Zr₈Cu₄] with Cu atom as the center and (b) [Zr-Cu₄Zr₉] with Zr atom as the center, with the yellow spheres representing Zr atoms and the red ones representing Cu atoms

Phase name CuZr	Structure type ClCs	Pearson symbol cP2	Space group Pm $3 ¯$ m			No.221
a=0.32620(5) nm
Cu	1a	m $3 ¯$ m	x=0	y=0	z=0	Occ.=1
Zr	1b	m $3 ¯$ m	x=1/2	y=1/2	z=1/2	Occ.=1

Table 2 Structure information of CuZr phase^[22]

Fig.2 Two kinds of clusters in CuZr_{phase (a) [Cu-Zr₈Cu₆] with Cu atom as the center and (b) [Zr-Cu₈Zr₆] with Zr atom as the center, with the grey spheres representing Zr atoms and the blue ones representing Cu atoms}

Fig.3 X-ray diffraction spectrogram of 5 mm Zr₁₇Cu₁₀-Al₃Ni₂ BMG

Fig.4 EDS area scan analysis of Zr₁₇Cu₁₀Al₃Ni₂ BMG

Table 3 Composition of glassy matrix in Zr₁₇Cu₁₀Al₃Ni₂after EDS area scan

Fig.5 Microstructure of Zr₁₇Cu₁₀Al₃Ni₂ BMG

Table 4 Composition of a precipitated crystal after EDS

Fig.6 Curves of DSC (a) and DTA curve (b) of the Zr₁₇Cu₁₀Al₃Ni₂ bulk metallic glass at the heating rate of 10 K/min and a constant heating rate

Fig.7 DSC traces of the Zr₁₇Cu₁₀Al₃Ni₂ bulk metallic glass at different heating rates, where the measured heat flow, in arbitrary unit, points downwards, showing heat-absorption reactions

Fig.8 DTA traces of the Zr₁₇Cu₁₀Al₃Ni₂ bulk metallic glass at different heating rates, where the measured heat flow, in arbitrary unit, points upwards, showing heat-release reactions

Fig.9 Kissinger plots of the Zr₁₇Cu₁₀Al₃Ni₂ bulk metallic glass

Table 5 Thermal parameters of Zr₁₇Cu₁₀Al₃Ni₂ BMG at different heating rates

Fig.10 XRD patterns of Zr₁₇Cu₁₀Al₃Ni₂ with complete crystallization after heat treatment for 1 hour at 800 K

Fig.11 EDS area scan analysis of the annealed alloy Zr₁₇Cu₁₀Al₃Ni₂

Fig.12 Microstructure diagram of the annealed Zr₁₇Cu₁₀Al₃Ni₂ BMG，in which 1 and 2 representing CuZr₂ phases, 3 and 4 representing CuZr phases

Table 6 EDS analysis of points in Fig.12 (atomic fraction, %)

