Physica C 386 (2003) 366369 www.elsevier.

com/locate/physc

A newly designed ultrasonic spray pyrolysis device to fabricate YBCO tapes

M. Liu *, M.L. Zhou, L.H. Zhai, D.M. Liu, X. Gao, W. Liu
Department of Materials Science and Technology, Beijing Polytechnic University, Beijing 100022, PR China

Abstract A newly designed ultrasonic spray pyrolysis device has been manufactured to fabricate YBCO tapes. The apparatus is primarily composed of four zones: the ultrasonic generator, the atomization chamber, the pyrolysis chamber and the rotating equipment. Every part of them is designed and fabricated by us. The whole system costs far less than the readymade equipment facility in which there is always a vacuum apparatus. This apparatus with processing parameters accurately controlled can fabricate short and long YBCO tapes. In this paper, we mainly focused on how to design and manufacture four parts of the ultrasonic spray pyrolysis. We have deposited c-axis aligned short YBCO tapes on biaxially textured Ag f1 1 0gh1 1 0i substrates with Jc 103 A/cm2 using this method with our device. The method is very promising in terms of its precise control of metal compositions, high deposition rate and low cost non-vacuum approach. Improvements of this technique are being carried out to fabricate long YBCO tapes. 2002 Elsevier Science B.V. All rights reserved.
PACS: 74.76; 81.15 Keywords: YBCO; Ultrasonic spray pyrolysis; Textured Ag

1. Introduction YBCO is the most obvious candidate material for conductor applications because of its high irreversibility eld. However, it is quite dicult to apply with the powder-in-tube (PIT) method. Coated conductor technology starts as a material challenge to get even on a long exible substrate. The most essential factor for the technique is biaxial crystalline alignment control of HTS lms on metallic tapes in order to diminish weak links at misaligned grain boundaries. Recent research

Corresponding author. Tel.: +86-1067392947; fax: +861067392840. E-mail address: htsliu@yahoo.com (M. Liu).

has mainly concentrated on epitaxial growth on buered substrates using the so-called IBAD [1], or RABiTS [2] techniques. Even though Jc values that exceed 1 MA/cm2 are obtained, a denitive answer about which technique is the most appropriate for industrial applications has not yet been given. Therefore, it is of great importance to search for alternative solutions. One such technique is ultrasonic spray pyrolysis of Y, Ba, Cu nitrates. This technique has the advantage of leading to high deposition rates in a non-vacuum environment as well as its precise control of metal compositions. In this paper, we will focus on the ultrasonic spray pyrolysis device designed by us. The apparatus is primarily composed of four zones: the ultrasonic generator (Fig. 1(1)), the atomization

0921-4534/02/$ - see front matter 2002 Elsevier Science B.V. All rights reserved. doi:10.1016/S0921-4534(02)02200-1

M. Liu et al. / Physica C 386 (2003) 366369

367

ser that appears at the liquid surface, where the acoustic waves are focused, varies. By controlling the number of working ultrasonic transducers and the intensity of the geyser we can obtain required mist. Maximal liquid is generated at a rate of 3 cm3 /min.
Fig. 1. Schematic diagram of ultrasonic spray pyrolysis system: (1) the ultrasonic generator, (2) the atomization chamber, (3) the pyrolysis chamber, (4) the rotating equipment, (5) temperature controller, (6) mass owmeter, (7) argon, (8) oxygen.

2.2. Atomization The outer covering of the chamber is made up of transparent organic glass. This material is hard to rust and not as brittle as other ones. There are the outlet and inlet nozzles (Fig. 2(16,17)) for the carrier gas on ektexine of the chamber. Tough surface of the nozzles makes them easy to be connected with other parts of the apparatus. The carrier gas goes into the chamber along the tangent direction to the inside of the atomization chamber, so large droplets, which are detrimental to spray homogeneity, will be thrown away by the eccentric force. In addition, a at splashboard (Fig. 2(19)) placed in the chamber can also prevent large droplets from being transported to the pyrolysis chamber. 2.3. Pyrolysis chamber The pyrolysis chamber consists of two parts: a tubular furnace (Fig. 3(24)) and a quartz tube (Fig. 3(22)) inside. There is an inlet nozzle (Fig. 3(25)) for mist on the top of the furnace and tube. When the droplets travel through the hot-wall furnace and the tube, they will be heated before reaching the surface of the substrates. Because of this, the deposit temperature can maintain stability, which makes it available to carry on sequential deposition (the spray is generated for 1 min, followed by a 2-min delay to allow the surface temperature of the lm to reach the predeposition temperature). It goes without saying that the eciency of the process is improved in this way. Rotating equipment coiled with Ag substrates is placed in the quartz tube. The hot-wall furnace is completely preheated to the deposit temperature. Compared to the substrate heating system, in which only the substrate is preheated to the deposit temperature while the surrounding is very cool, the deposit condition is more stable.

chamber (Fig. 1(2)), the pyrolysis chamber (Fig. 1(3)) and the rotating equipment (Fig. 1(4)).

