ࡱ>  % pbjbj%% TGG lJJJJ  KKK$^ ~A!K|KKKAA JJbA A A KJlA KA vA , }4dx04 "4A JJJJZirconium titanate coatings by sol-gel process Jelena Macan Faculty of Chemical Engineering and Technology, University of Zagreb HR-10001 Zagreb, Maruliev trg 19, p.p. 177, Croatia Abstract: Zirconium titanate sols were prepared from zirconium butoxide and titanium isopropoxide. Thin coatings were deposited on glass substrates, and influence of viscosity, alkoxide concentration and drawing speed on appearance of coatings was studied. Crystallization behaviour of amorphous ZrTiO4 powder was studied by X-ray diffraction, combined differential thermal and thermogravimetric analysis and selected area electron diffraction. Change of cell parameters indicates unusual transformation from disordered to ordered structure with increasing temperature of isothermal treatment. Zirconium titanate, ZrTiO4, is a ceramic material with very good thermal and electrical properties, which lead to its widespread use in electronic components and catalysts, and research into suitability for sensors. Sol-gel process enables synthesis of very pure and homogeneous ZrTiO4 ceramic bodies and coatings necessary for these applications. Zirconium butoxide and titanium isopropoxide in stoichiometric 1:1 ratio were dissolved in 2propanol and stabilised with acetylacetone (0.3:1 ratio to alkoxides). Stoichiometric quantity of water for full hydrolysis of alkoxides (4:1 ratio to alkoxides) was added dropwise as 4.64 mol/dm3 nitric acid. Coatings were immediately drawn from the sol on previously cleaned glass substrates with a custom-made dip-coating apparatus and drawing speeds of 0.18 and 0.05 cm/s. Viscosity of sols was modified by dilution with 2propanol, from 8.4 mPas (sol A) to 3.3 mPas (sol B). Due to condensation during 3 hours that coating procedure lasted, the viscosity increased to 91.8 mPas (sol A) and 38.4 mPas (sol B). Each substrate was coated 1-3 times, and coatings were dried at 110C for 1 h after each coating. Coatings from sol A were cracked regardless of drawing speed. Crack-free coatings were obtained from diluted sol B with drawing speed of 0.05 cm/s. Coatings remained crack-free even after the third layer was deposited, enabling preparation of thicker coatings. Since viscosity of sols increased by an order of magnitude during the coating procedure, alkoxide concentration in sols was probably the deciding factor in obtaining crack-free coatings. Sols were left to gel, dried at 110 C and calcined at 500 C to obtain amorphous ZrTiO4 powder, which was characterised by combined differential thermal and thermogravimetric analysis (DTA-TGA). Exothermic reaction at 703C was ascribed to crystallization of orthorhombic ZrTiO4, and for confirmation amorphous ZrTiO4 powder was isothermally treated at several temperatures in 6001000 C range for 2 h and analysed by X-ray diffraction analysis (XRD) and selected area electron diffraction (SAED). First appearance of crystalline ZrTiO4 is detected at 635 C by XRD (Fig. 1) and at 620 C by SAED (Fig. 2), which is more sensitive to presence of very small crystallites. Cell parameters were determined from peak positions of fully crystallized samples calcined at 900-1400 C temperature range for 8 h. Change of cell parameters between 1100 and 1200 C is characteristic of disorder-order transition, the opposite of usual order-disorder transition at that temperature. Since ZrTiO4 prepared by sol-gel process initially crystallizes in disordered state, increased ordering is probably caused by prolonged treatment at high temperatures.    EMBED Origin50.Graph  Fig. 1 - XRD spectra of ZrTiO4 powders calcined at listed temperatures Fig 2 - SAED pattern of ZrTiO4 powder calcined at 620 C zp#$& ' { % ; hikl+, PQopɺH*jL CJUVaJmH sH  jUjCJUmHnHsH ujCJUmHnHsH u CJH*\CJ\CJH* 5CJ\CJ5CJmH sH 5CJmH sH *^`znp f Q23mnop$a$$a$$`a$ $&dPa$$da$$a$o,1h. 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x) yO y` zA z; { |G |V }E }) ~; ~- E  O  ; T 7  = E T 1 1 K T 3 = 7 = 1 = G = K & ) & A 7 - G A T = ) O E 3 T  E 1 G G T V 3 ) = ; O ; - T 3  " E 1 = 3 Z - ; G G A 3 1 " & =  1 3 3 1 - G " ; K & ) " A & 7 E ) & G  V 7 - T ; ` ; O - ; E ) E ; E G A 3 = 3 E G ) Z & - E O G & ; = ; 7 ; T 1 A 1 \ 3 K ; 7 " = O  3 ;  A ; A K 3 O   O G O E G = ) K = - O G  ; A 1 E Q ; Q T G  b T = & ; - ) " ; G ) b E -  3 G 3 7 G Q 3 1 - ; 3 & 1 K E E T 3 Q A \ E ; Z 1 G = & = - ; ) A = O Q E T 3 3 = - ; T & T 7 T G A E K K "  Z O \ O E O - E f j G K T ; 1 = 7  E 7 Z - ;  G = T E 1 1 = - = E = 3 h E Z E - ) O V !1 !E "O #E #; $G $E %3 %O &3 &G '` 'O (Q )Z )G *Z * +` +; ,A -Q -E .= /E 0) 0K 1) 1A 2E 2T 3; 3T 47 5f 5E 6& 6G 7= 7- 8; 8E 9O 9\ := ;A ;= <3 <Q =O =E >; >T ?Q ?1 @E AQ AT Bn B3 CE DT D= EO E- FO GO G= HK |%HK Hn I= IO JV J\ K1 KQ L7 MO M3 N; N\ O= OV PV PT Q\ Q7 R& SG Sh T" T- UE UT VE VQ WE W& XZ Y7 YG ZE Zj [G [V \A \f ]3 ]` ^) _= `G `K aO aZ bQ b; c3 cT dG eG eE fT fA gG gA h= hE iG ib jV kf lG lZ m; 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