中國機械工程學刊第二十八卷第二期第123~131頁(民國九十六年) Journal of the Chinese Society of Mechanical Engineers, Vol.28, No.2, pp.123~131 (2007) Producing Aluminum-oxide brake nanofluids using plasma charging system Mu-Jung Kao *, Ho Chang*, Yuh-Yih Wu *, Tsing-Tshih Tsung*, Hong-Ming Lin** Keywords: Aluminum-oxide brake nanofluids (AOBN), plasma, vapor-lock. INTRODUCTION It has been recognized that the heat transport properties of nanofluids which contain the suspensions of solids particles in liquids is greater than that of fluids with no nanoparticles. The Argonne Research Institute also unveiled the first nanofluid patent [1] claiming heat conductivity to be 1.6 times over the yield of water. The use of Al2O3 particles about 13 nm in diameter at 4.3% volume fraction increased the thermal conductivity of water under stationary conditions by 30% [2].This showed that nanofluid is a revolutionary product as a heat transmitter or lubrication agent. The metal aluminum block can be vaporized instantly by a self-designed plasma electric arc at a high temperature. A self-designed collecting and processing chamber was used to carry out the experiment and produce nanofluid. Vaporized gas and particles were then directed into the collecting pipe by a guiding system and mixed sufficiently with the pre-cooled DOT3 brake fluids to form the nano-aluminum suspension in brake fluid. The minimum particle diameter is about 10nm and average diameter is about 50nm. The study showed that when the temperature of the cooling liquid decreased to 3℃ the nanoparticles had a small diameter and even distribution in brake fluid. The confirmation of appearance of nano-suspension was determined by Transmission Electron Microscopy (TEM), a particles distribution analyzer (LB-500 HORIBA) and X-RAY. The X-ray diffraction (MAC-MXP18, wavelength: 1.54nm) was used to show the pattern of nanoparticles in brake fluid. The average diameter reached about 50nm and the shape of the nano Aluminum oxide fluid particle showed circle geometry and was uniformly dispersed in the brake fluids thus warranting nanofluids to be a revolutionary product as a heat transmission or ABSTRACT This study examines the characteristics of Aluminum-oxide brake nanofluids (AOBN) manufactured by a home-made machine, the plasma arc system. The plasma electric arc welding machine was specially modified to be a nanofluid production system in the experiment. Argon was chosen to be the plasma gas because it can be ionized very easily and needs only lower voltage to keep the production of plasma electric arcs continuous. The aluminum bulk specimen is then mixed with DOT3 break fluid. The AOBN thus obtained shows a higher boiling, higher viscosity and higher conductivity. Furthermore, they are affected by the synthesizing parameters such as cooling liquid temperature and vacuum pressure. The confirmed appearance of nanoparticles was determined by Transmission Electron Microscopy (TEM) and X-RAY. This study revealed that a home made plasma arc machine can produce AOBN which surpasses the boiling point to reduce the occurrence of vaporlock, higher viscosity, higher conductivity and circle geometry common to the superior performance of brake nanofluids. Paper received June, 2005. Revised September, 2005, Accepted October, 2005, Author for Correspondence: Mu Jung Kao * Graduate Institute of Mechanical and Electrical Engineering, National Taipei University of Technology, Taipei, Taiwan, 106,R.O.C ** Department of Materials Engineering, Tatung University, Taipei, 104, R.O.C. 1 J, CSME Vol.28,No.2 (2007) lubrication agent. EXPERIMENTAL & THEORY Experimental The plasma electric arc welding machine was designed to be a nano production system. Operating parameters are shown in table 1. The cooling liquid is set at 3℃ and 15A current operated with voltage at 220. The plasma system was used to vaporize the aluminum in the processing chamber by high temperature from the instantly extracted plasma electric arc. Figure 1 Schematic diagram of plasma nanofluid system To control the parameters such as cooling temperature, plasma gas and nanofluids collecting chamber