1	Wang W H. A brief history of metallic glasses[J]. Physics, 2011, 40: 701
	汪卫华. 金属玻璃研究简史[J]. 物理, 2011, 40: 701
2	Chen H S. Thermodynamic considerations on the formation and stability of metallic glasses[J]. Acta Metall., 1974, 22: 1505 doi: 10.1016/0001-6160(74)90112-6
3	Inoue A, Zhang T. Fabrication of bulk glassy Zr₅₅Al₁₀Ni₅Cu₃₀ alloy of 30 mm in diameter by a suction casting method[J]. Mater. Trans., JIM, 1996, 37: 185
4	Wang H J, Chen S S, Hu Q, et al. The glass-forming ability and die casting performance of Zr-based bulk metallic glasses[J]. Mater. Sci. Technol., 2020, 28(5): 38
	王浩杰, 陈双双, 胡强等. Zr基块体非晶合金玻璃形成能力与压铸成型性能研究[J]. 材料科学与工艺, 2020, 28(5): 38
5	Turnbull D. Under what conditions can a glass be formed?[J]. Contemp. Phys., 1969, 10: 473 doi: 10.1080/00107516908204405
6	Lu Z P, Liu C T. A new glass-forming ability criterion for bulk metallic glasses[J]. Acta Mater., 2002, 50: 3501 doi: 10.1016/S1359-6454(02)00166-0
7	Wu Z F. Thermal analysis kinetics and its application in bulk amorphous alloy[J]. Mater. Rev., 2011, 25(18): 262
	吴志方. 热分析动力学及其在大块非晶合金研究中的应用[J]. 材料导报, 2011, 25(18): 262
8	Gao Y L, Shen J, Sun J F, et al. Crystallization behavior of ZrAlNiCu bulk metallic glass with wide supercooled liquid region[J]. Mater. Lett., 2003, 57: 1894 doi: 10.1016/S0167-577X(02)01096-0
9	Yavari A R, Uriarte J L, Tousimi K, et al. In-situ detection of the onset crystallisation of Zr₅₅Cu₃₀Al₁₀Ni₅ from the bulk glass and the liquid states using synchrotron radiation[J]. Mater. Sci. Forum, 1999, 307: 17 doi: 10.4028/www.scientific.net/MSF.307
10	Zhang Q S, Deng Y F, He L L, et al. Isothermal nanocrystallization of Zr55Al10Ni5-Cu30 bulk amorphous alloy near the glass transition temperature[J]. Acta Metall. Sin., 2003, 39: 301
	张庆生, 邓玉福, 贺连龙等. Zr₅₅Al₁₀Ni₅Cu₃₀块状非晶合金靠近玻璃转变点的等温纳米晶化[J]. 金属学报, 2003, 39: 301
11	De Oliveira M F, Botta F W J, Kaufman M J, et al. Phases formed during crystallization of Zr₅₅Al₁₀Ni₅Cu₃₀ metallic glass containing oxygen[J]. J. Non-Cryst. Solids, 2002, 304: 51 doi: 10.1016/S0022-3093(02)01003-7
12	Hu Q, Lin X, Yang G L, et al. Crystallization behavior of Zr₅₅Al₁₀Ni₅Cu₃₀ amorphous alloys with different morphologies and thermal history conditions[J]. Acta Metall. Sin., 2012, 48: 1467 doi: 10.3724/SP.J.1037.2012.00433
	胡桥, 林鑫, 杨高林等. 不同形态和热历史条件下Zr₅₅Al₁₀Ni₅Cu₃₀非晶合金的晶化行为[J]. 金属学报, 2012, 48: 1467
13	Wu Z F. Effect of differential thermal analysis experimental condition on crystallization behavior of bulk amorphous alloy Zr₅₅Cu₃₀Al₁₀Ni₅ [J]. Hot Work. Technol., 2013, 42(10): 106
	吴志方. 差热分析实验条件对大块非晶合金Zr₅₅Cu₃₀Al₁₀Ni₅晶化行为的影响[J]. 热加工工艺, 2013, 42(10): 106
14	Arias D, Abriata J P. Cu-Zr (copper-zirconium)[J]. J. Phase Equilib., 1990, 11: 452 doi: 10.1007/BF02898260
15	Sakata M, Cowlam N, Davies H A. Chemical short-range order in liquid and amorphous Cu₆₆Ti₃₄ alloys[J]. J. Phys., 1981, 11F: L157
16	Dong C, Wang Q, Qiang J B, et al. From clusters to phase diagrams: composition rules of quasicrystals and bulk metallic glasses[J]. J. Phys., 2007, 40D: R273
17	Dong C, Wang Z J, Zhang S, et al. Review of structural models for the compositional interpretation of metallic glasses[J]. Int. Mater. Rev., 2020, 65: 286 doi: 10.1080/09506608.2019.1638581
