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1 Jurnal f the Krean Ceramic Sciety Vl. 47, N. 4, pp. 319~324, DOI: /KCERS Preparatin f Screen Printable Cnductive MSi 2 Thick Films fr Ceramic Sheet Heater Bae-Yen Kim, Dng-Bin Han*, and Chel-Wen Jeng* Department f Materials Science and Engineering, University f Inchen, Inchen , Krea *Winnertechnlgy, Pyengtaek , Krea (Received July 13, 2010; Revised July 19, 2010; Accepted July 20, 2010) Screen Printable MSi 2 Paste w ½ Áw *Á * w œw *( ) lj ( ; ; ) ABSTRACT Screen printable MSi 2 paste and its ceramic sheet heater were investigated. MSi 2 pwder withut M 5 secnd phase, which causes s-called pest phenmena, was synthesized by SHS technique. Over glaze was als develped fr preventing pest phenmenn. The maximum temperature f MSi 2 ceramic heater was ver 500 C. After several heat up and cling cycle, the MSi 2 heater reveals pest phenmenn. Cnductive MSi 2 paste culd be used in electrnic ceramics, i.e., MLCC, LTCC, HTCC, and etc. Key wrds : MSi 2, Sheet heater, Ceramic, Paste, SHS MSi 2 / w j v q ƒ w paste w z» ü» wš. 200 C w ƒ w ƒ, C ü Ag Ag-Pd RuO 2 š 700 C~800 C š ƒ W, M-Mn ƒ.»q PETù plyimide/xide d Al wš š»q wš.»q w» w ƒ š q w v ƒ ƒ w, g x». š ü t P fvsp ƒ t š» ƒ û, HTCC green sheet w Crrespnding authr : Bae-Yen Kim bykim@inchen.ac.kr Tel : Fax : W w š. Watlw ELS» wš. š ƒ ƒ t ù y š v l ƒ e ƒ wù w» xr. MSi 2 ƒ g/cm Ag/Pd w ûš, 2,020 C, š y w k ƒ j š ) Kanthal ƒ» yw» 1,800 C ü š. MSi 2 þƒ ƒ wš, ƒ w» w yƒ ƒ ƒ w š. ù MSi 2 j v q ƒ w r p w. MSi 2 ƒ ƒ w þƒ ƒ w q. w» MSi 2 w û 6~7 V 20~30 A» w w SCR w p s 319

2 320 ½ Áw Á w w, r p w z» w f» 220 V ƒ w ƒ. MSi 2» š wù yx j pest x w» w r p w. w š MSi 2 w yx w ver glaze wš w MSi 2 pest x r p MSi 2 y, ³y yw š y w, y x ƒ. x mp pest x 2,3) š š. pest x 1955 Fitzer w š, ƒ 3) ¾ z MSi 2ƒ w» pest x š. yƒ. MSi 2 w, yw š. 3,4) MSi 2 (s)+7/2o 2 (g)=mo 3 (s)+2sio 2 (s) (1) MSi 2 (s)+7/5o 2 (g)=1/5m 5 (s)+7/5sio 2 (s) (2) MSi 2 (1) t ù, MO 3 { ú ƒ. w 4) MSi 2 t SiO 2 d û š, t d MSi 2 y w barrier w., y v MSi 2 (2) w w t w ù, yv MSi 2 y» š y w ùkü. MSi 2 t yd 550 C š, yd»» 450 C~550 C (2) w M 5 ƒ. M 5 ƒ g/cm MSi g/cm w 30% ƒ û» ü q w crack jš, crack mw ù pest x k š š š. 1,4-8) w pest x œ w micrcrack,» œ w w š. œ 1) MSi 2»» ù y ƒ,»œ MSi 2 y ƒ x j š š 6)wš. MSi 2 MSi 2 y w š9) w crack r pest x, MSi 2 MSi 2ƒ pest x w w { j š š. MSi 2ƒ 900 C l (1) w MO 3 š w ú ƒ t SiO 2 y v x, z y v š y ww y w pest x w. 10) ww pest x w MSi 2ƒ pest x w š M 5 ƒ MSi 2 w w, ƒ»œ ù w xk r p z w w, y v x g w., 11) M 5 ƒ 2 w, š k» MSi 2 w { w w w screen printing r p t pest x ú.,» 900 C ƒ w»» t SiO 2 y v x j». w» w 2 M 5 x š MSi 2 w wš w, t SiO 2 y v x» w t y wš» w ver glaze wš w. 2. x % M (HM11, Hngb, China) 99.99% Si (Si-9999, Lngfast Silicn, China) w. Screen printablew paste EC(DOW ) w Terpinel (Nippn Terpin ), pe m l p w š, vk p(dbp ) ƒ w x M Si yww ball mill yw w s³j» 2~3 µm w. ƒƒ H 2 w wz

