Scripta Materialia 243 (2024) 115960

Contents lists available at ScienceDirect

Scripta Materialia
journal homepage: www.journals.elsevier.com/scripta-materialia

In-situ localization of damage in a Zn-Al-Mg coating deposited on steel by

continuous hot-dip galvanizing
Houssem Eddine Chaieb a,b,∗ , Vincent Maurel b , Kais Ammar b , Samuel Forest b ,
Alexandre Tanguy c , Eva Héripré d , Franck Nozahic a , Jean-Michel Mataigne e , Joost De Strycker a
a
ArcelorMittal Global R&D Ghent, J.F. Kennedylaan 3, B-9060 Zelzate, Belgium
b
Mines Paris, PSL University, MAT - Centre des Matériaux, CNRS UMR 7633, BP 87 91003 Evry, France
c
CNRS UMR 7649, Laboratoire de Mécanique Des Solides, Ecole Polytechnique, Palaiseau, France
d
Université Paris-Saclay, CentraleSupélec, ENS Paris-Saclay, CNRS, Laboratoire de Mécanique Paris-Saclay, 91190, Gif-sur-Yvette, France
e
ArcelorMittal Global R&D Maizières, Voie Romaine, Maizières lès Metz, France

A R T I C L E I N F O A B S T R A C T

Keywords: Zn-Al-Mg coatings are characterized by a complex microstructure with dendritic and eutectic phases. This
Coating heterogeneous phase distribution contributes to multiple deformation and damage mechanisms. The presence
Mechanical properties of brittle phases promotes crack initiation and propagation. This study reveals a new deformation and damage
Twinning
mechanism of a Zn-Al-Mg coating, where twinning can induce crack initiation in the eutectic region. The
Solidification microstructure
chronology of different events leading to crack initiation and propagation is clearly established by in-situ tensile
Deformation and damage mechanisms
testing in a scanning electron microscope, which helps to establish a detailed characterization of the mechanical
behavior of the coating.

The increasing use of zinc-based coatings is justified by their high The present work provides new insights into the chronology of de-
corrosion resistance as well as their excellent mechanical properties formation and damage events in Zn-Al-Mg coatings. This allows for a
such as wear resistance and adhesion [1,2]. Zinc-aluminum-magnesium better understanding of how cracks are initiated and what can be done
coatings represent a significant part of the production of galvanized to further optimize the microstructure and improve the formability of
coatings, especially in the automotive industry and in the production of the coatings. In particular, a new damage mechanism resulting from
solar panels. They are characterized by the presence of different phases, the interaction between dendrites and eutectic phases is revealed. In-
including brittle phases [3–5]. The latter are preferential sites for crack- deed, a causal interaction between these two phases is observed, which
ing and can significantly affect the structural integrity of the coating. affects the deformation and damage mechanisms of the coating. Special
The mechanical behavior of zinc-based coatings has been studied attention is paid to the contribution of each phase to the crack propa-
in several previous works [2,3,6–9]. The respective influence of com- gation in 3D in order to clarify the crack growth mechanisms through
position, microstructure and crystallographic texture were related to the thickness of the coating.
the formability of the coatings. However, the deformation and damage In this work, an industrial Zn-Al-Mg coating deposited on steel by
mechanisms of Zn-Al-Mg coatings have not been thoroughly investi- continuous hot-dip galvanizing is studied. The steel composition and
gated. Such coatings are characterized by the presence of dendritic and mechanical properties are shown in Table 1 and Table 2 respectively.
eutectic phases, which makes them significantly different from pure The bath composition of the coating is Zn-1.2%Al-1.2%Mg. The mi-
zinc coatings or coatings with low alloying element content (< 0.2 crostructure of the coating is shown in Fig. 1. The coating is composed
wt%). Previous work has focused on the role of the binary eutectic of pro-eutectic zinc dendrites and two eutectic phases: a coarse bi-
phase present in Zn-Al-Mg coatings and its contribution to the forma- nary eutectic Zn/MgZn2 and a thin ternary eutectic Zn/Al/MgZn2 . The
bility of the coating: it was found to be a brittle phase in which most dendritic phase is predominant with an area fraction of about 67% as
cracks preferentially form [3,4,10,11]. determined by surface image analysis. The film thickness is 5 μm.