pressure reached the specified criteria. When it falls within the specified criteria the specimen is regarded as a stabilized nanofluid. The Redwood universal Viscometer and the transient hot-wire method were also employed to measure viscosity and thermal conductivity (Decagon KD2 measure meter). Table 1 Parameters for Plasma charging system processing Curr ent (A) Volta ge (V) 15 220 Cooling Liquid Temperat ure (℃) 3 Press ure (torr) Processi ng (min) 760 12 The parameters to vaporize metal into gas in a short period are as follow: the increase of current will result in rising temperature of the plasma electric arc and the diameter of the electric arc is also increased. The influence will reflect on the particle diameter of the particle produced. Too large plasma current density produces overheat of the plasma injection point. The current of 50A and temperature of 3℃ is the best experiment parameter. So to get the distribution of particles a diameter of about 50~60nm is used. As can be seen from figure 1, the nanofluid production system was improved from a plasma electric arc welding machine. In order to obtain the electric arc, plasma gas was used. Argon was chosen as the plasma gas because it can be ionized very easily and needs only low voltages to keep the continuous production of plasma electric arcs. A shield gas is used to protect the electrode, welding pool and melting metal from pollution or oxidation. The same type of the plasma gas (mixture of Ar +H2 and mixture of Ar+He) was chosen to be the shield gas. This was incorporated with the self-designed collecting and processing chamber to carry out the experiment and produce nanofluid. The nanoparticles after vaporization were guided into the collecting chamber by pressure difference. Theory Nanoparticles Nucleation The process of Al2O3 nanoparticle synthesis that entails embedding pure bulk aluminum in the cooling liquid (the brake fluid) to create vapor through arc spraying requires undergoing three stages. These stages are synthesis, growth and cooling [4]. The crystal growth process starts with the nucleation stage. Several atoms or molecules in a supersaturated vapor or liquid start forming clusters. The bulk free energy of the cluster is less than that of the vapor or liquid. The total free energy of the cluster is increased by the surface tension energy. However, this is significant only when the cluster is small. A cluster of radius smaller than a critical radius, r*will evaporate (or dissolve in the solution) but a cluster of radius greater than r* will become stable and will increase its size by the addition of other atoms and is thus "growing"! The critical radius r* defines a critical energy barrier, △GT , that we need to overcome in order to obtain a stable nucleus that will keep growing and eventually become a large single crystal! Thermodynamics can help us describe the process. Assuming a spherical shape for the nucleus the free energy [3,4] of its formation is: 2 △GT = 4π r2 s + (4/3) πr3 △Gv (1) where △GT is the total free energy; r is the radius of cluster; s is the specific surface free energy, △Gv is the volume free energy; △GT is the free energy change per unit volume forming the stable solidification from vapor or liquid. The total free energy △GT goes through a maximum △GT *at a critical radius r* which can be obtained by derivation of total free energy as given above with respect to radius and solving: (d△GT /dr) = 0 The Plasma arc method is the crystal growth under vapor - solid equilibrium conditions. The temperature of the starting material (powder form) is higher than the nucleation/crystal growth region. This imposed temperature gradient leads to a mass flow resulting in a net mass transport of vapor species towards the nanoparticles growth site. In the process, a material is transformed from a gas state to a solid state, △GT is correlated to the saturation level, while a high level of saturation is determined by the differential in arc current discharge temperature and cooling liquid temperature This means that in order to derive a higher metal nanoparticle synthesis