18	Wang Z R, Qiang J B, Wang Y M, et al. Composition design procedures of Ti-based bulk metallic glasses using the cluster-plus-glue-atom model[J]. Acta Mater., 2016, 111: 366 doi: 10.1016/j.actamat.2016.03.072
19	Geng Y X, Wang Y M, Qiang J B, et al. Composition design and optimization of Fe-B-Si-Nb bulk amorphous alloys[J]. Acta Metall. Sin., 2016, 52: 1459 doi: 10.11900/0412.1961.2016.00033
	耿遥祥, 王英敏, 羌建兵等. Fe-B-Si-Nb块体非晶合金的成分设计与优化[J]. 金属学报, 2016, 52: 1459 doi: 10.11900/0412.1961.2016.00033
20	Zhang S, Dong D D, Wang Z J, et al. Spherical periodicity as structural homology of crystalline and amorphous states[J]. Sci. China Mater., 2018, 61: 409 doi: 10.1007/s40843-017-9161-4
21	Wang Z J, Dong D D, Zhang S. Characteristics of cluster formulas for binary bulk metallic glasses[J]. J. Alloys Compd., 2016, 654: 340 doi: 10.1016/j.jallcom.2015.08.244
22	Pierre V. Pearson's handbook desk edition[J]. Crystallogr. Data Intermet Phases., 1997, 1: 2
23	Köster U, Herold U. Crystallization of metallic glasses[A]. GüntherodtHJ, BeckH. Glassy Metals I[M]. Berlin Heidelberg: Springer, 1981: 225
24	Kneller E, Khan Y, Gorres U. ChemInform abstract: the alloy system copper-zirconium. Part 1. phase diagram and structural relations[J]. Chem. Informationsdienst, 1986, 17: 43
25	Kalay I, Kramer M J, Napolitano R E. High-accuracy X-ray diffraction analysis of phase evolution sequence during devitrification of Cu₅₀Zr₅₀ metallic glass[J]. Metall. Mater. Trans., 2011, 42A: 1144
26	Ma Y P, Dong D D, Dong C, et al. Composition formulas of binary eutectics[J]. Sci. Rep., 2015, 5: 17880 doi: 10.1038/srep17880 pmid: 26658618
27	Fan C, Takeuchi A, Inoue A. Preparation and mechanical properties of Zr-based bulk nanocrystalline alloys containing compound and amorphous phases[J]. Mater. Trans., JIM, 1999, 40: 42
28	Inoue A. Stabilization of metallic supercooled liquid and bulk amorphous alloys[J]. Acta Mater., 2000, 48: 279 doi: 10.1016/S1359-6454(99)00300-6
29	Inoue A, Zhang T. Fabrication of bulky Zr-based glassy alloys by suction casting into copper mold[J]. Mater. Trans., JIM, 1995, 36: 1184
30	Kawamura Y, Shibata T, Inoue A, et al. Workability of the supercooled liquid in the Zr₆₅Al₁₀Ni₁₀Cu₁₅ bulk metallic glass[J]. Acta Mater., 1998, 46: 253 doi: 10.1016/S1359-6454(97)00235-8
31	Inoue A, Zhang T, Masumoto T. Zr-Al-Ni amorphous alloys with high glass transition temperature and significant supercooled liquid region[J]. Mater. Trans., JIM, 1990, 31: 177
32	Inoue A, Zhang T. Impact fracture energy of bulk amorphous Zr₅₅Al₁₀Cu₃₀Ni₅ alloy[J]. Mater. Trans., JIM, 1996, 37: 1726
33	Lu Z P, Liu C T, Thompson J R, et al. Structural amorphous steels[J]. Phys. Rev. Lett., 2004, 92: 245503 doi: 10.1103/PhysRevLett.92.245503
34	Inoue A, Zhang T, Kim Y H. Synthesis of high strength bulk amorphous Zr-Al-Ni-Cu-Ag alloys with a nanoscale secondary phase[J]. Mater. Trans., JIM, 1997, 38: 749
35	Zhang T, Inoue A. Density, thermal stability and mechanical properties of Zr-Ti-Al-Cu-Ni bulk amorphous alloys with high Al plus Ti concentrations[J]. Mater. Trans., JIM, 1998, 39: 857
36	Kissinger H E. Reaction kinetics in differential thermal analysis[J]. Anal. Chem., 1957, 29: 1702 doi: 10.1021/ac60131a045