3 Screen Printable MSi 2 Paste w 321» š 550 C SHS(Selfprpagating High-temperature Synthesis) w w, w óù w w y DTA/TG(STA1500, PlymerLab.) Pwder X-ray Diffractmeter w. w óù y azetrpic vehicle yww PL mixer ywwš, N 4 3-rll mill mw yw, g screen printable r p w. w r p 99% alumina» q AlN»q xk z j v q w 1300 C» y wš Silicate glaze wš 800 C 20 w y v x w r w.» ƒw t k w, w y» p. 3. š 3.1. MSi 2 w x w M Si w MSi 2 ƒ Fig. 1 ùkù. M 400 C w 49.76% w ƒƒ ùš. M y w MO 3ƒ q. M 95.9ƒ y g/ml ë ù ƒ 50% ew. MO C ùk, v ùkùš., 900 Cƒ š { MO 3ƒ { w ƒ ùkùš š, 1,000 C { w û kƒ. Fig. 1 v (b) Si, 900 C l ƒƒ ù. Si t y w ù w w. Fig. 1 (c) x w w MSi 2. v M w 400 C w w ƒ ùküš. ƒ 33.20% MSi 2 +7/2O 2 MO 3 +2SiO 2 w ù ƒ 56(7/2O 2 ) 152.1(MSi 2 ) =36.8% w w., Si w 900 C t yƒ ù, MSi 2 yw Fig. 1. Result f DTA/TGA, (a) M, (b) Si, and (c) synthesized MSi 2. Nte that M pwder reacts abut 450 C with weight gain, then near 800 C, due t evapratin, weight lss ccurs. And Si gains weight frm 900 C, with its xidatin, and synthesized MSi 2 gains weight near 450 C, then decmpse arund 800 C, but within the initial weight. w M y w w yƒ w q. z ƒ w û š, MO C vjƒ ùkùš. z M w š, 47«4y(2010)

4 322 ½ Áw Á Table 1. Type f Over Glaze and Their Thermal Prperties Type Tα 1 Tg 2 Tp 3 Ts 4 Tw 5 Clr Silicate A white B white Bi glass C D light pink light pink Zn E white glass 1. Tα : Thermal expansin cefficient ( 10-7 ) 2. Tg : Glass transitin pint ( C) 3. Tp : Yield pint ( C) 4. Ts : Sftening pint ( C) 5. Tw : Wrking pint ( C) z tw. Fig. 2»ü» w w MSi 2 x- z.» š13,14) ù w Fig. 2. Pwder X-ray diffractin pattern f synthesized MSi 2 pwder. (a) withut preheating at ambient atmsphere, (b) purging Ar but n preheating, and (c) with bth preheating and prepurging Ar. Nte that the secnd phase M 5 disappeared after preheating and prepurging H 2 gas. 900 C ù. MO 3ƒ t SiO 2 w { ù» ƒ MSi 2 w MSi 2 r p» w MSi 2 w w. SHS MSi 2 w w» w x mw 2~3 µm ƒ w ùkü q w, 550 Cƒ ƒ w ùkû. MSi 2 w w, w s œ x e k» SHS g. w w ü w w 2 M 5 O 3 ùkùš. XRD detect limit Ÿ (crystallinity) z ƒ ¼ w, 3~5%, 42 y M 5 phase 3% wš š w.» MSi 2ƒ pest x (initiatr) w.»» SHS ww» ü w ƒ M w yw ƒ p ù,» w SHS w l v w w» 2 q Over glaze MSi 2ƒ 900 C š yv x š, yv w pest x w w ƒ w š w, wš w 900 C¾ ƒ š,» v w» MSi 2 z v w ver glaze v w. x verglaze p š, MSi 2 r p w œ r p w. w wz

5 Screen Printable MSi 2 Paste w 323 Fig. 3. Temperature vs. applied vltage f ceramic sheet MSi 2 heater. Fig. 4. Phtgraph f ceramic sheet MSi 2 heater while wrking at ver 500 C. ƒ D E ƒ û w. A, B, C A Bƒ MSi 2, wetting w A B ver glaze kw z x w w w MSi 2 w w MSi 2 r p 99% ù AlN»q screen printer w z ql x g. x z ql 30 leveling w ü rsw œ e k 80 C» 24 g. ƒ óù»q 1,300 C» 2 w. z z ql Ì 15 µm ±1.5 µm. ƒ óù z»q z ql ver glaze wš e 800 C 20 w t yv x g. óù ƒƒ w d w thermcuple w. ƒ ùkü Fig. 3. d ceramic sheet t w thermcuple d w IR d w ƒ ùkù. v MSi 2ƒ ƒ w ƒ. thermcuple d w IR d w ƒ, thermcuple t w û š q., Fig. 4 ùkù MSi 2 Fig. 5. Electrical current and resistivity f MSi 2 ceramic sheet heater with applied vltage. ƒ š. ƒ 600 C q. w x IR d ƒ s³» q. Fig. 5 ƒ y,» w y ùkü. ƒ wš, MSi 2 w ƒ ƒw ƒwš. 500 C pest ƒ ƒ y w ù š 1,3-10)., MSi 2ƒ pest x w x, z þ ƒ t yƒ ù 47«4y(2010)

