Addition of TiO 2 to the HotVeGas Oxide database
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1 Addition of TiO 2 to the HotVeGas Oxide database, Herzogenrath GTT Users Meeting, Herzogenrath Tatjana Jantzen, Klaus Hack
2 Contents of presentation Introduction Binary systems Solid solution phases in ternary systems Cubic Spinel Titania Spinel Pseudobrookite Corundum Conclusions
3 Addition of TiO 2 to GTOX database Binary systems Al-O Ti-O Al-Ti Al 2 O 3 -TiO 2 Al 2 O 3 -Ti 2 O 3 -O 2 MgO-TiO 2 CaO-TiO 2 FeO-TiO 2 -Fe Fe 2 O 3 -TiO 2 -O 2 MnO-TiO 2 -Fe Mn 2 O 3 -TiO 2 -O 2 SiO 2 -TiO 2 Ternary systems Al-O-Ti Al 2 O 3 -MgO-TiO 2 MnO-Mn 2 O 3 -TiO 2 FeO-Fe 2 O 3 -TiO 2 SiO 2 -TiO 2 -Ti 2 O 3 Al 2 O 3 -SiO 2 -TiO 2 Al 2 O 3 -TiO 2 -Ti 2 O 3 MnO-Ti 2 O 3 -TiO 2 MgO-SiO 2 -TiO 2 MgO-TiO 2 -Ti 2 O 3
4 Introduction The associate species were added in order to describe the liquid phase in TiO x - containing systems. The composition of the liquid oxide species are as introduced by Spear taking two moles of cations per associate. Species for similar systems are modelled in the same way, i.e. using the same stoichiometry. System Associate species Used data for Gibbs energy Ti-O Ti (SGPS), Ti 2 O 2*, Ti 2 O 3*, Ti 2 O 4 SGPS database, [99Waldner] Me 2 O 3 -TiO 2 Al 2 TiO 5 Fe 2 TiO 5 MeO-TiO 2 CaTiO 3 FeTiO 3 MgTiO 3*, Mg 2 TiO * 4 MnTiO 3, Mn 2 TiO 4 SGPS SGPS MeO-Ti 2 O 3 MgTi 2 O 4, MnTi 2 O 4 * H f changed in this work.
5 Modelling of ternary systems System Phase Description Used data Al 2 O 3 -MgO-TiO 2 Spinel Pseudobrookite (Al +3,Mg +2,Ti +4 ) 1 (Al +3,Mg +2,Va) 2 (Mg +2, Va) 2 (O -2 ) 4 (Al, Mg,Ti) 1 (Al, Ti) 1 (Ti) 1 (O) 5 Al 2 O 3 -SiO 2 -TiO 2 Pseudobrookite (Al, Ti) 1 (Al, Ti) 1 (Ti) 1 (O) 5 FeO-Fe 2 O 3 -TiO 2 MgO-TiO 2 -Ti 2 O 3 MnO-Mn 2 O 3 -TiO 2 - Ti 2 O 3 Spinel Pseudobrookite Corundum Titania-Spinel Pseudobrookite Corundum Spinel Titania-Spinel Pseudobrookite Corundum (Fe +2,Fe +3,Ti +4 ) 1 (Fe +3,Va) 2 (Fe +2,Va) 2 (O -2 ) 4 (Fe, Ti) 1 (Ti, Fe) 1 (Ti) 1 (O) 5 (Fe +3, Ti +3, Fe 0.5 Ti ) 2 (Va) 1 (O -2 ) 3 (Mg +2,Ti +4 ) 1 (Ti +3,Mg +2,Va) 2 (O -2 ) 4 (Mg, Ti) 1 (Ti) 1 (Ti) 1 (O) 5 (Ti +3,Mg 0.5 Ti ) 2 (Va) 1 (O -2 ) 3 (Mn +2,Ti +4 ) 1 (Mn +2, Mn +3,Mn +4,Va) 2 (Va) 2 (O -2 ) 4 (Mn +2,Ti +4 )(Mn +2, Mn +3, Ti +3,Va) 2 (O -2 ) 4 (Mn, Ti) 1 (Ti) 1 (Ti) 1 (O) 5 (Mn +3, Ti +3,Mn 0.5 Ti ) 2 (Va) 1 (O -2 ) 3
