Journal of Alloys and Compounds 915 (2022) 165400

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Journal of Alloys and Compounds

journal homepage: www.elsevier.com/locate/jalcom

Hierarchical eutectic structure and superior mechanical property in low

cobalt content AlCo0.2CrFeNi2.1 alloy by laser metal deposition ]]
]]]]]]
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Chong Feng a, Xiaoyu Chai a, Zhonggang Sun a, Xiaochun Liu b, Jiang Wang c, Xiaoma Tao d,
⁎
Fuwen Chen a,e, Guanglong Xu a, , Yuwen Cui a
a
College of Materials Science and Engineering, Nanjing Tech University, Nanjing 211816, China
b
Institute of Metals, Changsha University of Science & Technology, Changsha 410114, China
c
Guangxi Key Laboratory of Information Materials, Guilin University of Electronic Technology, Guilin 541004, China
d
MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials & Guangxi Key Laboratory of Processing for Non-ferrous Metals and
Featured Materials, Guangxi University, Nanning 530004, China
e
School of Materials Science and Engineering, Central South University, Changsha 410083, China

a r t i cl e i nfo a bstr ac t

Article history: The fabrication of AlCo0.2CrFeNi2.1 high entropy alloy via laser metal deposition (LMD) was motivated and
Received 24 February 2022 implemented by the demand for overcoming the strength-ductility trade-off of the as-cast alloys due to the
Received in revised form 9 May 2022 Co concentration. The microstructure features of AlCo0.2CrFeNi2.1 alloy were characterized by scanning
Accepted 10 May 2022
electron microscopy, X-ray diffraction, transmission electron microscopy, and electron back-scattered dif­
Available online 13 May 2022
fraction. The mechanical properties were evaluated by a tensile test at room temperature. The synergy of
reduced Co content and LMD process led to the formation of hierarchical eutectic microstructures con­
Key words:
Laser metal deposition (LMD) sisting of columnar grains, eutectic colonies, alternately arranged fcc(L12)+B2 lamellae, and coherent Cr-rich
AlCo0.2CrFeNi2.1 nanoprecipitates in B2. The growth direction of those eutectic structures was found to be mainly parallel to
Microstructure features the building direction (BD). The fcc(L12)/B2 eutectics agreed well with the Kurdjumov–Sachs orientation
Tensile property relationship of {110}B2//{111}L12, and < 111 > B2// < 110 > L12. The LMD fabricated AlCo0.2CrFeNi2.1 exhibited
Strengthening anisotropic mechanical properties when stretched in BD and transverse direction (TD). An excellent com­
bination of the ultimate tensile strength (1246 MPa) and ductility (17.1%) was achieved in the BD, better
than the as-cast counterpart. The elevated mechanical properties could be attributed to the high cooling
rate solidification induced microstructural refinement. The same interlamellar spacing in BD and TD em­
braced a nearly equal ability to block dislocation movement and gave rise to the similar yield tensile
strength. The differences in grain/colony size induced boundary strengthening in BD and TD were evaluated
to account for the remarkable changes in ultimate tensile strength as well as ductility.
© 2022 Elsevier B.V. All rights reserved.

1. Introduction
High-entropy alloys (HEAs) are a category of unique alloys. The
complex chemical composition consisting of several elements with
equal or near-equal molar ratios produces high mixing entropy but
exhibits a simple single-phase or dual-phase microstructure and
leads to extraordinary mechanical properties different from single-
solvent alloys [1–10]. Thus, they have received considerable interest
and boosted the promotion of new alloy design strategies. The ele­
ment components in HEA concentrate on the systems of AlCoCrFeNi
[11–14], ZrTaNbTiMo [15–18], CrMnFeCoNi [19–22] etc. and form fcc
⁎ The HEAs in the alloy family of AlCrCoFeNi have been widely
Corresponding author.
E-mail address: guanglongxu@njtech.edu.cn (G. Xu).
[23], bcc [24], or hcp [25] solid solution. The interaction among
elements in the single solid solution gives rise to good strength and
hardness [26–29], corrosion resistance [30–32], thermal stability
[33,34], and/or radiation resistance [35]. To improve the poor casting
performance and overcome the strength-plasticity trade-off of the
single-phase HEA, the concept of eutectic HEA with the fine layered
structure of phase has been proposed[36–43]. It takes advantage of
superior yield strength of the bcc phase and outstanding ductility of
the fcc phase [44–48] as well as the synergetic effect of interface
between bcc and fcc phases [49,50]. Moreover, the excellent cast­
ability [51–53] inspires the initiatives of additively manufactured
eutectic HEAs to obtain finer microstructure and superior mechan­
ical performance [53–56].
reported [57–61]. The synergy of chemical composition tuning and

