Direct alloying of immiscible molybdenum-silver system and its thermodynamic mechanism

doi:10.1016/j.jmst.2020.04.083

Abstract

Abstract:

Direct alloying is difficult to be realized in an immiscible Mo-Ag system with a positive formation heat due to the absence of thermodynamic driving force at equilibrium. In this work, a direct alloying method is developed to realize the direct alloying between Mo and Ag and construct Mo-Ag interface. The direct alloying method was mainly carried out through a direct diffusion bonding for Mo and Ag rods at a temperature close to the melting point of Ag (T_mAg). Then the microstructure and phase constitution of the as-constructed Mo-Ag interface are characterized. The results show that Mo-Ag metallurgical bonding interface has been constructed successfully, indicating that a direct alloying in the immiscible Mo-Ag system has been realized. Additionally, mechanical tests are carried out for the Mo-Ag joints prepared through the direct alloying method. The test results show that the average maximum tensile strength of the joints is about 107 MPa. The effect of alloying parameters on the tensile strength is also discussed, which shows that there is an effective temperature range for the direct alloying between Mo and Ag. Lastly, an improved thermodynamic model that considers the formation of Mo-Ag crystalline and amorphous phase is presented to reveal the thermodynamic mechanism of the direct alloying. Combining the calculation and differential scanning calorimetry (DSC) tests results, the Gibbs energy diagram for the direct alloying is obtained. It is confirmed that the co-release of storage energy and surface energy can serve as the thermodynamic driving force to overcome the effect of positive formation heat and lead to direct alloying for Mo-Ag systems.

Key words: Direct alloying, Immiscible Mo-Ag system, Metallurgical bonding interface, Thermodynamic driving force, Joints

Jinlong Du, Cai Li, Zumin Wang, Yuan Huang. Direct alloying of immiscible molybdenum-silver system and its thermodynamic mechanism[J]. J. Mater. Sci. Technol., 2021, 65: 18-28.

Figures/Tables 11

Fig. 1. Schematic diagram of temperature varying with time during the direct alloying carried out through a direct diffusion bonding for Mo and Ag rods.

Fig. 2. SEM micrographs of powder particles (a) Ag and (b) Mo.

Table 1 Parameters used in thermodynamic calculation of Mo-Ag system [27].

Parameters	${{V}^{2/3}}$(cm²)	$n_{ws}^{1/3}$ ((d.u.)^1/3)	ϕ (V)	γ	E (GPa)	K (GPa)	G (GPa)	${{S}^{f}}$ (10⁵ m²)	${{\gamma }^{S,0}}$(mJ/m²)	ρ (g/cm³)	M (g/mol)	T^m (K)
Mo	4.45	1.77	4.65	0.324	330	313	125	1.67	3000	10.20	95.94	2893
Ag	4.72	1.36	4.35	0.38	82	114	30	2.03	1250	10.49	107.87	1235

Fig. 3. Interfacial microstructure characterization results of the of Mo-Ag joint prepared at 950 °C for 180 min under 100 MPa: (a) the high-angle annular dark-field (HAADF) image of Mo-Ag interface, (b) and (c) element mapping of Mo and Ag, respectively; (d) HRTEM images of as-constructed Mo-Ag interface and (e) the corresponding SAED pattern.

Fig. 4. Microstructure characterization results of the Mo50Ag50 sintered powder materials: (a) and (c) HRTEM images of the powders milled for 40 h and 60 h, (b) and (d) the corresponding SAED pattern, respectively.

Fig. 5. The effect of (a) bonding temperature with 180 min and 100 MPa, (b) bonding time with 950 °C and 100 MPa and (c) bonding pressure with 950 °C and 180 min on the tensile strength of the Mo-Ag joints.

Fig. 6. (a) SEM image of the tensile fracture surface of the Mo-Ag joint prepared at 950 °C for 180 min and (b) EDS results of the region marked with a white rectangle in (a).

Fig. 7. DSC test curves of the original and pre-annealed Ag rods (a) and Mo rods (b).

Fig. 8. DSC test curves of Mo50Ag50 powder mixtures. There are two kinds of test specimens: one is the Mo50Ag50 powder mixture that is just milled for 60 h, the other is the Mo50Ag50 powder mixture that is milled for 60 h firstly and then annealed at 960 °C for 3 h.

Fig. 9. Gibbs energy diagram for the direct alloying in immiscible Mo-Ag system.