* Corresponding author at: ArcelorMittal Global R&D Ghent, J.F. Kennedylaan 3, B-9060 Zelzate, Belgium.
E-mail address: [email protected] (H.E. Chaieb).

https://doi.org/10.1016/j.scriptamat.2023.115960
Received 21 September 2023; Received in revised form 18 December 2023; Accepted 26 December 2023
Available online 6 January 2024
1359-6462/© 2024 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
H.E. Chaieb, V. Maurel, K. Ammar et al. Scripta Materialia 243 (2024) 115960

Fig. 1. SEM image showing the microstructure of the Zn-1.2Al-1.2Mg coating in backscattered electrons: Area 1 shows a zinc dendrite, area 2 is the binary eutectic
phase Zn/MgZn2 and area 3 is the ternary eutectic phase Zn/Al/MgZn2 , the sample is prepared by ion polishing.

Fig. 2. EBSD analysis of Zn-1.2Al-1.2Mg coating, Z is normal to the coating surface. (For interpretation of the colors in the figure(s), the reader is referred to the
web version of this article.)

Table 1 Table 2
Chemical composition (wt%) of the steel substrate. Mechanical properties of the steel substrate.

C Mn P S Si Ti Rm - Tensile Strength (MPa) 270 - 330

ReH - Yield Strength (MPa) 170 - 180
≤ 0.12 ≤ 0.6 ≤ 0.1 ≤ 0.045 ≤ 0.5 ≤ 0.3
A - Elongation L0=80 mm (%) 41

The crystallographic texture of the coating is studied using electron the c-axis of the hexagonal cell is perpendicular to the surface of the
backscatter diffraction (EBSD) (Fig. 2). It is recalled that zinc has a coating. However, some grains have different orientations, which can
hexagonal close packed (HCP) structure. The coating is characterized change the mechanical behavior of the coating (Fig. 2b) [10]. An im-
by a strong basal orientation (Fig. 2c), meaning that for most grains portant finding is the epitaxial relationship between the proeutectic

2
H.E. Chaieb, V. Maurel, K. Ammar et al. Scripta Materialia 243 (2024) 115960

Fig. 3. SEM in-situ study of deformation and damage mechanisms in Zn-1.2Al-1.2Mg coating.

zinc dendrites and the eutectic zinc located in their vicinity (Fig. 2b). In increment of global strain. The stress-strain curve corresponding to the
other words, the eutectic zinc has the same orientation as the adjacent coated substrate as well as the strain values where the SEM images were
primary zinc dendrite, which can also affect the behavior of the coating. taken are shown in Fig. 3b. The area of the specimen gauge is 8 × 4
An in situ dog bone tensile specimen was cut from an industrial mm2 with a thickness of 0.8 mm for the substrate (Fig. 3a). Within this
product processed at ArcelorMittal. The surface was prepared using a gauge, a region of interest (ROI) corresponding to 1.5 × 1.5 mm2 was
Gatan PECS II ion polisher. An in-situ SEM tensile test was then per- defined on which gold patterns were deposited by electron beam lithog-
formed up to 15% macroscopic strain. Images were taken for each 1% raphy [12] for further digital image correlation (DIC) analysis (Fig. 4b).

3
H.E. Chaieb, V. Maurel, K. Ammar et al. Scripta Materialia 243 (2024) 115960

Fig. 4. Strain field measurements using DIC (1% of macroscopic strain) showing the relationship between the twinning mechanism and crack formation within the
binary eutectic phase, tensile direction is horizontal.

