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Article history: This paper describes an investigational study of the spheroidization of refractory metal tungsten powders by
Received 5 November 2016 radio frequency thermal plasma, with emphasis on the melting, solidification and growth behavior of the tung-
Received in revised form 23 January 2017 sten powder particles during the spheroidization process. The flight time and melting time of tungsten powder
Accepted 29 January 2017
particles in the plasma were estimated, and the growth behavior of the tungsten powder particles was analyzed
Available online 24 February 2017
in detail by investigating the change in the average particle size before and after plasma spheroidization. The
Keywords:
morphology and spheroidization rate were analyzed using field emission scanning electron microscopy. The
Radio frequency thermal plasma flight time and melting time for tungsten powder particles with radius of 7.8 μm were calculated to be 9.3 ms
Spheroidization and 2.9 ms, respectively. The change in powder particle size during the process showed that the growth of tung-
Tungsten powders sten powder particles was mainly caused by the coalescence of droplets in the thermal plasma system. The exper-
DPV-2000 imental results demonstrated that the spheroidization rate can reach up to 95% under the operating conditions
used in this work.
© 2017 Elsevier Ltd. All rights reserved.
1. Introduction spraying, powder metallurgy, and so on. Thermal plasma technique has
been proven as an effective technique for preparing spherical tungsten
At or close to atmospheric pressure, the high-power radio frequency powders because of its properties of high temperature and high
(RF) thermal plasma has become effective heat and chemical reaction enthalpy, and it may be used in the industrial production after further
sources for various material processes such as synthesis nanoparticles studies [18,20].
[1–3], spheroidization of micron-sized powders [4–6], and preparation Plasma spheroidization of refractory metal tungsten powders con-
of novel nano-carbon materials [7–9]. These applications are based on sists of two main processes: first, the raw tungsten powder injected
the unique advantages of RF thermal plasma such as ultra-high temper- into the high temperature region of RF thermal plasma is heated up
ature (thousands of Kelvin, even up to 104 K), high chemical reactivity, and melted to form spherical droplets due to surface tension, then the
large plasma volume, high cooling rate (104–105 K/s) as well as long res- melted droplets solidify into spherical particles due to rapid quenching
idence/reaction time due to its comparatively low plasma velocity [10, when they spurt out of the plasma. The melted status of the powder par-
11]. Specifically, the RF thermal plasma can be considered an innovative ticles is essential for the formation of spherical tungsten powder; how-
and powerful tool for spheroidization of refractory metals and ceramic ever, not all powder particles can be melted completely in spite of the
powders into spherical powders by one-step production [12]. plasma temperature being much higher than the melting point of tung-
Tungsten is one of the most useful and unique metals, with the sten. The reasons for this incomplete melting could be that the powder
advantages of high melting point, high specific mass, good corrosion particles cannot absorb sufficient plasma energy due to the non-uni-
resistance, and low release of gases. It has many industrial applications form temperature inside the plasma torch, the local cooling effect of
and has been widely used in fields such as electronics, military, and the plasma by the cold carrier gas and flow of powder particles [19], as
nuclear industry [13–17]. In addition to the above-mentioned advan- well as insufficient optimization of experimental parameters. Therefore,
tages, spherical tungsten powders exhibit outstanding properties such fully understanding the melting and solidification behaviors of tungsten
as excellent flowability, high bulk density, and low sintering shrinkage, particles and the influence of powder feed rate on the spheroidization
making them suitable for a broad range of applications such as thermal rate is very important. Recently, Jiang [20] reported that a tungsten par-
ticle with a diameter of 60 μm requires 1.4 × 10−3 J of heat energy for
⁎ Corresponding author. complete melting. However, for a given powder feed rate of 80 g/min,
E-mail address: zhuhl@sxu.edu.cn (H. Zhu). the corresponding heat energy required for completely melting all
http://dx.doi.org/10.1016/j.ijrmhm.2017.01.017
0263-4368/© 2017 Elsevier Ltd. All rights reserved.
H. Zhu et al. / Int. Journal of Refractory Metals and Hard Materials 66 (2017) 76–82 77
tungsten particles is about 51.6 kJ. Xiong et al. [21] presented a dimen- system, DPV-2000 monitoring instrument, powder reaction and collec-
sionless parameter called the melting index to describe the melting sta- tion chamber, and exhaust system. The schematic illustration of the
tus of powder particles, and revealed that the total melting time is setup is shown in Fig. 1.
reciprocal to the particle diameter and velocity. For a given powder, In a typical experimental procedure, a soft vacuum of approximately
the melted status of the powder particles is determined by plasma tem- 40 kPa was created by the vacuum pump and a plasma-forming gas
perature and velocity, because the plasma temperature is related to the (argon) was injected into the plasma torch at 25 slpm before the igni-
melting time of the powder particles, and the plasma velocity deter- tion of the plasma. The power was gradually increased, and a spark dis-
mines the flight time of the powder particles. Several studies [20–23] charge was generated due to the direct electrostatic field generated by
have shown that oxidation and crystallization behaviors of in-flight par- the coils. Following the ignition, the power and gas flow including plas-
ticles occur during plasma spheroidization of metal powders. For most ma-forming and protective sheath gases were increased gradually to
metal powders, it is hard to be oxidized at room temperature, but is rap- maintain a stable plasma. Then, the raw tungsten powder particles
idly oxidized at high temperature if there is a small amount of air were carried by the carrier gas (argon) to a powder injection probe
remaining in the chamber, or in the air thermal plasma environment. inserted into the plasma high temperature region. The injected tungsten
High oxidation rate of tungsten particles occurs in the tail of the thermal powder was melted in the plasma high temperature region and solidi-
plasma under atmospheric pressure or soft vacuum condition. Besides fied into spherical particles at the exit of the plasma. A DPV-2000 mon-
the melting, solidification, oxidation and crystallization behaviors, pow- itoring instrument (TECNAR Automation, St-Bruno, QC, Canada) fixed at
der particles also show a growth behavior rather than refinement in the the end of the plasma flame (at 80 mm down the spout of plasma torch)
plasma spheroidization of refractory metal and ceramic powders [24, was employed for monitoring the in-flight particle temperature, veloc-
25]. However, the growth behavior of powder particles and the related ity, size and the average values of these parameters. Finally, the
mechanism have rarely been reported. spheroidized powder particles were collected at the collection point.