rate, the metal would need to evaporate under high temperature of plasma and coagulate under low temperature in order to achieve the effect. Plasma arc spray converts metal rod material into vapor and then is put through coagulation and mixed with the brake liquid to form brake nanofluid. hN b ⎛ E ⎞ + ⎛ MRT exp ⎜ ⎟ 5⎜ Vm ⎝ π ⎝ RT ⎠ A Aσ 2 - RESULTS AND DISCUSSION With the conductivity measure meter, Decago with KD2, the specimen was measured 20 times, each lasting 10 sec. The measurement time should be kept short to avoid convection which may undermine the measurement accuracy. Table 2, the boiling point of AOBN would increase approximately 8 oC and the heat conductivity of AOBN is 1.5 times over the DOT3 brake fluid thus warranting nanofluid to be a revolutionary product as a heat transmission or lubrication agent. Nanofluids with the aluminum oxide provide the conductivity rising from 0.13 w/moc to 0.19 w/moc. (2) 1/ 2 ⎛ MRT ⎞ 5⎜ ⎟ π ⎠ η = ⎝ 16 N A σ 2 / 16 N In which, M being a mass; NA being the Avogadro’s number; π being a gas viscosity; being a molecule’s radius; what can be deduced from equation(3) is that rising temperature will cause gas viscosity to rise. Nanofluid viscosity is derived from the liquid plus gas model (2) +(3) as denoted in equation (4). When the liquid‘s temperature rising, the first part of equation (4) would steer the liquid viscosity to drop in relation to the exponential function, and as the temperature T increases, the second parts of equation. (4) would drive the nanofluid’s viscosity to rise alongside the nanoparticle mass and the multiplication of the constant number R, hence concluding how the viscosity rating of nanofluids tends to be higher than most liquids from which it can be concluded to related to second term. The Eyring thermal activation theory [5,6] is used to derive a liquid viscosity expressed by equation. (2) hN b ⎛ E ⎞ exp⎜ ⎟ Vm ⎝ RT ⎠ 1/ 2 --------------- (4) Nanofluids Viscosity µ= ⎞ ⎟ ⎠ Table 2 brake fluid’s boiling point & Conductivity (3) DOT3 (brake fluid) The letter h being a Planck constant; Nb being a molecule mass; E being the molecular kinetic energy; Vm being the volume of molecule. What can be extrapolated from equation (2) is that rising temperature would trigger the viscosity to appear in an exponential function (with the denominator value going up) to cause the µ value to diminish. The gas viscosity is then put through the gas movement equation [7] to express by equation. (3), Dry boiling 240℃ point (min) Conductivity 0.13 w/m℃ (25℃) 3 DOT3+2%wt Al2O3 248℃ 0.19 w/m℃ J, CSME Vol.28,No.2 (2007) 14 beams and only allowing light from electron gun central beam through. 12 q(%) 10 8 6 4 2 0 10 100 1000 Diameter(nm) Figure 2 Diameter distribution of aluminum oxide under 50A Figure 4 The TEM image of Aluminum Oxide Figure 2 shows the XRD analysis for second particle diameter distribution from 20-110nm and the average diameter is about 50nm. (0 4 6) Delta Al2O3 (0 4 0) 200 100 (3 1 1) (0 2 0) Intensity 150 50 0 0 10 20 30 40 50 60 70 80 90 Figure 5 The brakefluid’s temperature and viscosity fluctuations 2 Theta Figure 3 The XRD pattern of Al2O3 Figure 5 shows the temperature fluctuation come to affect the viscosity of AOBN and DOT3 brake fluid. The nanofluids are subjected to the rising temperature and the nanofluids’ viscosity to drop. The viscosity of nanofluid consisting of aluminum-oxide nanoparticles tends to be higher than DOT3 liquid. The viscosity of nanoparticles is like the kinetic theory of gases. The theory allows one to estimate the hard sphere collision of molecules from the measurement of the gas viscosity. Equation (3) can be rearranged to obtain an expression for the gas viscosity in terms of the collision diameter. The T1/2 dependence is unusual because gases demonstrate the opposite type of temperature. That is, nanoparticles viscosities increase with increasing temperature. However the nanofluids demonstrate the By inspecting the XRD results of the Nanoparticles, as shown in figure 3. the XRD analysis for the crystalline phase of Aluminum Oxide (Al2O3) can be seen. The crystalline phase was determined by X-ray Diffraction (XRD, MACMXP18). All peaks obtained by XRD analysis were assigned by comparison with data from the Joint Committee on powder Diffraction Standards (JCPDS). The micro structure of the prepared nanofluid was determined using a Transmission Electron Microscope (TEM, JEOL JSM1200EX2). Figure 4 depicts an image of aluminum oxide particles with diameters from 2050nm. The growth of nucleus shows that the aluminum oxide cohesion is big than surface tension which so form as the round geometer. The bright field image is the substrate area which is obtained by intentionally excluding all diffracted 4 opposite type of temperature dependence from liquids, that is, liquid viscosities decrease with increasing temperature so nanofluids’ viscosity drops slowly at high temperature. The higher boiling point of AOBN is contributed by the aluminum oxide nanoparticles. According to a rudimentary braking theory of converting kinetic energy into heat energy, AOBN thus obtained possesses such characteristics as high boiling point, high viscosity and a stabilized state; making it a novel product as a heat transmission or lubrication agent. In a vehicle brake system, the heat energy is absorbed through braking parts and the braking command dispersion is mainly achieved through the braking bearing pads, braking drum or friction between the disks to create the blocking effect. A vehicle’s kinetic energy is dispersed through the heat generated during the braking motion, and the braking command is thus generated through the presence of the heat energy, while the heat energy at the bearing pads arisen from braking is conveyed to the brake fluid through the braking fluid’s hydraulic pistons. However, if the brake fluid’s temperature surges to the boiling point to create a boiling phenomenon. It turn forms a vaporlock, this effectively disables the hydraulic system from conveying the heat, resulting in the moving hazard of brake failure. The study reveals that brake nanofluids serve to enhance the boiling point and higher conductivity which then reduces the occurrence of vapor-lock, thus increasing driving safety. This study was supported by the Depart of Industrial Technology, Ministry of Economic Afairs, R.O.C., contract No. 94-EC-17-A-16-S1051-B3) REFERENCES Argonne National Laboratory, Kate of Patent, No.:US 6221275 B1,Date of Patent:Apr.24.2001. Masuda H., Ebata A. et. al. “Alteration of thermal conductivity and viscosity of liquid by dispersing ultra-fine particles(dispersions of γ- Al2O3, SiO2and TiO2 particles),” Netsu Bussei (Japan) 4, pp.227-233(1993). William D. Callister., materials science and Engineering : an Introduction, Wiley, Seventh Edition, New York, U.S.A, pp.313-315 (2006) William F. S., Foundations of materials science and Engineering, Mcgraw-Hill, third Edition, U.S.A, pp.120-124 (2004) 5Eyring,H.& Eyring,H. :Significant liquid structures New York: Wiley, pp.30-55 (1969) Philip. T E., Mukund. R.P, et. al. J.Appl. Phys.73, pp. 7900-7909. (1993) Keith J L.: The World of Physical Chemistry, Oxford University Press,(1993) p.150154 電漿電弧系統生產奈米氧 化鋁煞車油 CONCLUSION 高木榮 張合 吳浴沂 鐘清枝 +林鴻明 國立台北科技大學機電所 + 大同大學材料所 Aluminum-oxide brake nanofluids can be prepared by plasma charging system when applying the cooling temperature and plasma arc produce rate. There are three good characteristics in aluminum oxide brake nanofluids deriving from the home-made plasma charging system. First, the boiling point of AOBN would increase approximately 8oc. Second, the viscosity of AOBN is consistently higher than that of DOT3 (traditional) brake fluid. Finally, AOBN conductivity is 1.5 times over the yield of DOT3 brake fluid which is from 0.13 w/moc to 0.19 w/moc. The stable and even distribution nanoparticles provide good performance, thus warranting nanofluids to be a revolutionary product as a heat transmission or lubrication agent. 本文旨在探討電漿電弧放電所產生之 奈米氧化鋁煞 車油製程和分析其特 性,對於產出奈米氧化鋁顆粒大小進 行檢測分析,對煞車油共沸點及粘度 具體之探討;其奈米粒徑約為50nm奈 米氧化鋁粒,奈米氧化鋁顆粒外形呈 現圓形提供煞 車系統較低起始摩擦 力,同時提升煞車油共沸點及粘度性 能增加煞車安全性。 ACKNOWLEDGMENT 5
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