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DOI: 10.1039/c8ta00405f
rsc.li/materials-a
Large sized Fe-based bulk metallic glasses (BMGs) and BMG/stainless while the outstanding characteristics of Fe-based BMGs make
steel (SS) composites with excellent mechanical properties were their application as structural materials highly desirable, this
successfully fabricated using a thermal spray three-dimensional (3D) application is at present critically limited. First, the achievable
printing (TS3DP) technique. The 3D-printed BMG and BMGC (rein- dimensions of fabricated components are small. Although
forced with 50% SS powder) parts exhibited high fracture strength (2 some centimeter Fe-based BMGs have been reported previ-
GPa) and fairly good fracture toughness (13–21 MPa m1/2, which is ously,9 they are usually processed under ideal fabrication
200–400% greater than that of the as-cast BMG of the same conditions. If using low-purity raw materials or under industrial
composition). The enhanced fracture toughness originates from the processing conditions, the critical casting dimension of BMGs
intrinsically layered structure of the 3D-printed BMG components, would be dramatically decreased.10 Secondly, most of the Fe-
which caused crack deflection and thus the increase of energy dissi- based BMGs demonstrate little plasticity and low toughness
pation during crack propagation. The TS3DP technique developed in (less than 5 MPa m1/2 for sizes larger than 3 mm diameter) at
this work opens up a new avenue for the production of BMGs and room temperature.8,11,12 This intrinsic brittleness forbids the use
BMG composites of theoretically limitless size, and facilitates their of Fe-based BMGs in practical applications as structural
application as structural and functional materials. materials.
In 2013, a three-dimensional (3D) printing technique (also
known as additive manufacturing) was rst utilized by Pauly
et al.13 to fabricate 3D Fe-based BMG components. Here, the
1. Introduction glassy powder was employed as the starting material which was
melted by laser irradiation, and built up layer by layer into a 3D-
Bulk metallic glasses (BMGs) lack a crystalline lattice, which BMG component. However, the fabrication of dense, crack-free
deters the formation of large-scale defects such as grain and fully amorphous Fe-based BMG components remains great
boundaries and dislocations, and generally imparts superior challenge by using conventional laser 3D printing techniques
strength and greater elasticity to these materials compared to due to the contradiction between requirements of a high cool-
conventional crystalline metals.1–6 In particular, the ing rate for glass formation and a slow solidication process for
outstanding characteristics of Fe-based BMG systems, such as ensuring a crack-free structure.14 Herein, we present an alter-
ultrahigh yield strength (3.0–4.5 GPa), excellent corrosion native 3D-printing-compatible approach, denoted as thermal
resistance and low raw material cost, have attracted consider- spray 3D printing (TS3DP), to manufacture crack-free Fe-based
able attention for their potentially widespread applications BMG and BMG composite (BMGC) structures of theoretically
ranging from surface coatings to magnetic devices.7,8 However, unlimited dimensions using a high velocity oxygen fuel (HVOF)
system. It not only breaks through the size limitation but also
a
School of Materials Science and Engineering, State Key Lab for Materials Processing creates BMG and BMGC components exhibiting high strength
and Die & Mould Technology, Huazhong University of Science and Technology,
and enhanced toughness compared with the as-cast BMGs. As
Wuhan 430074, China. E-mail: lliu2000@mail.hust.edu.cn
b
Laboratory for Corrosion and Protection, Institute of Metal Research, Chinese
such, the proposed TS3DP technique shows considerable
Academy of Sciences, Shenyang 110016, China promise for the application of BMGs and BMGCs as structural
c
Department of Physics and Astronomy, University of North Carolina at Chapel Hill, and/or functional materials.
Chapel Hill, NC 27599-3255, USA The principle of the proposed TS3DP technique is sche-
† Electronic supplementary information (ESI) available. See DOI: matically illustrated in Fig. 1a, where the glassy powder was
10.1039/c8ta00405f
brought into a semi-molten state when injected into an ignited
‡ These authors contributed equally to this work.
6800 | J. Mater. Chem. A, 2018, 6, 6800–6805 This journal is © The Royal Society of Chemistry 2018
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This journal is © The Royal Society of Chemistry 2018 J. Mater. Chem. A, 2018, 6, 6800–6805 | 6801
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6802 | J. Mater. Chem. A, 2018, 6, 6800–6805 This journal is © The Royal Society of Chemistry 2018
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Fig. 3 (a) The representative stress–strain curves of as-cast BMG, TS3DP-BMG and TS3DP-BMGC samples under uniaxial compression. The
insets present images of the fractured samples after compression failure, wherein the as-cast BMG sample suffered catastrophic fragmentation,
while the TS3DP-BMGC underwent standard shear fracture. (b) Force-displacement curves for notched samples under 3-point bending. The
inset presents an image of the TS3DP-BMGC sample after failure. (c) The fracture toughness (KJ) of the samples calculated on the basis of the
ATSM standard.
fractured into fragments, as observed for the as-cast BMG, BMG and 21 MPa m1/2 for the TS3DP-BMGC, which are 200–
which is indicative of an enhanced toughness. The most 400% greater than that of the as-cast BMG. It is expected that the
intriguing nding is that the TS3DP-BMGC sample reinforced toughness of the TS3DP-BMGCs can be further enhanced via
with 50% SS exhibited a high strength of 1.85 GPa and an modication of the reinforcements employed in terms of both
appreciable plastic strain of around 2%. This composite dis- composition and component fractions. This is an important
played a fracture behavior very similar to so-called “ductile” Zr- advantage of the TS3DP technique developed in this work.
based BMG materials, i.e., shear fracture with a shear angle of To further understand the toughening mechanism of the
41 (see the inset in Fig. 3a). These results indicate that, TS3DP-BMG and TS3DP-BMGC materials, the fracture surfaces
compared to the TS3DP-BMG, the TS3DP-BMGC sample of the samples were further characterized by scanning electron
demonstrated fairly good toughness. microscopy (SEM) and laser scanning confocal microscopy, and
The fracture toughness of the three different types of samples compared to the fracture surface of the as-cast BMG material.
was then measured via single-edge notched beam (SENB) testing, The results are shown in Fig. 4a–f. It can be seen that the
and the corresponding force–displacement curves are plotted in fracture surface of the as-cast BMG sample exhibited a very
Fig. 3b. As expected, the as-cast BMG exhibited a purely elastic smooth morphology with a surface roughness (Ra) of less than 4
response prior to catastrophic failure, which is a typical charac- mm due to catastrophic fracture with an ultrafast crack propa-
teristic of extremely brittle materials. In contrast, the TS3DP-BMG gation velocity, which coincides with previous observations
and TS3DP-BMGC samples exhibited remarkably higher exural regarding extremely brittle Fe-based BMGs.11 The fracture
force and noticeable strain-to-failure behavior. The inset in surface thus exhibits no indication whatsoever of crack deec-
Fig. 3b shows an image of the TS3DP-BMGC sample aer failure, tion. In contrast, both TS3DP-BMG and TS3DP-BMGC samples
which indicated that the TS3DP-BMGC sample was not fully exhibit a step-shaped morphology aer fracture with Ra values
broken aer being exposed to a displacement of 1.8 mm (corre- of 41 mm and 82 mm, respectively, demonstrating that
sponding to a strain of 1.5%). According to the ASTM standard,22 substantial crack deection occurred during crack propagation
the J-integral fracture toughness KJ can be calculated by using the in the two samples as shown in Fig. 4b, c, e, f. The relationship
following equations: between the fracture toughness and the reduced roughness (Ra/
1:9A R0, where R0 is the roughness value of the fracture surface for
J¼ (1) the as-cast BMG) is plotted in Fig. 4g, showing that the fracture
BðW aÞ
toughness increases with increasing fracture surface roughness.
0:5 Because the roughness of the fracture surface is closely related
JE
KJ ¼ (2) to the pathway of crack propagation, larger roughness indicates
1 v2
larger deection (or twisting) and a longer trajectory during
where J is the fracture energy, E is the Young's modulus, A is the crack propagation, leading to an increased energy dissipation
total area under the force–displacement curves as shown in on the basis of the fact that the energy dissipation for crack
Fig. 3b, Poisson's ratio n was 0.3 for all samples, and a thickness B propagation is proportional to the crack length.25
¼ 1.5 mm, width W ¼ 3 mm and notch depth a ¼ 750 mm was To quantitatively assess the contribution of crack deection
uniformly employed in this work. Based on the obtained data, KJ to toughness, we further calculated the fracture toughness of
for the three samples is plotted in Fig. 3c. For the as-cast BMG, KJ the three different samples according to the crack-deection
is 5.1 MPa m1/2, which is very small and similar to previously and crack-twisting mechanics proposed by Kotoul et al.26 (see
published results for brittle Fe-based BMG materials prepared by details in the ESI†), and the results are also shown in Fig. 4g.
casting.23,24 In contrast, KJ is about 13 MPa m1/2 for the TS3DP- Interestingly, the calculated toughness of the three samples
This journal is © The Royal Society of Chemistry 2018 J. Mater. Chem. A, 2018, 6, 6800–6805 | 6803
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6804 | J. Mater. Chem. A, 2018, 6, 6800–6805 This journal is © The Royal Society of Chemistry 2018
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masks used. At present, the resolution for our TS3DP technique 5 E. Ma and J. Ding, Mater. Today, 2016, 19, 568–579.
can reach around 1 mm, which is still larger compared to the 6 D. C. Hofmann, L. M. Andersen, J. Kolodziejska,
laser 3D printing methods, e.g., the beam size for selective laser S. N. Roberts, J. P. Borgonia, W. L. Johnson, K. S. Vecchio
melting and laser foil printing is only 80 mm and 430 mm,20 and A. Kennett, Adv. Eng. Mater., 2017, 19, 1600541.
respectively. The resolution of the TS3DP technique can be 7 Z. P. Lu, C. T. Liu, J. R. Thompson and W. D. Porter, Phys.
Published on 20 March 2018. Downloaded by Huazhong University of Science & Technology on 25/04/2018 02:55:07.
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employed as starting materials in the TS3DP process, it is easy 18 J. W. Qiao, H. L. Jia and P. K. Liaw, Mater. Sci. Eng., R, 2016,
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Conflicts of interest 22 E08 Committee, E1820–11e2 standard test method for
measurement of fracture toughness, ASTM International,
There are no conicts to declare. West Conshohocken, PA, 2011.
23 P. A. Hess, S. J. Poon, G. J. Shiet and R. H. Dauskardt, J.
Acknowledgements Mater. Res., 2005, 20, 783.
24 J. H. Yao, J. Q. Wang and Y. Li, Appl. Phys. Lett., 2008, 92,
This work was nancially supported by the National Natural 251906.
Science Foundation of China (Grant No. 51531003 and 25 B. A. Sun and W. H. Wang, Prog. Mater. Sci., 2015, 74, 211–
51471074) and National Program on Key Basic Research Project 307.
(973 Program) (Grant No. 2015C856801). The authors are 26 M. Kotoul, J. Pokluda, P. Sandera, I. Dlouhy, Z. Chlup and
grateful to the Analytical and Testing Center, Huazhong A. R. Boccaccini, Acta Mater., 2008, 56, 2908–2918.
University of Science and Technology for technical assistance. 27 C. Q. Zhang, D. A. Mcadams II and J. C. Grunlan, Adv. Mater.,
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