Fig. 3c details an area where a crack is observed within a den- the coating by drastically reducing the number of grains susceptible to
drite. This crack is located at twin boundaries. In fact, a twin band is twinning and eventually the number of transgranular cracks.
observed at 3% macroscopic strain. The latter grows with increasing To better understand this mechanism, strain fields were calculated
strain and induces microcracking of the binary eutectic phase (inside using the DIC technique (Fig. 4). This is done using the CMV software
MgZn2 ). Starting from 6% macroscopic strain, this microcrack extends [13]. Twinning is observed within a zinc dendrite at early stages of
in the eutectic zinc of the binary eutectic phase and then grows towards strain. This twinning induces a high local level of strain that causes the
the zinc dendrite along the twin boundaries. At higher strain levels this fracture of the brittle MgZn2 phase, which belongs to the binary eutec-
crack propagates and opens. The formation of cracks within the binary tic phase (Fig. 4c). Such a mechanism is often observed in this study
and is thought to be the main cause of cracking in the binary eutectic.
eutectic phase can occur without necessarily being associated the for-
However, it should be noted that some other microcracks are observed
mation of a twin in an adjacent primary dendrite, but the occurrence of
within the binary eutectic phase without being caused by a twin.
such a phenomenon promotes the cracking within this phase. This find-
The mechanism of mutual cracking between pro-eutectic zinc and
ing is well in line with the results reported in previous works [3,4,6]
the binary eutectic phase is unique and is observed for the first time on
where the MgZn2 phase was identified as the most brittle phase and the
coatings. The initiation of cracks at twin boundaries for steel has been
most prone to cracking and where the role of twinning has been identi- discussed in [14], but no previous work has dealt with this mechanism
fied as detrimental for similar coatings with coarse grain structure. The for coatings or established a link between the phases. The specificity
crystallographic orientation of the grains as well as the steel substrate of the mechanism studied in this work is that it shows the influence
condition the cracking behavior of the coating [10,11], but this topic is of each phase on the other phases: the twin initially formed is respon-
beyond the scope of this short paper. However, the results showing the sible for crack initiation within the binary eutectic phase. The same
role of twinning in the formation of cracks within the binary eutectic crack grows and induces crack initiation at the twin boundaries inside
phase and at the twin boundaries suggest that a crystallographic ori- the zinc dendrites. We also recall the fact that the basal orientation is
entation with less basal grains could improve the cracking behavior of dominant in the coating, meaning that most of the grains have an ori-

4
H.E. Chaieb, V. Maurel, K. Ammar et al. Scripta Materialia 243 (2024) 115960

Fig. 5. 3D FIB analysis of Zn-1.2Al-1.2Mg coating.

entation that promotes twinning, making this mechanism very likely to having a higher yield strength compared to primary zinc and ternary
occur. Furthermore, the epitaxial relationship between the pro-eutectic eutectic. The presence of the brittle intermetallic compound MgZn2 is
zinc dendrites and the eutectic zinc justifies the extension of twinning the main cause for such a difference in micro-mechanical properties.
bands within the binary eutectic phase. The strain localization at the interface could also be explained by
Concerning strain localization, it is noteworthy that interfaces be- the difference in topography between the phases. In fact, the primary
tween phases play a key role, Fig. 4. This could be explained by the zinc dendrites occupy a plateau region while the eutectic phases rep-
heterogeneity of the micro-mechanical properties of the phases in- resent a valley. This contrast in topography and height could make the
volved. For example, the primary zinc dendrite shows a very different interfaces a preferential site for strain localization.
behavior compared to the binary eutectic phase. This aspect is well de- A more detailed study of the observed crack is performed using SEM
scribed in a previous work [3] where the binary eutectic was shown to - Focused Ion Beam (SEM-FIB), where the 3D Slice&View technique is
be the most detrimental constituent in terms of micro-ductility, despite used [15] (Fig. 5). To observe the extent of the crack in the coating