[1]	MAO Jianjun, FU Tong, PAN Hucheng, TENG Changqing, ZHANG Wei, XIE Dongsheng, WU Lu. Kr Ions Irradiation Damage Behavior of AlNbMoZrB Refractory High-entropy Alloy[J]. 材料研究学报, 2023, 37(9): 641-648.
[2]	SONG Lifang, YAN Jiahao, ZHANG Diankang, XUE Cheng, XIA Huiyun, NIU Yanhui. Carbon Dioxide Adsorption Capacity of Alkali-metal Cation Dopped MIL125[J]. 材料研究学报, 2023, 37(9): 649-654.
[3]	ZHAO Zhengxiang, LIAO Luhai, XU Fanghong, ZHANG Wei, LI Jingyuan. Hot Deformation Behavior and Microstructue Evolution of Super Austenitic Stainless Steel 24Cr-22Ni-7Mo-0.4N[J]. 材料研究学报, 2023, 37(9): 655-667.
[4]	SHAO Hongmei, CUI Yong, XU Wendi, ZHANG Wei, SHEN Xiaoyi, ZHAI Yuchun. Template-free Hydrothermal Preparation and Adsorption Capacity of Hollow Spherical AlOOH[J]. 材料研究学报, 2023, 37(9): 675-684.
[5]	XING Dingqin, TU Jian, LUO Sen, ZHOU Zhiming. Effect of Different C Contents on Microstructure and Properties of VCoNi Medium-entropy Alloys[J]. 材料研究学报, 2023, 37(9): 685-696.
[6]	OUYANG Kangxin, ZHOU Da, YANG Yufan, ZHANG Lei. Microstructure and Tensile Properties of Mg-Y-Er-Ni Alloy with Long Period Stacking Ordered Phases[J]. 材料研究学报, 2023, 37(9): 697-705.
[7]	XU Lijun, ZHENG Ce, FENG Xiaohui, HUANG Qiuyan, LI Yingju, YANG Yuansheng. Effects of Directional Recrystallization on Microstructure and Superelastic Property of Hot-rolled Cu71Al18Mn11 Alloy[J]. 材料研究学报, 2023, 37(8): 571-580.
[8]	XIONG Shiqi, LIU Enze, TAN Zheng, NING Likui, TONG Jian, ZHENG Zhi, LI Haiying. Effect of Solution Heat Treatment on Microstructure of DZ125L Superalloy with Low Segregation[J]. 材料研究学报, 2023, 37(8): 603-613.
[9]	LIU Jihao, CHI Hongxiao, WU Huibin, MA Dangshen, ZHOU Jian, XU Huixia. Heat Treatment Related Microstructure Evolution and Low Hardness Issue of Spray Forming M3 High Speed Steel[J]. 材料研究学报, 2023, 37(8): 625-632.
[10]	YOU Baodong, ZHU Mingwei, YANG Pengju, HE Jie. Research Progress in Preparation of Porous Metal Materials by Alloy Phase Separation[J]. 材料研究学报, 2023, 37(8): 561-570.
[11]	REN Fuyan, OUYANG Erming. Photocatalytic Degradation of Tetracycline Hydrochloride by g-C₃N₄ Modified Bi₂O₃[J]. 材料研究学报, 2023, 37(8): 633-640.
[12]	WANG Hao, CUI Junjun, ZHAO Mingjiu. Recrystallization and Grain Growth Behavior for Strip and Foil of Ni-based Superalloy GH3536[J]. 材料研究学报, 2023, 37(7): 535-542.
[13]	LIU Mingzhu, FAN Rao, ZHANG Xiaoyu, MA Zeyuan, LIANG Chengyang, CAO Ying, GENG Shitong, LI Ling. Effect of Photoanode Film Thickness of SnO₂ as Scattering Layer on the Photovoltaic Performance of Quantum Dot Dye-sensitized Solar Cells[J]. 材料研究学报, 2023, 37(7): 554-560.
[14]	QIN Heyong, LI Zhentuan, ZHAO Guangpu, ZHANG Wenyun, ZHANG Xiaomin. Effect of Solution Temperature on Mechanical Properties and γ' Phase of GH4742 Superalloy[J]. 材料研究学报, 2023, 37(7): 502-510.
[15]	GUO Fei, ZHENG Chengwu, WANG Pei, LI Dianzhong. Effect of Rare Earth Elements on Austenite-Ferrite Phase Transformation Kinetics of Low Carbon Steels[J]. 材料研究学报, 2023, 37(7): 495-501.

No Suggested Reading articles found!

Viewed

Full text

Abstract

Cited

Shared

Discussed