https://doi.org/10.1016/j.jallcom.2022.165400
0925-8388/© 2022 Elsevier B.V. All rights reserved.
C. Feng, X. Chai, Z. Sun et al.
processing initiatives has the ability to broaden the window of
mechanical properties [62–67]. The diverse ever-improving me­
chanical properties, such as high strength, hardness, wear resistance,
fatigue resistance, and fracture toughness have been addressed
[68–72]. Among them, the alloying strategy of Co-free or lowering
the Co content is promising to reduce the raw material cost and
enhance the strength [73–75]. The as-cast AlCrFe2Ni2 alloy enables a
strength promotion in comparison to that of AlCoCrFeNi2.1 [76–78].
However, the enhanced strength has been achieved at the expense of
reduced ductility, similar to the strength-ductility trade-off in other
AlCrCoFeNi alloys [36,47,48,66,67,76–79]. Many novel processing
techniques have been employed to overcome the strength-ductility
trade-off as a result of lowered Co. The directional solidification al­
lows to harvest excellent ductility of at least 25% by sacrificing the
performance of strengths [66,67]. The cutting-edge additive manu­
facturing processes of laser metal deposition (LMD) [64], laser rapid
directional solidification (LRDS) [63], and laser engineered net
shaping (LENS) [80] open up new ways to enhance the strengths of
AlCoCrFeNi2.1 and maintain the ductility similar to that by conven­
tional casting. In the present work, we attempt to tune the chemical
composition of Co in the alloy family of AlCrCoFeNi and take ad­
vantage of LMD additive manufacturing to overcome the strength-
ductility trade-off of the as-cast alloys. The microstructure features
which are strongly correlated to the mechanical performances are
unveiled by phenomenological analyses based on microstructural
strengthening/toughening mechanisms.
2. Materials and experimental procedure
The raw materials for the LMD process were commercial pow­
ders of pure elements (Al, Cr, Fe, Co, and Ni ≥ 99.9 wt% from Jinyu
New Materials Co., Ltd., China). The size of the powder particles
varied between 45 and 75 µm. The pure metal powders were firstly
dried in a vacuum drying oven (DZF-6032, Shanghai Yiheng
Scientific Instrument Co., Ltd., China) at 45 °C for 10 h and then
mixed according to the nominal composition ratio of
AlCo0.2CrFeNi2.1 in the centrifuge tube. The composition homo­
geneity was obtained by the rotary mixing process in a double-cone
mixer. The mixing parameters were set to 20 rpm for 6 h. The LMD
experiment was performed using RC-LDM 8060 (Zhongke Yuchen
Laser Tech. Co., Ltd., China) equipped with a YLS-3000 fiber laser, an
air-carried double-cylinder powder feeder, and a four-way coaxial
powder nozzle. The protective gas and carrier gas in the system were
argon. In the LMD of every single layer, the serpentine scanning path
was employed for depositing. Meanwhile, the moving directions of
the laser beam and powder feeder were perpendicular to each other
between the neighboring layers (see Fig. 1). The mixed powder was
delivered into the laser molten pool on a sandblasted and cleaned
plate of 316 L stainless steel (with a size of 160 × 160 × 15 mm)
through a coaxial nozzle. The processing parameters are summar­
ized in Table 1. The as-deposited sample was built in block shape
with the size of 50 mm in length, 20 in width and 23 mm in height.
The schematic drawing of the LMD process in this work is shown
in Fig. 1.
The tensile samples in the flat dog-bone shape were wire cut
using electrical discharge machining from area b shown in Fig. 1. The
tensile directions were cut along the transverse direction (TD) and
the building direction (BD) within the YOZ plane. The geometry
parameters of the tensile samples are shown in Fig. 1. The uniaxial
tensile test was performed at room temperature on a Bairoe WDW-
50 testing machine under displacement control with a strain rate of
5 × 10−3/s. The high-precision video extensometer without physical
touch was employed to obtain temporal changes in the gauge length
and the average strains of the test sample. Three independent tests
were performed to ensure the reliability of the results.
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Journal of Alloys and Compounds 915 (2022) 165400
Optical Microscope (OM, Zeiss AxioCam MRc5, Germany) and
Scanning Electron Microscopy (SEM, Tescan S8000, Czech) were
employed to observe the phase morphology of the LMD alloy. The
width of eutectic colonies, the interlamellar spacing, and the phase
fractions were measured using Image-Pro Plus software. These
morphology features had been measured repeatedly in different
areas in the LMD sample; thus the values of the average phase
fraction and the average size were of statistical significance. X-Ray
Diffraction (XRD, SmartLab, Rigaku, Japan) was employed to detect
the phases presented in the alloy. It was operated using Cu Kα ra­
diation (λ = 1.5406 Å) at 40 kV and 40 mA with the scanning rate of
2°/min in the range of 2θ = 30–100°. Transmission Electron
Microscopy (TEM) analyses were performed on FEI Talos F200X. The
Selected Area Electron Diffraction (SAED) was employed to verify the
phase identification at the micro-scale. The element distribution
between phases was detected by Energy Dispersive X-ray
Spectrometer (EDS). The crystallographic orientations of the phases
were determined via Electron Back-Scattered Diffraction (EBSD,
EDAX, Pegasus, U.S.) equipped with the Scanning Electron
Microscopy (SEM, Tescan S8000, Czech). It was conducted at an
accelerating voltage of 20 kV with a step size of 0.05–1.00 µm. The
concept of Kernel Average Misorientation (KAM) was employed to
estimate the local misorientation and then to evaluate the accu­
mulation of plastic strain near the fracture.
The SEM and EBSD samples were mechanically ground and po­
lished with sandpapers, 2.5 µm diamond suspension, and 0.04 µm
SiO2 suspension. The stress-free surface finish was obtained via
electro-chemical polishing in an electrolyte consisting of 90 vol%
acetic acid and 10 vol% perchloric acid using a voltage of 50 V and a
polishing time of 50 s. The TEM sample is ground into a foil with a
thickness less than 50 µm, punched into disks with a diameter of
3 mm, and then electro-polished to an electronic-transparent
thickness in an electrolyte containing 10 vol% perchloric acid and
90 vol% ethanol using a twin-jet polishing system.
3. Results
3.1. Chemical composition and microstructure features of the as-
deposited AlCo0.2CrFeNi2.1
The actual chemical composition of LMD fabricated
AlCo0.2CrFeNi2.1 has been measured via EDS and listed in Table 2. The
EDS detections have been duplicated twice or more in different
positions of the deposited block to check the compositional homo­
geneity. The displayed actual composition is the average of multiple
tests in different positions of region b. Fig. 2 shows the phase
identification by XRD demonstrating that the LMD fabricated Al­
Co0.2CrFeNi2.1 is composed of fcc and bcc phases. The diffraction
peaks at 31° and 55° have been indexed as (100) and (111) of the
ordered B2 structure, indicating the bcc phase is ordered B2. The
phases presented in AlCo0.2CrFeNi2.1 are proven similar to those in
AlCrFe2Ni2 and AlCoCrFeNi2.1 [47,67,78]. The slight differences will
be discussed later via TEM inspection.
Fig. 3 presents a hierarchical microstructure of LMD fabricated
AlCo0.2CrFeNi2.1 alloy by OM and SEM. The images are photographed
from the side view of the sample and correspond to areas a, b, and c.
The microstructure in the millimeter-scale is featured by the alter­
nately stacking of the coarse eutectics zone and the fine eutectics
zone (see areas b and c in Fig. 3b and c) except for the top part of the
LMD sample (containing a small number of coarse dendrites). With
OM and SEM, Table 3 summarizes the phase percentages of fcc and
B2 with different morphologies.
At the top of the LMD sample (see Fig. 3a, d, g), there is an arc-
shaped coarse eutectic zone which outlines the geometric feature of
the molten pool in LMD. The location of the arc coarse eutectic zone
implies the position of the heat-affected zone at the bottom of the
C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 1. Schematic drawings of (a) the laser scanning path, (b) the positions of tensile sample selection in LMD fabricated block, and (c) the three-dimensional size of the tensile
sample.

Table 1
Some important process parameters used for LMD of AlCo0.2CrFeNi2.1.

Process parameters Value

Laser power 1200 W

Laser scanning velocity 360 mm/min
Powder feeding rate ~5.0 g/min
Laser spot diameter 3.2 mm
Protective argon flow rate 5.0 L/min
Overlap rate 50%
Layer thickness 0.5 mm
Volumetric energy density ~ 250 J/mm3

molten pool. It infers that the formation of coarse eutectics is as­

sociated with the phase growth in the short-period quiescence ra­
ther than the re-melting and re-solidification in the LMD. The
mechanism is similar to the formation of anomalous Al2O3/GdAlO3/
ZrO2 eutectics in a similar laser deposition [81]. In addition, there are
a small number of coarse dendrites at the top part of the deposited
sample (see area a in Fig. 3a). Either the dark or the light phase can
Fig. 2. XRD patterns of the LMD fabricated AlCo0.2CrFeNi2.1.
form dendrites, as is the LENS fabricated AlCoCrFeNi2.1 by Vikram
et al. [80].
annealing during the intervals of the LMD process [53]. Thus, the
The coarse eutectics zone is extended in the band shape ap­
coarse eutectics zone indicates the boundary of the melt pool [83].
proximatively perpendicular to BD. The thickness of the coarse eu­
The eutectic colonies are produced in the fine eutectics zone,
tectics zone ranges from 20 µm to 200 µm and increases with the
indicating the morphology pattern of a spatially periodic array
height during the layer-on-layer deposition (Fig. 3b and c). Fig. 3f
structure consisting of lamellar plates of the two phases [84]. Dif­
and i illustrates the phase morphology in the coarse eutectics zone.
ferent from the conventional eutectic colonies, the LMD process has
Some domains of the dark gray phase are shaped in bamboo joints
introduced additional microstructural complexity in the hierarchy.
and arranged in alignments. In between the aligned domains, there
The three dimensional reconstruction of the hierarchical micro­
is irregular eutectic microstructure. These morphology features are
structure in the fine eutectics zone is illustrated in Fig. 4, and the
similar to the reported anomalous eutectics in the previous laser re-
details of the morphological features are clearly shown in Fig. 3e and
melted eutectic alloys [53,82]. The formation of coarse eutectics
h. The fine eutectics zone is divided into dozens of columnar grains.
zone has resulted from the partial re-melting of previously de­
The columnar grains have grown approximatively parallel to the BD.
posited layers in the overlapped melt pools and the short-time

Table 2
The chemical composition of LMD fabricated AlCo0.2CrFeNi2.1 (at%).

Items Al Co Cr Fe Ni

Nominal composition 18.87 3.77 18.87 18.87 39.62

Actual composition 17.57 ± 1.05 4.56 ± 0.28 18.67 ± 0.38 18.95 ± 0.26 40.25 ± 0.43
Deviation 1.3 0.79 0.2 0.08 0.63

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C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 3. (a-c) OM images at the top, middle and bottom parts of the LMD block corresponding to areas a, b, and c in Fig. 1; (d-f) the enlarged images for the rectangular areas
(outlined by yellow dashed lines) in the subfigures (a), (b), and (c); SEM images of the dendrites (g), the eutectic colonies in the fine eutectic zone (h), and the irregular eutectic
microstructure in the coarse eutectics zone (i).

Table 3
Phase percentages of fcc and B2 with different morphologies.

Microstructural morphology fcc (L12) B2

eutectic colonies 61.8% 38.2%

coarse eutectics 60.0% 40.0%
dendrites 53.9% 46.1%

There are only 15% of the grains showing an angular difference of the
major axis from BD greater than 15°. The major axis lengths of the
columnar grains, on average, are ~56 µm on the YOZ and XOZ planes,
which is significantly longer than ~21 µm on the XOY plane. The
average width of the columnar grains is similar in XOY, YOZ, and XOZ
planes, showing a value of ~13 µm.
Inside the columnar grain, there are one primary eutectic colony
and several secondary eutectic colonies (see Fig. 3e and h). The
primary eutectic colony consists of multilayers of lamellar phases
which stretch parallel to columnar grain boundaries. The secondary Fig. 4. Stereoscopic three-dimensional (3D) reconstruction of the eutectic micro­
structure.
eutectic colony branches from the axis of primary eutectics at the
approximately same angle of 35°. The remaining domains present
the presence of superlattice spots at 1/2{200}fcc and 1/2{022}fcc
the eutectic morphology with the curved phase boundary. TEM in­
positions along [011]fcc zone axis and 1/2 {200}bcc and 1/2{020}bcc
spections in Figs. 5 and 6 further verify the phase identifications and
positions along [001]bcc zone axis, respectively [48]. The high-re­
the spatial distributions of chemical elements in the fine eutectics
solution transmission electron microscope (HRTEM) images and the
zone. The SAED patterns in Fig. 5b and c indicate that the primary
SAED patterns in Fig. 6 further elaborate that the L12 ordering has
constituent phases are ordered fcc, namely L12, and B2 because of
formed in short-range in the fcc structured lamellar matrix while the

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C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 5. (a) TEM image of the eutectic morphology in the fine eutectics zone fabricated by LMD; (b) and (c) the SAED patterns of L12 and B2 phases. The superlattice spots are
indicated by cyan and yellow circles, respectively; (d) The magnified STEM-High-Angle Annular Dark-Field (HAADF) image of the blue squared area in (a) and the corresponding
EDS maps.

disordered bcc precipitate in nanosize (~30 nm) has been embedded
in the B2 lamellar matrix. These disordered bcc nano precipitates are
rich in Cr evidenced in Fig. 5d. The inserted image in Fig. 6b proves
that the bcc nano precipitate is coherent with the lamellar matrix of
B2 whose interface has been indexed as (020) and (200) planes. The
alternate lamellae of fcc(L12)+B2 with disordered bcc precipitate in
this work are slightly different from the lamellae of disordered fcc
+bcc(B2) in LMD fabricated AlCoCrFeNi2.1 [64].
Fig. 5d illustrates the element distribution mapped with EDS. Al
and Ni have been preferentially enriched in the B2 phase, whereas Fe
and Cr prefer to dwell in the fcc(L12) phase. The partitioning of Co
between B2 and fcc(L12) is inconspicuous. The average chemical
compositions of fcc(L12) and B2 phases are measured Al10.17 ± 1.50-
Co8.12 ± 1.08-Cr26.71 ± 2.12-Fe24.41 ± 1.33-Ni30.57 ± 2.09 and Al34.43 ± 2.55-
Co5.77 ± 0.53-Cr5.13 ± 2.42-Fe9.88 ± 1.23-Ni44.79 ± 2.24 (at%), respectively.
Fig. 7 illustrates the EBSD results for the lamellar microstructure
in the fine eutectics zone. The inverse pole figure (IPF) (in Fig. 7a)
and phase identification images (in Fig. 7b) not only verify the
presence of fcc(L12) and B2 phases but also demonstrate the or­
ientation relationship (OR) between them. The same crystal­
lographic orientation of the B2 phase has been characterized in the
primary and the secondary eutectic colonies. Although the

Fig. 6. (a) HRTEM image and SAED pattern fcc (L12) phase, the inset is the Fast Fourier Transform (FFT) pattern; (b) HRTEM image of a nano-precipitate of bcc inside B2 phase, The
inset shows the coherent feature of B2/disordered bcc interface; (c) and (d) FFT patterns corresponding to the B2 matrix and disordered bcc nano-precipitate, respectively.

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C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 7. (a) IPF map on YOZ plane (the directions OY and OZ are indicated in Fig. 4); (b) Phase map; (c) The locally enlarged view of the black line marked in (a) and the pole figures
of B2, V1 and V2. (V1 and V2 are L12 variants with a twinning relationship).

characteristic also applies to the fcc(L12) phase in most columnar

grains, there are domains in which the fcc(L12) phase can exhibit
different crystallographic orientations in primary and secondary
eutectic colonies (in Fig. 7c). According to the enlarged IPF, the co­
incidences of the poles from the two variants of fcc(L12) and the B2
phase (in Fig. 7c) have been analyzed as [011]L12-V1//[111]B2, (111)
L12-V1//(011)B2 and [101] L12-V2//[111]B2, (111) L12-V2//(011)B2, respec­
tively. It demonstrates that the OR of the B2/fcc(L12) eutectics fol­
lows the Kurdjumov–Sachs (K-S) OR with {110}B2//{111}L12,
and < 110 > L12// < 111 > B2. The fcc(L12) variants of V1 and V2 are
twin-related with a misorientation angle of 60° by rotating against
the axis of [111] [66,85]. Although we only representatively show the
Euler angles of B2, fcc(L12) variant V1, and V2, the K-S orientation
relationship between B2 and fcc(L12) phases and the twinning re­
lationship between fcc variants are generally confirmed in different
colonies. The OR between B2 and fcc(L12) in this work is the same as
AlCoCrFeNi2.1by casting [85] and LRDS [63,86].

Fig. 8. The engineering stress-strain curves of LMD fabricated AlCo0.2CrFeNi2.1 with

3.2. Tensile properties and fracture microstructure of the LMD the tensile directions in BD and TD. The stress-strain responses are compared to those
of as-cast AlCoCrFeNi2.1 [79] and AlCrFe2Ni2 [77].
AlCo0.2CrFeNi2.1

Table 4
The engineering stress-strain curves with the tensile directions in
Tensile properties of the LMD fabricated AlCo0.2CrFeNi2.1 in the tensile direction of BD
BD and TD are shown in Fig. 8. The tensile properties of yield and TD.
strength (YS), ultimate tensile strength (UTS), and ductility (%) at
Direction Yield strength Ultimate tensile Ductility (%)
room temperature are summarized in Table 4. It is clear that the
(MPa) strength (MPa)
LMD fabricated AlCo0.2CrFeNi2.1 alloy exhibits remarkable mechan­
BD 675 ± 27 1246 ± 13 17.1 ± 0.5
ical anisotropy at the macro scale. The sample stretching in the BD
TD 630 ± 29 930 ± 52 5.5 ± 0.8
shows a better combination of UTS of 1246 MPa and ductility of
17.1%, which is obviously superior to UTS of 930 MPa and ductility of
5.5% in the TD. In contrast, the YS stretching in the BD shows The LMD fabricated AlCo0.2CrFeNi2.1 alloy shows mechanical an­
675 MPa, slightly higher than that of 630 MPa in TD. It's worth noting isotropy when the tensile tests are implemented along BD and TD.
that the microstructural features on XOZ plane are identical to those The fracture morphologies of the tensile samples are shown in Fig. 9.
on YOZ plane, the tensile properties in the third direction (side di­ The tensile fractography of the sample stretched in BD appears a
rection SD) would be similar to those in the TD with great prob­ ductile fracture mode due to the densely distributed dimples and
ability considering the same chemical composition of raw materials, grooves [63]. In contrast, the fractography of the sample stretched in
processing parameters, and microstructure features. TD exhibits a mixed fracture mode, which is characterized by the

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C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 9. The fracture morphology of tensile samples stretched in (a-c) BD and (d-f) TD.

cleavage facets with river marking and ravines [66]. A fine lamellar
eutectic structure with bifurcate phase boundaries parallel to the
loading direction can effectively release stress concentration and
impede crack propagation [64].

4. Discussion

In this section, the microstructural features and the mechanical

properties of the LMD fabricated AlCo0.2CrFeNi2.1 are compared to
other alloys in the AlCrCoFeNi family, especially for AlCrFe2Ni2 and
AlCoCrFeNi2.1. The microstructural strengthening mechanisms are
elaborated focusing on the hierarchical characteristics in the eutectic
microstructures.

4.1. Mechanical property comparison in variation arrays of chemical

composition and processing

Fig. 10 demonstrates the strength-ductility trade-off in the alloy

family of AlCrCoFeNi. The combination of UTS and ductility of LMD
fabricated AlCo0.2CrFeNi2.1 in the condition of high volumetric en­
ergy density of ~250 J/mm3 is similar to that of SLM [65] and LMD
[64] fabricated AlCoCrFeNi2.1 with lower volumetric energy density.
The strength-ductility imbalance due to the high volumetric energy
density seems less detrimental in LMD than in SLM. Meanwhile, the
mechanical performances of AlCo0.2CrFeNi2.1 are superior to those of
as-cast AlCrFe2Ni2 [77] and AlCoCrFeNi2.1 [79] under similar condi­
tions of strain rate and sample geometry but are comparable to those
of as-cast AlCrFe2Ni2 tested by a large-sized sample [76]. The sy­
nergy of reduced Co addition and applied LMD process has enhanced
the UTS but maintained the noticeable tensile ductility.
When the tensile properties of the LMD prepared AlCo0.2CrFeNi2.1
are qualitatively compared with those of AlCoCrFeNi2.1 and
AlCrFe2Ni2 in different processes, the mechanisms of solid solution
strengthening, grain/colony boundary strengthening, phase inter­ Fig. 10. (a) UTS and ductility trade-off, (b) YS and ductility trade-off of LMD fabricated
facial strengthening, and dislocation strengthening have been jus­ AlCo0.2CrFeNi2.1 are compared with those of AlCoCrFeNi2.1 and AlCrFe2Ni2 alloys via
tified [78,87]. Fig. 11 summarizes the average chemical compositions different processes.

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C. Feng, X. Chai, Z. Sun et al. Journal of Alloys and Compounds 915 (2022) 165400

Fig. 11. The average chemical compositions of (a) fcc(L12) and (b) B2 phases in the
alloys of AlCoCrFeNi2.1 [36,62,67,88,89], AlCo0.2CrFeNi2.1(this work), and AlCrFe2Ni2
[90] prepared via different processes. The number in the square bracket indicates the
reference number.

of fcc(L12) and B2 phases in three alloys through different processes.

The addition of Co and the reduction of Fe in alloys have greater
effects on the element partitioning between fcc(L12) and B2 than the
variations of processing conditions. Casting, directional solidifica­
tion, and most additive manufacturing processes produce the almost
identical chemical compositions of fcc(L12) and B2 in AlCoCrFeNi2.1.
The less addition of Co in AlCo0.2CrFeNi2.1 than AlCoCrFeNi2.1 leads to
the increased contents of Cr and Fe in the fcc(L12) phase and Al and
Ni in the B2 phase. It also results in the element partitioning of Cr
from B2 lamellar matrix to disordered bcc nano precipitate (see
Fig. 5d). These variations are more apparent in AlCrFe2Ni2 except
that the content of Cr in fcc(L12) falls back to a value similar to Al­
Fig. 12. The comparisons of (a) the columnar grain width, (b) the primary colony
CoCrFeNi2.1.
width, and (c) the interlamellar spacing in the alloys of AlCo0.2CrFeNi2.1(this work)
With the element contents in individual phases, the effect of and AlCoCrFeNi2.1 [47,63,64,66,67,88,95–101] prepared via different processes. The
solid solution strengthening owing to the composition tuning of Co number in the square bracket indicates the reference number.
element is evaluated. Following the model of Archard [91] and
Fleischer [92] and materials parameters from [93,94], the strength [63,64,95–97]. The comparisons of the primary colony width and the
increments caused by the variations of element partitioning of Co interlamellar spacing between AlCo0.2CrFeNi2.1 and AlCoCrFeNi2.1 are
and Fe range from 1.42 to 11.12 MPa following the strategy of [87]. shown in Fig. 12b and c [47,63,64,66,67,88,95–101]. The LMD fabri­
The estimated values are much tiny when the actual strength in­ cated AlCo0.2CrFeNi2.1 in this work exhibits a comparable inter­
crement due to the LMD process is compared with that of the casting lamellar spacing of ~800 nm to AlCoCrFeNi2.1 by LRDS [63], and
and the directional solidification process. It infers that solid solution smaller than that in AlCoCrFeNi2.1 fabricated by LMD [64].
strengthening is not the foremost mechanism in the LMD process. The Hall-Petch-like size relationship also applies to phase inter­
The tiny composition variations of Co and Fe between Al­ facial strengthening. According to the continuum dislocation pile-up
Co0.2CrFeNi2.1 and AlCoCrFeNi2.1 alloys seem trivial in solid solution theory [102], the phase interfacial strengthening Δσint is related to
strengthening. The same conclusion has been obtained in the pro­ the barrier stress τint and the pile-up length L, expressed as:
cesses of magnetron sputtering [87] and laser remelting [78].
The strengthening effects of refined grains, colony, and lamellae 1
Gb int
2 1
in different processes is always evaluated via the generalized Hall- int = L 2
(1 ) (2)
Petch equation:

= + kd 1/ n
HP 0 (1) τint is induced by shear modulus mismatch and lattice mismatch
[50]. Considering shear modulus is microstructure insensitive [103]
In Section 3.1, the average widths of the columnar grain and the
and the tiny compositional variations of Co and Fe with similar
primary eutectic colony have been measured as ~13 µm and ~2.5 µm,
atomic size hardly introduce the noticeable lattice mismatch [78],
respectively. In Fig. 12a, we compare the width of columnar grains in
the term in the square bracket can be nearly constant for the sam­
alloys of AlCo0.2CrFeNi2.1 and AlCoCrFeNi2.1 prepared via different
ples fabricated by LMD, casting, and directional solidification. We
processes. The columnar grains introduced by different additive
assume that the pile-up length L is equal to interlamellar spacing,
manufacturing processes are without exception much thinner than
the interfacial strengthening can attribute to the smaller lamellar
those prepared by conventional casting and directional solidification

8
C. Feng, X. Chai, Z. Sun et al.
spacing ~0.8 µm in the LMD AlCo0.2CrFeNi2.1 than ~1.1 µm in the as-
cast AlCoCrFeNi2.1.
In summary, the advantage of the high cooling rate in LMD
produced refined grains, eutectic colonies and lamellae in the hier­
archy and contribute to the improved strengths. Considering the
phase fractions, the sizes of eutectic colony and lamellae, and the
element partitioning are almost the same for AlCo0.2CrFeNi2.1 in this
work and LMD [64] and LRDS [63] fabricated AlCoCrFeNi2.1, it can
imperfectly infer that the laser additive manufactured alloys with
similar microstructural features would exhibit similar mechanical
performance in tensile tests. On the other hand, the strength-duc­
tility trade-off in the alloys by laser additive manufacturing seems
less obvious than those by casting. The change of process conditions
surpasses the composition tuning of Co and Fe and plays a more
important role in the size refinement strengthening.
4.2. Microstructural origins of anisotropic mechanical properties
To figure out the microstructural origins of anisotropic mechan­
ical properties, the KAM map has been scanned to estimate the
average misorientation between the adjacent pixels and is asso­
ciated with the magnitude of accumulated dislocation density.
Considering that the amount of statistically stored dislocations in
the as-deposited alloy is small [104], the estimated dislocation
density includes the contributions from geometrically necessary
dislocation and regenerated dislocation in the tensile test. The total
dislocation density ρ can be simplified as [105]:
2KAMave
= Herein, we put forward a sequential dislocation strengthening
µb
where KAMave represents the average misorientation of the selected
area; μ is the unit length of the point, which is 50 nm in this study;
and b is the Burgers vector measured by HRTEM, which is 0.22 nm
for L12 phase and 0.20 nm for B2 phase. Fig. 13 shows the IPFs and
KAM of the lamellar microstructure near the fracture. The corre­
sponding local misorientation frequency is shown. The data of the
sample stretched in BD are illustrated in subfigures (a)-(c), and those
of TD are illustrated in subfigures (d)-(f). In comparison with the
orientations and phases that were perfectly indexed in the as-
Fig. 13. The IPF map (a, d), KAM distribution map (b, e), and local misorientation frequency (c, f) near the fracture with the tensile direction of (a-c) BD and (d-f) TD.
Journal of Alloys and Compounds 915 (2022) 165400
deposited state before the tensile test (see Fig. 7), there are some
unindexed areas near the colony collisions and grain boundaries in
IPFs indicating that the tensile deformation has induced noticeable
lattice distortion and stress concentration. The evaluated KAMave
values and dislocation densities are summarized in Table 5. The local
misorientation is mainly distributed at grain and phase boundaries
as the greater KAM data indicate (Fig. 13 b and e). The values of
KAMave are estimated as 0.68° and 1.01° after the tensile test in BD
and TD, respectively (Fig. 13 c and f). It infers that more dislocations
have been accumulated when the tensile direction is TD than those
for BD, which leads to a considerable plastic strain gradient near the
fracture. The greater plastic strain gradient accumulated accounts
for the poor performance of ductility.
To further clarify the anisotropic mechanical performance, the
increment of dislocation strengthening (approximate to strain-
hardening) is correlated to dislocation density via equation [106]:
= M Gb (4)
Here, M is the Taylor factor (3.06), α is a constant (0.26), and G is
the shear modulus of 43.1 GPa derived from the tensile test at room
temperature, Burger’s vector is extracted from the HRTEM image, Δρ
is the difference in dislocation densities between TD and BD from
Table 5. ∆σ between BD and TD is estimated ~250 MPa, close to the
measured UTS difference in Table 4. Moreover, there is an inversely
proportional relationship between and size parameter λ
reads [107]:
= c/ (5)
(3)
mechanism corresponding to the hierarchical microstructure to in­
terpret the different behaviors of YS and UTS. Different size para­
meters λ dominate the strengthening in different stages in the
tensile test. At the early stage of the tensile test, the mechanism
triggered at the earliest to hinder the dislocation motions is the la­
mellar phase boundaries between fcc(L12) and B2. Thus, the ‘mean
free path’ of dislocation movement within the lamella equals lamella
width which serves as the size parameter λ at the smallest scale in
the hierarchical microstructure. Because (1) the lamella width is
almost identical on the BD, TD, and SD planes, and (2) the synergy of
9
C. Feng, X. Chai, Z. Sun et al.
Table 5
The Phase percentages (%), KAMave (°) and ρ(×1015/m2) near the fracture of the samples stretched in BD and TD.
Sample L12 Phase percentage B2 Phase percentage KAMave (Total)
BD 87.1 12.9 0.68
TD 66.7 33.3 1.01
variously oriented fcc(L12) and B2 lamellae within different colonies
and grains gives rise to the isotropic average size parameter λ in
statistics, the YS values with the tensile directions in BD and TD only
show a slight difference. Thus, dislocation strengthening at lamellar
phase boundaries is considered the main mechanism to determine
the YS of LMD AlCo0.2CrFeNi2.1.
With the loading processed, the average ‘mean free path’ of the
dislocation movement is increased. The strengthening mechanisms
of colony and grain boundaries have been triggered. The disloca­
tions, as well as the severe deformation and lattice distortions, are
accumulated in the areas of colony collisions and grain boundaries.
The preferred colony orientations and the elongated grains result in
the anisotropic ultimate strength and ductility at the macro-scale. It
is because the average aspect ratio of colony/grain on the YOZ plane
is significantly greater than that on the XOY plane, the total dis­
location accumulated at colony collisions and grain boundaries/
triple junctions can’t be uniformly shared by more colony/grain
boundaries, thus the stress concentration should be more severe
when the tensile stress is applied in TD. Thus, dislocation strength­