Fig. 10. The SEM image of the Mo-Ag powder mixture that has been milled for 60 h.

References 56

[1]	F. Findik, H. Uzun, Mater. Des. 24 (2003) 489-492. DOI URL
[2]	Y. Huang, D.Y. Kong, F. He, Y.L. Wang, W.X. Liu, Acta Metall. Sin. 48 (2012) 1253-1259. DOI URL
[3]	M. Madej, Arch. Metall. Mater. 57 (2012) 605-612.
[4]	S. Packirisamy, D. Schwam, M.H. Litt, J. Mater. Sci. 30 (1995) 308-320. DOI URL
[5]	M.R. Reddy, J. Mater. Sci. 30 (1995) 281-307. DOI URL
[6]	J.L. Du, X.Y. Chen, X.G. Jia, Y. Huang, Z.M. Wang, Y.C. Liu, Mater. Sci. Eng. A 743(2019) 675-683. DOI URL
[7]	I.L. Harris, A.R. Chambers, G.T. Roberts, Mater. Lett. 31 (1997) 321-328. DOI URL
[8]	P. Kannan, K. Balamurugan, K. Thirunavukkarasu, Int. J. Adv. Manuf. Tech. 81 (2015) 1743-1756. DOI URL
[9]	F.C. Nix, D. Macnair, Phys. Rev. B 61 (1942) 74-78. DOI URL
[10]	E. Ma, Prog. Mater. Sci. 50 (2005) 413-509. DOI URL
[11]	G. D’Accolti, G. Beltrame, E. Ferrando, L. Brambilla, R. Contini, L. Vallini, R. Mugnuolo, C. Signorini, H. Fiebrich, A. Caon, ESA Bull. 502 (2002) 445.
[12]	F.T.N. Vüllers, R. Spolenak, Acta Mater. 99 (2015) 213-227. DOI URL
[13]	K. Sarakinos, G. Greczynski, V. Elofsson, D. Magnfält, H. Högberg, B. Alling, J. Appl. Phys. 119 (2016) 379.
[14]	V. Elofsson, G. Almyras, B. Lü, R. Boyd, K. Sarakinos, Acta Mater. 110 (2016) 114-121. DOI URL
[15]	R. Banerjee, A. Puthucode, S. Bose, P. Ayyub, Appl. Phys. Lett. 90 (2) (2007), 021904. DOI URL
[16]	T.L. Wang, J.H. Li, K.P. Tai, B.X. Liu, Scr. Mater. 57 (2007) 157-160. DOI URL
[17]	X. Bai, T.L. Wang, N. Ding, J.H. Li, B.X. Liu, J. Appl. Phys. 108 (2010) 7069.
[18]	T.L. Wang, J.H. Li, K.P. Tai, B.X. Liu, Scr. Mater. 57 (2007) 157-160. DOI URL
[19]	N. Al-Aqeeli, M.A. Hussein, C. Suryanarayana, Adv. Powder Technol. 26 (2015) 385-391. DOI URL
[20]	B.C. Hornbuckle, T. Rojhirunsakool, M. Rajagopalan, T. Alam, G.P. Purja Pun, R. Banerjee, K.N. Solanki, Y. Mishin, L.J. Kecskes, K.A. Darling, JOM 67 (2015) 2802-2809.
[21]	R. Lei, M.P. Wang, H.P. Wang, S.Q. Xu, Mater. Charact. 118 (2016) 324-331.
[22]	J.Z. Jiang, C. Gente, R. Bormann, Mater. Sci. Eng. A 242 (1998) 268-277. DOI URL
[23]	N. Al-Aqeeli, M. Hussein, C. Suryanarayana, Adv. Powder Technol. 26 (2015) 385-391. DOI URL
[24]	J.L. Du, Y. Huang, J.W. Liu, Y.C. Liu, Z.M. Wang, Mater. Des. 170 (2019), 107699. DOI URL
[25]	L.T. Li, J. Zhang, X.C. Pan, Y. Huang, Z.M. Wang, Y.C. Liu, RSC Adv. 7 (2017) 53763-53769. DOI URL
[26]	H. Li, C. Wu, Shanghai Metals 33 (2011) 1-5.
[27]	F.R. De Boer, R. Boom, W.C.M. Mattens, A.R. Miedema, A.K. Niessen, Cohesion in Metals: Transition Metal Alloys, North-Holland, Amsterdam, 1989.