2. Ultrasonic spray pyrolysis system 2.1. Ultrasonic generator The whole generator is designed and fabricated by retting some old equipment-ultrasonic humidiers. It primarily consists of four independent ultrasonic transducers (Fig. 2(15)), each of which works with the frequency of 1.5 MHz. By varying the voltage xed at a value close to the resonance frequency of the ceramic, the intensity of the gey-

Fig. 2. Schematic of the ultrasonic generator and the atomization chamber: (1) the ultrasonic generator, (2) the atomization chamber, (10) transformer, (11) protecting shell, (12) switch, (13) PC board, (14) box gutter ume, (15) transducers, (16) gas and mist outlet, (17) gas inlet, (18) indicator light, (19) splashboard.

368

M. Liu et al. / Physica C 386 (2003) 366369

Fig. 3. Schematic of the pyrolysis chamber and the rotating equipment: (20) core axis, (21,26) brackets, (22) quartz tube, (23) ceramic tube, (24) tubular furnace, (25) inlet nozzle, (27,28,29) straps, (30) electromotor.

2.4. Rotating equipment We designed and made this part of the equipment innovatively. The aim of this work is to fabricate long tapes of YBCO on textured Ag substrates, which is the core of all the problems, and this equipment can help us achieve the nal purpose. It is not likely to carry reel-to-reel deposition for the exible character of Ag substrates. We wrap Ag substrates on a tube (Fig. 3(23)) made of ceramic, and then place a supporting core axis (Fig. 3(20)) inside of the tube. A screw thread is made between the axis and its brackets (Fig. 3(21,26)) on the end of tubular furnace (the relation similar to between nut and bolt). In the process of deposition, a direct current electromotor (Fig. 3(30)) is used to drive the core axis to rotate. The tube wrapped with Ag substrate worms accordingly. The whole apparatus is designed so delicately that the tube can rotate and meanwhile move forward. Three straps (Fig. 3(27,28,29)) are used for connecting the electromotor and the tube. The electromotor is equipped with a retarder. In this way, the tube will move at any ideal speed. 3. Primary experiment by this device Y, Ba, Cu nitrate solution were made by respectively dissolving Y(NO3 )3 , Ba(NO3 )2 , Cu(NO3 )2 in distilled water. The nal precursor solution was made by mixing the individual solution with cation solution ratio of Y:Ba:Cu 0:9:2:0.5. Overall solution concentration is 0.030 mol/l. The nitrate solution was formed into a mist using the ultra-

sonic generator that gives droplets size of 15 lm [3]. Then argon (3 cm3 /min) was used as the carrier gas to transfer the mist onto the polycrystalline textured Ag substrate preheated at 900 C. At such high temperatures, Y, Ba and Cu oxides produced by the decomposition of nitrate solution react mutually to form the nal compound YBCO. The spray was generated for 20 min. After growth, lms were slowly cooled to 500 C. Oxygenation was carried out at 500 C for 30 min followed by naturally cooling to room temperature.

4. Results and conclusions We have fabricated in-plane c-axis textured YBCO lms with Jc value of 103 A/cm2 (77 K, 0 T) on textured Ag f1 1 0gh1 1 0i substrates by this apparatus. We see good c-axis texture from the Xray diraction diagram (Fig. 4). Fig. 5 shows the

Fig. 4. X-ray diraction diagram of YBCO lm.

M. Liu et al. / Physica C 386 (2003) 366369

369

lm can be obtained by further optimized deposition conditions. The result shows that this device can completely meet the demands of depositing YBCO tapes on textured Ag substrates.

Acknowledgement The authors would like to thank the 973 project of China for funding the work.

References
Fig. 5. Pole gure of (1 0 3) plane of YBCO lm. [1] Y. Iijima, M. Kimura, T. Saitoh, K. Takeda, Physica C 335 (2000) 15. [2] A. Goyal, D.P. Norton, D.M. Kroeger, D.K. Christen, M. Paranthaman, E.D. Specht, J.D. Budai, Q. He, B. Safan, F.A. List, D.F. Lee, E. Hateld, P.M. Martin, C.E. Martin, C.E. Klabunde, J. Mathis, C. Park, J. Mater. Res. 12 (1997) 2924. [3] M. Schindl, J.Y. Genoud, H.L. Suo, IEEE Trans. Appl. Supercond. 11 (2001) 3313.

pole gure of (1 0 3) plane of YBCO lm. Obviously, two high-density zones are symmetric and their intensities are uniform. The orientations in these two areas spread widely, however, which indicates that in-plane biaxial alignment YBCO