6 Modelling of Ti-containing phases Phase fcc-a1 Description (Al, Ca, Fe, Cr, P, Mg, Mn, S, Si, Zn, Ti, O) (Va) bcc-a2 (Al, Ca, Fe, Cr, P, Mn, S, Zn, Ti, O, TiO 3 ) (Va) 3 hcp-a3 (Al, Ti) 2 (O, Va) Cubic Spinel (Al +3,Cr +2,Cr +3,Fe +2,Fe +3,Mg +2,Mn +2,Zn +2,Ti +4 )(Al +3,Ca +2,Cr +3,Fe +2, Fe +3,Mg +2,Mn +2,Mn +3,Mn +4,Va) 2 (Cr +2, Fe +2, Mg +2,Va) 2 (O -2 ) 4 Titania Spinel (Fe +2,Fe +3,Mg +2,Mn +2,Ti +4 )(Al +3,Fe +2,Fe +3,Mg +2,Mn +2,Mn +3,Va, Ti +3 ) 2 (O -2 ) 4 PSbrookite-Ti 3 O 5 (Al, Mg, Fe, Mn, Ti) 1 (Al,Ti, Fe) 1 (Ti) 1 (O) 5 TIOX (Ti +3, Ti +2, Va) 1 (Ti, Va) 1 (O -2 ) 1 Rutile (Ti +3, Ti +2, Va) 1 (Ti, Va) 1 (O -2 ) 1 Al3M_D022 (Al,Ti) 3 (Ti) TI3AL (Al, Ti) 3 (Al, Ti)(O,Va) 2 TIAL (Al, Ti)(Al, Ti)(O,Va) 2,Ti Ti Ti ,Mn 0.5 Ti +3 Corundum (Al +3,Cr +2,Cr +3,Fe +3,Mn +3, Ti +3,Fe 0.5 Ti ,Mg 0.5 Ti , Mn 0.5 Ti ) 2 ) 2 (Cr +3,Va) 1 (O -2 ) 3 SiO 2 -HT (Si +4,Ti +4 )(Si +4, Ti +4 ) (O -2 ) 4 MeO (Al +3,Ca +2,Cr +3,Fe +2,Fe +3,Mg +2,Mn +2,Mn +3,Ti +4,Ti +3,Zn +2 )(O -2 )
7 Ti-O phase diagram T.B. Massalski (ed), Binary Alloy Phase Diagrams, Second Edition, ASM International, Metals Park, OH Phase Description Used data Slag bcc-a2 hcp-a3 TIOX Rutile Ti 3 O 2, TiO, Ti 2 O 3, Ti 3 O 5, Ti 4 O 7, Ti 5 O 9, Ti 6 O 11, Ti 7 O 13, Ti 8 O 15, Ti 9 O 17,Ti 10 O 19, Ti 20 O 39 (Ti, Ti 2 O 2, Ti 2 O 3, Ti 2 O 4 ) (Ti, O, TiO 3 ) (Va) 3 (Ti) 2 (O, Va) (Ti +3, Ti +2, Va) 1 (Ti, Va) 1 (O -2 ) 1 (Ti) 1 (O, Va) 2 stoichiometric stoichiometric [07Cancarevic] [07Cancarevic] [99Waldner] [99Waldner] [99Waldner]
8 T(C) Al 2 O 3 -TiO 2 phase diagram Al 2 O 3 - TiO 2 1 bar [Pena, De Aza, 1980] [Lejus, Goldberg, 1966] [Boden, Glasser, 1973] 2200 Slag Slag + CORUNDUM Slag + PSBROOKITE Slag + Rutile P. Pena, S. DeAza, Ceramica (Florence), 33 [3], (1980), pp CORUNDUM + PSBROOKITE Rutile + PSBROOKITE 1200 Rutile + CORUNDUM TiO 2 /(Al 2 O 3 +TiO 2 ) (g/g) A.M. Lejus, D. Goldberg, A. Revcolevschi, C.R. Seances Acad. Sci., Ser. C, 263 [20], (1966), pp
9 Calculated Al 2 O 3 -Ti 2 O 3 phase diagram
10 T(C) CaO-TiO 2 phase diagram CaO - TiO 2 1 atm [Tulgar, 1976] 2600 Slag Slag + CaO(s) H.E. Tulgar, Istanbul Tek. Univ. Bul., 29 [1], (1976), pp CaO(s) + Ca 3 Ti 2 O 7 (s) CaTiO 3 (s) Ca 5 Ti 4 O 13 (s) CaTiO 3 (s) + TiO 2 (s) 600 Ca 3 Ti 2 O 7 (s) TiO 2 /(CaO+TiO 2 ) (g/g) A. Jongejan, A.L. Wilkins, J. Less-Comon Met., 20 [4], (1970), pp