In the present study, an experimental process of RF thermal
spheroidization of refractory metal tungsten powders has been intro-
duced firstly. The melting behaviors of the powder particles were inves-
tigated by estimating the plasma temperature, plasma velocity, and
melting and flight times of tungsten powder particles in the plasma.
The growth behavior of the tungsten powder particles during the
spheroidization process was focused on. Finally, the spheroidization
rate and proposed parameters were discussed.
Table 1
Experimental conditions for spheroidization of tungsten powder.
Parameters Values
enough time for the tungsten powder particles to melt. Increasing the gravity. The particle size distribution at the point of measurement is in
plasma temperature and reducing the plasma velocity as much as pos- the range of 5–47 μm, and the average particle size is about 20 μm (in
sible would be beneficial to ensure complete melting of the tungsten Fig. 3(c)). Compared to the raw powder, the particles display a growth
powder particles. behavior during spheroidization process. The detailed discussion on
the change in particle size is given in Section 3.4.
3.3. Experimental results of the temperature, velocity and size distribution
of the in-flight particles
3.4. Characterization of tungsten powder particles and spheroidization rate
Fig. 3 shows the results of the temperature, velocity and size distri-
bution of the tungsten powder particles at the flame tail measured by The FE-SEM image in Fig. 4(a) shows the morphology of raw tung-
DPV-2000. It can be seen from Fig. 3(a) that the average temperature sten powder, and it can be seen that the raw powder particles are irreg-
of all the monitored particles is 3032 °C (3035 K) lower than the melting ular. After being processed by plasma, spherical tungsten particles are
point of tungsten powders, and the typical standard deviation of the formed and the corresponding FE-SEM image is shown in Fig. 4(b).
particle temperature is about 182 °C. This result indicates that the mol- The prepared tungsten powder particles present an excellent spherical
ten droplets flowed out of the plasma high temperature zone and the degree and spheroidization rate close to 95%. This result indicates that
surface of the droplets began to solidify at the flame tail. Fig. 3(b) the raw tungsten powder particles are melted almost completely
shows that the average velocity of the particles at flame tail is 25 ± through absorbed plasma energy under these experimental conditions.
5.1 m/s, which is approximately equal to the velocity of the plasma. The spheroidization rate is an important parameter for the plasma
Compared to the DC arc thermal plasma, the lower velocity of RF ther- spheroidization of powders. In this work, the spheroidization rate of
mal plasma is beneficial for the spheroidization of powder particles, the tungsten powders was obtained from the FE-SEM images using
because low velocity leads to longer flight time in plasma high temper- the following method. The total number of tungsten powder particles
ature region. Nevertheless, Fig. 3(b) indicates that the powder particles counted in ten different FE-SEM images is A, and the number of spher-
undergo some acceleration in the plasma. The initial velocity of the ical particles in those images is B. Then the spheroidization rate, η, is
powder particles is controlled by the propulsion force of the carrier
gas and it is about 5.3 m/s. At the flame tail, the powder particles are
accelerated close to 25 m/s by the drag force of plasma and their own
Fig. 6. Variation of the apparent density, tap density and powder flowability with
Fig. 5. Effect of feed rate on the spheroidization rate of tungsten powder. spheroidization rate of tungsten powder.
80 H. Zhu et al. / Int. Journal of Refractory Metals and Hard Materials 66 (2017) 76–82
analysis indicated that the samples were nonporous since the character-
istic hysteresis loop was absent in the adsorption–desorption isotherms.
4. Conclusions
Table 2
Particle size distribution of the tungsten powders before and after the spheroidization.
In summary, micron-sized spherical tungsten powder particles have
Size (μm) Raw powder In-flight particles Spheroidized powder been successfully prepared via a rapid melting and solidification process
D5 5.78 / 4.52 in RF thermal plasma system, despite tungsten having the highest melt-
D10 7.09 / 7.11 ing point among all metals. The melting, solidification and growth
D50 15.60 20 28.79 behaviors of the tungsten powder particles during the spheroidization
D90 29.02 / 68.02
process were investigated by estimating the flight time and melting
H. Zhu et al. / Int. Journal of Refractory Metals and Hard Materials 66 (2017) 76–82 81
Fig. 8. The coalescence behavior of tungsten powder particles after the plasma spheroidization.
(1) The efficient melting of the tungsten powder particles in the plas-
ma requires the flight time to be greater than the melting time.
Under the experimental conditions in this work, the flight time
and melting time for tungsten powder particles with radius of
7.8 μm were calculated to be 9.3 ms and 2.9 ms, respectively.
These results are consistent with the experimental results and
confirm the high spheroidization rate.
(2) The tungsten powder particles show a growth behavior during
the entire flight process through the system. The coalescence of
droplets caused by collision in the thermal plasma system is
Fig. 10. The change in the average particle size along the axis of vacuum chamber.
Acknowledgement
Fig. 9. The adhesion behavior of tungsten powder particles after the plasma This work is supported by the National Natural Science Foundation
spheroidization. of China (Nos. 11205050, 11535003, and 11404198).
82 H. Zhu et al. / Int. Journal of Refractory Metals and Hard Materials 66 (2017) 76–82
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