[28]	L. Vitos, A.V. Ruban, H.L. Skriver, J. Kollár, Surf. Sci. 411 (1998) 186-202. DOI URL
[29]	J. Zhang, Y. Huang, Y.C. Liu, Z.M. Wang, Mater. Des. 137 (2018) 473-480. DOI URL
[30]	X.C. Pan, J. Zhang, Y. Huang, Y.C. Liu, J. Alloys Compd. 723 (2017) 1053-1061. DOI URL
[31]	R.F. Zhang, Y.X. Shen, H.F. Yan, B.X. Liu, J. Phys. Chem. B 109 (2005) 4391-4397. DOI URL PMID
[32]	B.X. Liu, W.S. Lai, Z.J. Zhang, Adv. Phys. 50 (2001) 367-429. DOI URL
[33]	K.P. Tai, X.D. Dai, Y.X. Shen, B.X. Liu, J. Phys. Chem. B 110 (2006) 595-606. DOI URL PMID
[34]	J. Zhang, Y. Huang, Z.M. Wang, Y.C. Liu, J. Alloys Compd. 774 (2019) 939-947. DOI URL
[35]	A.R. Miedema, A.K. Niessen, T. Calphad 7 (1983) 27-36.
[36]	J.M. López, J.A. Alonso, Z. Naturforsch. A 40 (1985) 1199-1205. DOI URL
[37]	S. Sheibani, S. Heshmati-Manesh, A. Ataie, J. Alloys Compd. 495 (2010) 59-62. DOI URL
[38]	Z.J. Zhang, O. Jin, B.X. Liu, Phys. Rev. B 51 (1995) 8076-8085. DOI URL
[39]	A.K. Niessen, A.R. Miedema, F.R. de Boer, R. Boom, Phys. B+C 151 (1988) 401-432.
[40]	C.Q. Sun, Prog. Mater. Sci. 54 (2009) 179-307. DOI URL
[41]	M. Methfessel, D. Hennig, M. Scheffler, Phys. Rev. B 46 (1992) 4816-4829. DOI URL
[42]	A. Bachmaier, M. Kerber, D. Setman, R. Pippan, Acta Mater. 60 (2012) 860-871. DOI URL
[43]	B.Y. Tsaur, J.W. Mayer, Appl. Phys. Lett. 37 (1980) 389-392. DOI URL
[44]	D. Dumchenko, C. Gherman, L. Kulyuk, E. Fortin, E. Bucher, Thin Solid Films 495 (2006) 82-85. DOI URL
[45]	I.M. Khan, H.Y. Kim, T. Nam, S. Miyazaki, J. Alloys Compd. 577 (2013) S383-S387. DOI URL
[46]	K.S. Suresh, A.D. Rollett, S. Suwas, Metall. Mater. Trans. A 44 (8) (2013) 3866-3881. DOI URL
[47]	P. Gerber, J. Tarasiuk, T. Chauveau, B. Bacroix, Acta Mater. 51 (2003) 6359-6371. DOI URL
[48]	M. Spanl, A. Korner, W. Pfeiler, W. Püschla, Scr. Mater. 41 (1999) 505-510. DOI URL
[49]	K.S. Vecchio, R.W. Hertzberg, J. Mater. Sci. 23 (1988) 2220-2224. DOI URL
[50]	F. Wang, J. Liu, J.M. Zhang, M. Xie, L.I. Aikun, S. Wang, Precious Met. 39 (2018) 43-49.
[51]	L. Kator, P. Nyulas, Strength Mater. 3 (1971) 28-31. DOI URL
[52]	S. Kobayashi, S. Zaefferer, A. Schneider, D. Raabe, G. Frommeyer, Mater. Sci.Forum 467-470 (2004) 153-158.
[53]	X. He, S.H. Liang, J.H. Li, B.X. Liu, Phys. Rev. B 75 (2007), 045431. DOI URL
[54]	R.F. Zhang, L.T. Kong, H.R. Gong, B.X. Liu, J. Phys.: Condens. Matter 16 (2004) 5251. DOI URL
[55]	X.D. Dai, J.H. Li, H.B. Guo, B.X. Liu, J. Appl. Phys. 101 (2007), 063512. DOI URL
[56]	X. Bai, T.L. Wang, N. Ding, J.H. Li, Bx Liu, J. Appl. Phys. 108 (2010), 073534. 28