5
H.E. Chaieb, V. Maurel, K. Ammar et al. Scripta Materialia 243 (2024) 115960

thickness, several sections are made in an area where this mechanism Acknowledgements
is observed. Fig. 5a shows some of the cross-sections. We observe that
cracks forming within the binary eutectic phase (MgZn2 phase) can This work was carried out in collaboration with several laboratories
reach the steel-coating interface in a discontinuous manner (Fig. 5d). (Centre des Matériaux, LMS X, LMPS, OCAS NV). The FIB-SEM work
Zinc dendrites, eutectic zinc, and the ternary eutectic act as barriers was carried out using the facilities available at the LMPS laboratory
to these cracks (Fig. 5b). As for the crack growth at the twin bound- within the MATMECA consortium, supported by the ANR under con-
aries and initially induced by the fracture of the binary eutectic phase, tract number ANR-10-EQPX-37. The contribution of Fabrice Gaslain,
it remains superficial (Fig. 5c): this type of cracks is associated with a Gwyneth Vandeborne and Dimitri Monteyne is highly appreciated. Spe-
slight perturbation of the local roughness of the coating without further cial thanks are due to Alain Koster who supervised some of the mechan-
propagation towards the steel substrate. ical tests related to this work.
This work complements the recently published works that have This research work was performed as a part of the PhD “Multi-
studied the mechanical behavior of Zn-Al-Mg coatings. It is clear that scale approach of mechanical behavior of hot-dip Zn-Al-Mg coatings
twinning plays a crucial role in conditioning the deformation and the deposited on steel sheet”, performed at Centre des Matériaux of MINES
damage mechanisms of such coatings. This was highlighted in [6] where Paris and was funded by ArcelorMittal Global R&D, OCAS N.V.
the effect of the grain size of a Zn-Al-Mg coating on its formability was
discussed. It was shown that a coating with a coarse microstructure References
would have a decrease in its mechanical performance and this is mainly
due to the presence of large transgranular cracks caused by twinning. [1] E. De Bruycker, B. De Cooman, M. Meyer, Experimental study and microstructure
simulation of Zn-Al-Mg coatings, Rev. Métall. (Impr.) 102 (2005) 543–550.
This aligns with the findings of the current work. This also gives an indi-
[2] R. Parisot, S. Forest, A. Pineau, F. Grillon, X. Demonet, J.M. Mataigne, Deformation
cation of a potential improvement path. In fact, a coating with a more and damage mechanisms of zinc coatings on hot-dip galvanized steel sheets: part I.
refined microstructure should perform better because the presence of Deformation modes, Metall. Mater. Trans. A 35 (2004) 797–811.
more grains leads to the presence of more grain boundaries that act as [3] M. Ahmadi, B. Salgın, B.J. Kooi, Y. Pei, Genesis and mechanism of microstructural
scale deformation and cracking in ZnAlMg coatings, Mater. Des. 186 (2020) 108364.
barriers to crack propagation. In addition, limiting the grain size should
[4] M. Ahmadi, B. Salgın, M. Ahmadi, B.J. Kooi, Y. Pei, Unraveling dislocation mediated
limit the occurrence of twinning and the size of the twins, resulting plasticity and strengthening in crack-resistant ZnAlMg coatings, Int. J. Plast. 144
in an optimized mechanical robustness. Another work [10] highlighted (2021) 103041.
the role of the crystallographic texture where a strong basal orienta- [5] F. Nozahic, M. Gauvin, D. Rosseel, K. Van den Bergh, J. De Strycker, D. Mercier,
tion was found to be a factor in improving formability. This contradicts J.M. Mataigne, Quantitative mapping of nanoscale mechanical properties of Zn-Al
and Zn-Al-Mg coatings on steel sheet by nanoindentation, in: Proceedings of the
with the previous statements since a strong basal orientation leads to