11 T(C) Fe 3 O 4 -TiO 2 phase diagram in air 2000 Fe 3 O 4 - TiO 2 - O 2 p(o 2 ) = 0.21 atm, 1 atm 1800 Slag [MacChesney, Muan, 1961] 1600 SPINEL Slag + Rutile 1400 CORUNDUM PSBROOKITE 1200 Rutile + PSBROOKITE wt.% TiO 2 J.B. MacChesney, A. Muan, Am. Mineral, 44 [9-10], (1959), pp
12 T(C) MgO-TiO 2 phase diagram MgO - TiO 2 1 atm 3000 [Shindo, 1980] 2500 [Woermann, Brezny, Muan, 1969] 2000 Slag + MgO Slag Slag + TiO SPINEL + MgO Mg 2 TiO 4 MgTi 2 O 5 PSEUDOBROOKITE E. Woermann, B. Brezny, A. Muan, Am. J. Sci., 267A, (1969), pp SPINEL MgTiO 3 CORUNDUM MgTi 2 O 5 + TiO TiO 2 /(MgO+TiO 2 ) (mol/mol) Phase Description Spinel (Mg +2,Ti +4 )(Mg +2, Va) 2 (Mg +2, Va) 2 (O -2 ) 4 PSbrookite (Mg, Ti) 1 (Ti) 1 (Ti) 1 (O) 5 Corundum (Ti +3, Mg 0.5 Ti ) 2 (Va) 1 (O -2 ) 3 J. Shindo, J. Chryst. Growth, 50 [4], (1980), pp
13 T(C) MnO-TiO 2 phase diagram MnO - TiO 2 - Mn Mn/(MnO+TiO 2 ) (mol/mol) = , 1 atm Slag [Leusmann, 1979] 1600 MeO + Slag Slag + TiO 2 (s) 1400 MeO MeO + SPINEL SPINEL CORUNDUM + TiO 2 (s) CORUNDUM TiO 2 /(MnO+TiO 2 ) (mol/mol)
14 T(C) SiO 2 -TiO 2 phase diagram SiO 2 - TiO 2 1 bar 2500 Slag [Kirillova, 2011] [DeVries, 1954] 2000 Slag + Slag#2 Slag + Rutile 1500 SiO2_HT Slag + Rutile R.C. DeVries, R. Roy, E.F. Osborn, Trans. J. Br. Ceram. Soc., 53 [9], (1954), pp Rutile + SiO2_HT Rutile + SiO 2 (s2) 500 Rutile + SiO 2 (s) TiO 2 /(SiO 2 +TiO 2 ) (mol/mol) R. Roy, R.C. DeVries, D.E. Rase, M.W. Shafer, E.F. Osborn, 1952.
15 Description of the phase Spinel Spinel (Al +3,Cr +2,Cr +3,Fe +2,Fe +3,Mg +2,Mn +2,Zn +2, Ti +4 ) (Al +3,Ca +2,Cr +3,Fe +2,Fe +3,Mg +2, Mn +2,Mn +3,Mn +4,Va) 2 (Cr +2, Fe +2, Mg +2,Va) 2 (O -2 ) 4 Gibbs energies of real Spinels are taken from SGPS database and G of fictive compounds are estimated using reciprocal equations. Mg 2 TiO 4 Fe 2 TiO 4 Mg 2 TiO 4 Fe 2 FeO 4 Al 2 MgO 4
16 T(C) Spinel in Al 2 O 3 -MgO-TiO 2 Spinel solid solution phase with end-members Al 2 MgO 4 and Mg 2 TiO 4 (Al +3,Mg +2,Ti +4 ) 1 (Al +3,Mg +2,Va) 2 (Mg +2, Va) 2 (O -2 ) 4 Mg 2 TiO Al 2 MgO 4 - Mg 2 TiO 4 1 atm [Boden, Glasser, 1973] 1400 [Hauck, 1981] Al 2 MgO SPINEL SPINEL + SPINEL# Mg 2 TiO 4 /(Al 2 MgO 4 +Mg 2 TiO 4 ) (mol/mol) P. Boden, F.P. Glasser, Trans. J. Br. Ceram. Soc., 72[5], (1973), pp
![T(C) Spinel in Al 2 O 3 -MgO-TiO 2 Al 2 MgO 4 - Mg 2 TiO 4 1 atm 1500 [Boden, Glasser, 1973] 1400 [Hauck, 1981] 1300](/docs-images/73/68951106/images/17-0.jpg "SPINEL 1200 1100 Mg 2 TiO 4 1000 SPINEL#1 + SPINEL#2 900 0 0.2 0.4 0.6 0.")
17 T(C) Spinel in Al 2 O 3 -MgO-TiO 2 Al 2 MgO 4 - Mg 2 TiO 4 1 atm 1500 [Boden, Glasser, 1973] 1400 [Hauck, 1981] 1300 SPINEL Mg 2 TiO SPINEL#1 + SPINEL# Mg 2TiO 4/(Al 2MgO 4+Mg 2TiO 4) (mol/mol) Al 2 MgO 4
18 Isothermal section at 1300 o C in FeO-Fe 2 O 3 -TiO 2 A.H. Webster, N.F.H. Bright, J. Am. Ceram. Soc., 44 [3], (1961), pp
19 Liquidus surface in MgO-SiO 2 -TiO 2 F. Massazza, E. Sirchia, Chim. Ind. (Milan), 40 [6], (1958), pp
20 Modelling of Titania Spinel Titania Spinel Ti +3 (Fe +2,Fe +3,Mg +2, Mn +2, Ti +4 ) (Al +3,Fe +2,Fe +3,Mg +2, Mn +2,Mn +3,Ti +3,Va) 2 (O -2 ) 4 40 Gibbs energies Mg 2 TiO 4, MgTi 2 O 4, Mn 2 TiO 4, MnTi 2 O 4, Fe 2 TiO 4 FeTi 2 O 4 does not exist J.-B. Kang, H.-B. Lee, ISIJ Intern., 45 (2005), pp A.D. Pelton, G. Eriksson, D. Krajewski, M.Göbbels, E. Woermann, Z. Phys. Chem., 207 (1998), pp B. Leusmann, N. Jb. Miner. Mh., 12 (1979), pp
21 Isothermal section at 1400 o C in MnO-TiO 2 -Ti 2 O 3 J.-B. Kang, H.-B. Lee, ISIJ Intern., 45 (2005), pp
22 Isothermal section at 1500 o C in MgO-TiO 2 -Ti 2 O 3 A.D. Pelton, G. Eriksson, D. Krajewski, M.Göbbels, E. Woermann, Z. Phys. Chem., 207 (1998), pp
23 Isothermal section at 1200 o C in MnO-TiO 2 -Ti 2 O 3
24 Pseudobrookite in Al 2 O 3 -MgO-TiO 2 Pseudobrookite solid solution phase (Al,Mg,Mn,Fe,Ti) 1 (Al,Fe,Ti) 1 (Ti) 1 (O) 5 with end-members: Ti 3 O 5 Al 2 TiO 5 MgTi 2 O 5 FeTi 2 O 5 Fe 2 TiO 5 P. Boden, F.P. Glasser, Trans. J. Br. Ceram. Soc., 72[5], (1973), pp
25 Isopleth Al 2 TiO 5 -MgTi 2 O 5 in Al 2 O 3 -MgO-TiO 2 P. Boden, F.P. Glasser, Trans. J. Br. Ceram. Soc., 72[5], (1973), pp
26 Isothermal section at 1200 o C in MnO-Ti 2 O 3 -TiO 2 I.E. Grey, C. Li, A.F. Reid, J. Solid State Chem., 17 [4], (1976), pp
27 Delta S(J), kj/mol. K Activity Corundum in FeO-TiO 2 -Fe 2 O 3 Corundum (Al +3,Cr +2,Cr +3,Fe +3,Mn +3, Ti +3, Fe 0.5 Ti ,Mg 0.5 Ti , Mn 0.5 Ti ) 2 (Cr +3,Va) 1 (O -2 ) a(fe 2 O 3 ) <A> FeTiO3 + <1-A> Fe2O3 T = 1300 C [Brown, Navrotsky, 1994]: a(fe 2 O 3 ) a(fetio 3 ) 0.60 a(fetio 3 ) mole fraction FeTiO 3 24 <A> FeTiO3 + <1-A> