In Situ Study on the Nucleation, Growth Evolution, and Motion Behavior of Hydrogen Bubbles at the Liquid/ Solid Bimetal Interface by Using Synchrotron Radiation X-Ray Imaging Technology

doi:10.11900/0412.1961.2022.00062

Acta Metall Sin

2022, Vol. 58

Issue (4): 567-580 DOI: 10.11900/0412.1961.2022.00062

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In Situ Study on the Nucleation, Growth Evolution, and Motion Behavior of Hydrogen Bubbles at the Liquid/ Solid Bimetal Interface by Using Synchrotron Radiation X-Ray Imaging Technology

DING Zongye, HU Qiaodan(

), LU Wenquan, LI Jianguo

School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

Cite this article:

DING Zongye, HU Qiaodan, LU Wenquan, LI Jianguo. In Situ Study on the Nucleation, Growth Evolution, and Motion Behavior of Hydrogen Bubbles at the Liquid/ Solid Bimetal Interface by Using Synchrotron Radiation X-Ray Imaging Technology. Acta Metall Sin, 2022, 58(4): 567-580.

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Abstract

Pore defects at the liquid/solid interface contribute to the interfacial bonding quality. Understanding the formation and growth mechanism of pores can help control their size distribution and eliminate their formation. However, the traditional static-research methods limit the in-depth study of the dynamic evolution behavior of bubbles. The growth, motion behavior, and morphological evolution of hydrogen bubbles at the liquid/solid bimetal interface during heating were characterized in situ, using synchrotron radiation X-ray imaging technology, and the bubbles' nucleation, growth mechanisms, and motion characteristics were investigated. The results show that the nucleation mechanism of hydrogen bubbles contains heterogeneous nucleation and bifilms. Bubble growth is divided into two stages: the inhomogeneous composition and bifilm transformation into hydrogen bubbles. The relationship between the bubbles' mean diameter and heating time conform to the stochastic model. The growth mechanism of bubbles exhibits jump merging and annexation behaviors, accompanied by the morphological transformation from spherical to elliptic and irregular shapes. The motion of the hydrogen bubbles includes upward migration and astatic jumping. The bubbles' growth, hindered by intermetallic compounds (IMCs), has experienced several jumps, attributed to the transformation of bifilms into bubbles, increasing bubble size and deformation, IMC dissolution, and IMC disturbance.

Key words: liquid/solid interface non-equilibrium solidification hydrogen bubble synchrotron radiation intermetallic compounds

Received: 17 February 2022

ZTFLH:

TG245

Fund: National Natural Science Foundation of China(51922068);National Natural Science Foundation of China(51727802);National Natural Science Foundation of China(51904187);China Postdoctoral Science Foundation(2019M661500)

About author: HU Qiaodan, professor, Tel: (021)54744246, E-mail: qdhu@sjtu.edu.cn

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	Zongye DING
	Qiaodan HU
	Wenquan LU
	Jianguo LI

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https://www.ams.org.cn/EN/10.11900/0412.1961.2022.00062 OR https://www.ams.org.cn/EN/Y2022/V58/I4/567

Fig.1 Real-time evolutions of hydrogen bubbles at different stages during heating at the liquid Al/solid Ni interface for growth and evolution of bubbles in the partially inhomogeneous melt (a-i) and growth behavior of hydrogen bubbles in the homogeneous melts (j-o) (Regions I-IV represent the inhomogeneous melting zones, the different colored dotted circles represent different growth behaviors)
(a) 646℃, 245 s (b) 650℃, 246 s (c) 652℃, 247 s
(d) 654℃, 248 s (e) 656℃, 249 s (f) 658℃, 250 s
(g) 660℃, 251 s (h) 662℃, 252 s (i) 664℃, 253 s
(j) 666℃, 254 s (k) 668℃, 255 s (l) 672℃, 257 s
(m) 682℃, 262 s (n) 690℃, 268 s (o) 731℃, 289 s

Fig.2 Magnifications of real-time images of hydrogen bubbles growth in region II (a), region III (b), and region IV (c) of inhomogeneous melts during heating at the liquid Al/solid Ni interface

Fig.3 Relationship between hydrogen bubbles number and heating time (a), mean diameter of groups of hydrogen bubbles versus heating time (b), mean diameter of the groups of hydrogen bubbles in the different regions during the first stage (c) and the second stage (d) (R² indicates mean squared error. The different colored lines in Fig.3d represent different bubbles during the second stage)

Fig.4 Schematic of single bubble growth during heating (C_H is hydrogen mean concentration in the melt, $C H'$ is hydrogen concentration at the bubble/melt interface, r_p is bubble radius, r_e is H diffusion layer radius)

Fig.5 In situ images of Al₃Ni intermetallic compounds (IMCs) dissolution and bubbles growth during heating at the liquid Al/solid Ni interface
(a) 596℃, 201 s (b) 607℃, 211 s (c) 612℃, 216 s
(d) 621℃, 225 s (e) 631℃, 235 s (f) 634℃, 237 s
(g) 646℃, 245 s (h) 660℃, 251 s (i) 678℃, 260 s
(j) 685℃, 264 s (k) 692℃, 269 s (l) 693℃, 270 s
(m) 695℃, 271 s (n) 718℃, 281 s (o) 750℃, 348 s

Fig.6 Relationship between hydrogen bubbles number and heating time (a), mean diameter of groups of hydrogen bubbles versus heating time (b), mean diameter of the different single hydrogen bubble versus heating time (c, d) under the hindrance of IMCs (The different colored lines in Figs.6c and d indicate the different hydrogen bubbles in the sample)

Fig.7 In situ images of bifilms evolution, and growth and jumping of hydrogen bubbles under the hindrance of Al₃Ni IMCs during heating at the liquid Al/solid Ni interface
(a) 600℃, 204 s (b) 605℃, 208 s (c) 610℃, 214 s (d) 613℃, 217 s (e) 614℃, 218 s (f) 615℃, 219 s
(g) 616℃, 220 s (h) 617℃, 221 s (i) 619℃, 223 s (j) 629℃, 233 s (k) 635℃, 238 s (l) 638℃, 240 s
(m) 639℃, 241 s (n) 640℃, 242 s (o) 659℃, 250 s (p) 675℃, 258 s (q) 676℃, 259 s (r) 679℃, 261 s
(s) 685℃, 264 s (t) 686℃, 265 s (u) 707℃, 277 s (v) 708℃, 278 s (w) 735℃, 290 s (x) 750℃, 339 s

Fig.8 In situimages of bifilms evolution, and growth and jumping of hydrogen bubbles during heating
(a) 603℃, 206 s (b) 604℃, 207 s (c) 606℃, 210 s (d) 608℃, 212 s (e) 609℃, 213 s
(f) 610℃, 214 s (g) 611℃, 215 s (h) 612℃, 216 s (i) 613℃, 217 s (j) 614℃, 218 s
(k) 615℃, 219 s (l) 618℃, 222 s (m) 621℃, 225 s (n) 626℃, 230 s (o) 638℃, 240 s

Fig.9 In situ images of growth evolution and jumping of hydrogen bubbles in the transition region at the melt/IMCs interface during heating
(a) 645℃, 244 s (b) 647℃, 246 s (c) 648℃, 247 s (d) 661℃, 252 s (e) 663℃, 254 s (f) 685℃, 264 s
(g) 691℃, 268 s (h) 692℃, 269 s (i) 693℃, 270 s (j) 695℃, 271 s (k) 696℃, 272 s (l) 698℃, 273 s
(m) 700℃, 274 s (n) 702℃, 275 s (o) 716℃, 280 s (p) 718℃, 281 s (q) 720℃, 282 s (r) 750℃, 335 s

Fig.10 Schematics of heterogeneous nucleation of hydrogen bubbles on the concave Al dendrites (a) and concave IMCs (b) at the liquid Al/solid Ni interface

Fig.11 In situ images of migration and coalescence of hydrogen bubbles during the first stage at the liquid Al/solid Ni interface (a), in situ images and schematic diagram of annexation of static hydrogen bubbles during the second stage at the liquid Al/solid Ni interface (b), and in situ images of coalescence of hydrogen bubbles at the liquid Al/solid Ni interface (c, d) ( J₁ and J₃ represents the H diffusion fluxes through the bubble/melt interface of large bubble and small bubble, respectively; J₂ indicates the H diffusion flux between different bubbles with various radius; $r p 1$ and $r p 2$ is the radius of large bubble and small bubble, respectively; $r e 1$ and $r e 2$ is the H diffusion layer radius of large bubble and small bubble, respectively; C_H1 and C_H2 is the H concentration at the diffusion layer/melt interface of large bubble and small bubble, respectively; $C H 1'$ and $C H 2'$ is the H concentration at the bubble/diffusion layer interface of large bubble and small bubble, respectively; d is the diffusion distance between two different bubbles with various radius)

Fig.12 Schematics of hydrogen bubbles jumping with the increasing volume (a) and hydrogen bubbles jumping due to the IMCs dissolution (b) (F—force on the bubble; R₁, R₂—radii of the two ends of the deformed bubble)

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