12th International Conference on Zinc and Zinc Alloy Coated Steel Sheet, Galvatech
a higher twinning rate. Therefore, it has become clear that there is a 2021, 2021.
certain trade-off between the grain size and the crystallographic tex- [6] M. Ahmadi, B. Salgın, B.J. Kooi, Y. Pei, The effect of grain refinement on the defor-
ture that needs to be defined: the grain size should be optimized first mation and cracking resistance in Zn–Al–Mg coatings, Mater. Sci. Eng. A 840 (2022)
then the actions towards having a fiber-like basal orientation should be 142995.
[7] J. Legendre, R. Créac’hcadec, A. Tanguy, S. Hallais, J.H. Schmitt, E. Héripré, F.
undertaken. Gilbert, D. Jacquet, J.M. Mataigne, A unique combination of in-situ and multi-scale
In conclusion, we have investigated a new deformation and dam- methodologies to analyze damage mechanisms of temper rolled zinc coating, Mater.
age mechanism for the Zn-1.2Al-1.2Mg coating where a mutual causal Sci. Eng. A 763 (2019) 138156.
effect between the pro-eutectic zinc dendrites and the binary eutectic [8] G.M. Song, W.G. Sloof, Y.T. Pei, J.Th.M. De Hosson, Interface fracture behavior of
zinc coatings on steel: experiments and finite element calculations, Surf. Coat. Tech-
phase is observed. Twinning causes high local strain levels leading to
nol. 201 (7) (2006) 4311–4316, Proceedings of the 33rd International Conference
crack initiation within the brittle MgZn2 phase. Such cracks can grow on Metallurgical Coatings and Thin Films.
through the zinc dendrite along the twin boundaries. Some other mi- [9] Y.B. Park, I.G. Kim, S.G. Kim, W.T. Kim, T.C. Kim, M.S. Oh, J.S. Kim, Orientation
crocracks are observed within the binary eutectic phase. The eutectic dependence of cracking in hot-dip Zn-Al-Mg alloy coatings on a sheet steel, Metall.
zinc and the ternary eutectic phase were observed to act as barriers Mater. Trans. A 48 (3) (Mar 2017) 1013–1020.
[10] M. Ahmadi, B. Salgın, B.J. Kooi, Y. Pei, Outstanding cracking resistance in Mg-
to crack propagation. The MgZn2 is the most detrimental phase in the alloyed zinc coatings achieved via crystallographic texture control, Scr. Mater. 210
coating. These observations give an idea of what could be done to im- (2022) 114453.
prove the formability of the coating: reducing the volume fraction of [11] M. Ahmadi, B. Salgın, B.J. Kooi, Y. Pei, Cracking behavior and formability of Zn-Al-
the binary eutectic phase is essential for better formability. The 3D ob- Mg coatings: understanding the influence of steel substrates, Mater. Des. 212 (2021)
110215.
servations showed that the coating has an overall good adhesion to the
[12] L. Allais, M. Bornert, T. Bretheau, D. Caldemaison, Experimental characterization of
steel substrate. Some cracks can reach the steel-coating interface in a the local strain field in a heterogeneous elastoplastic material, Acta Metall. Mater.
discontinuous manner and form mainly within the MgZn2 phase. 42 (11) (1994) 3865–3880.
This work is part of a more comprehensive analysis of the mechan- [13] M. Bornert, F. Valès, H. Gharbi, D. Nguyen Minh, Multiscale full-field strain mea-
ical behavior of hot-dip Zn-Al-Mg coatings that will be presented in surements for micromechanical investigations of the hydromechanical behaviour of
clayey rocks, Strain 46 (1) (2010) 33–46.
future work. [14] C. Blochwitz, W. Tirschler, Twin boundaries as crack nucleation sites, Cryst. Res.
Technol. 40 (1–2) (2005) 32–41.
Declaration of competing interest [15] T. Truglas, J. Duchoslav, C. Riener, M. Arndt, C. Commenda, D. Stifter, G. Angeli,
H. Groiss, Correlative characterization of Zn-Al-Mg coatings by electron microscopy
and FIB tomography, Mater. Charact. 166 (2020) 110407.
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.