ening at colony and grain boundaries is considered the main me­
chanism to determine the UTS and ductility of LMD AlCo0.2CrFeNi2.1.
The interpretation also applies to the anisotropic feature of strain-
hardening revealed by the stress-strain curves.
4.3. Limitations
Based on the above discussion, we understand that the high
cooling rate in LMD produced refined eutectic colonies and lamellae
in the hierarchy in the AlCo0.2CrFeNi2.1 alloy. The more percentage of
grain/phase boundaries and the shorter lamellar spacing improved
the strength of the alloy. However, the rationalizations have some
limitations. The discussion of the strengthening/toughening me­
chanisms is phenomenological and qualitative. Only the strength­
ening/toughening factors originating from the microstructure
features have been considered. The processing-related factors which
are capable of affecting strengths and ductility, e.g. thermal-induced
residual stress, haven’t been incorporated in the mechanism ana­
lyses. The proposed sequential dislocation strengthening mechanism
corresponding to the hierarchical microstructure requires further
validations and verifications via in-situ observation, although it is a
plausible and self-consistent explanation based on the available
experimental results. As far as the mechanical performance is con­
cerned, LMD maintains the mechanical performance at a high level
with less dosage of expensive Co, which is comparable to LMD
AlCoCrFeNi2.1. The ultimate tensile strength and the ductility of LMD
AlCo0.2CrFeNi2.1 are higher than the as-cast AlCoCrFeNi2.1 and
AlCrFe2Ni2 with similar test parameters and specimen geometry,
however, the improvements are not fantastic. The potential of LMD
and other additive manufacturing techniques to produce a combi­
nation of superior strength and ductility requires further ex­
ploration.
5. Conclusions
In this work, an AlCo0.2CrFeNi2.1 high entropy alloy was fabri­
cated by LMD to understand the strength-ductility trade-off origi­
nating from the composition tuning of Co under the additive
10
Journal of Alloys and Compounds 915 (2022) 165400
KAMave (fcc/L12) KAMave (B2) ρ (Total) ρ (fcc/L12) ρ (B2)
0.60 1.22 2.20 1.90 4.26
0.95 1.13 3.32 3.01 3.94
manufacturing processing condition. The hierarchical micro­
structure features were observed and the tensile mechanical prop­
erties were measured. The microstructural strengthening factors
leading to the improved strength-ductility combination compared to
the as-cast alloy and the anisotropic mechanical performance dif­
ferent in BD and TD were analyzed via a comprehensive comparison.
The main conclusions were as follows:
(1) The LMD fabricated AlCo0.2CrFeNi2.1 alloy mainly showed a eu­
tectic microstructure. The fine eutectic zone embraced a hier­
archical microstructure consisting of the columnar grains, the
eutectic colonies, and the alternately arranged fcc(L12)+B2 eu­
tectic lamellae with the growth direction approximatively par­
alleling the BD. In addition, there were coarse eutectics zones
and a small number of coarse dendrites.
(2) The fcc(L12)/B2 eutectics in fine lamellae followed the
Kurdjumov–Sachs orientation relationship of {110}B2//{111}L12,
and < 111 > B2// < 110 > L12. Compare to AlCoCrFeNi2.1 and
AlCrFe2Ni2, the chemical composition tuning of Co in
AlCo0.2CrFeNi2.1 gave rise to the increased contents of Cr and Fe
in the L12 phase as well as Al and Ni in the B2 phase, meanwhile
resulted in the element partitioning of Cr from B2 lamellar
matrix to disordered bcc nano precipitate.
(3) The tensile behaviors were evidenced to be different when the
tensile directions were applied along the BD and the TD. The
alloy exhibited an excellent combination of the ultimate tensile
strength of 1246 MPa and ductility of 17.1% in the BD. The per­
formance was comparable to AlCoCrFeNi2.1 via a similar LMD
process.
(4) The LMD process gave rise to the refined widths of columnar
grain and eutectic colony and interlamellar spacing in compar­
ison to the as-cast microstructure feature, thus resulted in
strengthening and toughening. The employment of LMD can
override the composition-induced strength-ductility trade-off in
the ac-cast samples.
(5) The same interlamellar spacing in BD and TD embraced a nearly
equal ability to block dislocation movement and gave rise to the
similar yield tensile strength. The differences in grain/colony
size induced boundary strengthening in BD and TD were eval­
uated to account for the remarkable changes in ultimate tensile
strength as well as ductility.
CRediT authorship contribution statement
Chong Feng: Investigation, Characterization, Writing-original
draft, Visualization;. Xiaoyu Chai: Investigation, Data curation;.
Zhonggang Sun: Conceptualization, Methodology, Validation,
Resources, Supervision, Funding acquisition;. Xiaochun Liu:
Investigation, Characterization, Writing-review & editing, Funding
acquisition;. Jiang Wang: Resources, Funding acquisition, Project
administration;. Xiaoma Tao: Resources, Software, Funding acqui­
sition;. Fuwen Chen: Methodology, Validation, Formal analysis,
Writing-original draft, Visualization;. Guanglong Xu: Methodology,
Validation, Writing-review & editing, Visualization, Funding acqui­
sition;. Yuwen Cui: Conceptualization, Methodology, Supervision,
Project administration.
C. Feng, X. Chai, Z. Sun et al.
Declaration of Competing Interest
The authors declare that they have no known competing fi­
nancial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgments
This work was financially supported by the Open Foundations of
Guangxi Key Laboratory of Processing for Non-ferrous Metals and
Featured Materials, Guangxi University [Grant no. 2021GXYSOF05],
Guangxi Key Laboratory of Information Materials, Guilin University
of Electronic Technology [Grant no. 211010-K]. ZS acknowledges the
financial support from the National Natural Science Foundation of
China [Grants no. 51875274]. XL acknowledges the Natural Science
Foundation of Hunan Province Youth Fund [2021JJ20011], and the
Natural Science Foundation of Hunan Province [2021JJ40590] XT
acknowledges the support from the Guangxi Natural Science
Foundation [Grant no. 2018GXNSFAA281254].
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