6 324 ½ Áw Á. ver glazeƒ t y z ùkü w. 4. š ù AlN»q w w. ù»q MSi 2ƒ p wù w þƒ wš q ù ƒ. AlN»q w q šƒ š. w 500 C ƒ ù, þƒ ü ver glazeƒ w q» w ù ƒ ƒ v w.» p w ùk ù t w MSi 2 w ƒ ù ùkü.»» w, ù ƒ d ü z ƒ» ƒw š w. d ü z Ag Ni š, HTCC M/Mn Wƒ š. Agù Ag/Pd q ƒ ù» š, W ù M/Mn w j» w. ù MSi 2ƒ Ag/ Pd w ƒ š, q ƒ š, W ù M/Mn w ƒ û œ ƒ, w ƒ š w MSi 2ƒ û w ƒ xk š w. 5. SHS š MSi 2 w wš w w ù AlN»q z, w» 500æ w w. 1. 2µm~3 µm SHS 550 C» ü Ar H 2» mw M 5 2 w š MSi 2 w w. 2. w MSi 2 w paste w, ù AlN»q w Ì 15 µm ± 1.5 µm z ql w w C, 450 C~550 C y w š š pest x Silicate ver glaze w w. Acknwledgment 2009 w» sƒ (KETEP) ww. REFERENCES 1. Y.-L. Jeng and E.J. Lavernia, Review : Prcessing f Mlybdenum Disilicide, J. Mat. Sci., (1994). 2. J.H. Westbrk and D.L. Wd, PEST Degradatin in Beryllides, Silicides, Aluminides, and Related Cmpunds, J. Nuclear Materials, 12 [2] (1964). 3. Y.Q. Liu, G. Sha, and P. Tsakirpuls, On the Oxidatin Behaviur f MSi 2, Intermetallics, (2001). 4. K. Hassn, M. Halvarssn, J. E. Tang, R. Pmpe, M. Sundberg, and J.-E. Svenssn, Oxidatin Behaviur f a MSi 2 -based Cmpsite in Different Atmspheres in the Lw Temperature Range (400~550 C), J. Eur. Ceram. Sc., (2004). 5. L. Shaw, R. Abbaschian, Chemical State f the Mlybdenum Disilicide(MSi 2 ) Surface, J. Mat. Sci., (1995). 6. K. Kurkawa, H. Huzumi, I. Saeki, and H. Takahashi, Lw Temperature Oxidatin f Fully Dense and Prus MSi 2, Mat. Sci. Eng., A (1999). 7. P.J. Meschter, Lw-temperature Oxidatin f Mlybdenum Disilicide, Metallung. Trans., 23A (1992). 8. D.A. Bertiss, R.R. Cerchiara, E.A. Gulbransen, F.S. Petit, and G.H. Meier, Oxidatin f MSi 2 and Cmparisn with ther Silicide Materials, Mater. Sci. Eng., A (1992). 9. F. Zhang, L. Zhang, A. Shan, and J. Wu, Oxidatin f Stichimetric Ply- and Single Crystalline MSi 2 at 773K, Intermetallics, (2006). 10. P. Feng, X. Wang, Y. He, and Y. Qiang, Effect f High-temperature Prexidatin Treatment n the Lw-temperature Oxidatin Behavir f a MSi 2 based Cmpsite at 500 C, J. Allys and Cmpunds, (2009). 11. C.L. Yeh and W.H. Chen, Cmbustin Synthesis f MSi 2 - M 5 Cmpsite, J. Allys and Cmpunds, (2007). 12. S.-W. J, G.-W. Lee, J.-T. Mn, and Y.-S. Kim, On the Frmatin f MSi 2 by Self-prpagating High-temperature Synthesis, Acta Mater., 44 [11] (1996). 13. I.-H. Sng, J.-Y Yun, and H.-D. Kim, Fabricatin f Prus MSi 2 Material fr Heating Element Thrugh Self-prpagating High Temperature Synthesis Prcess(in Krean), J. Kr. Ceram. Sc., 41 [1] 62-8 (2004). 14. I.-H. Sng, D.-W. Kim, J.-Y Yun, and H.-D. Kim, The Effects f Variatin in Si Cntent n the Prperties f Prus MSi 2 Fabricated by Self-prpagating High Temperature Synthesis Prcess(in Krean), J. Kr. Ceram. Sc., 41 [7] (2004). w wz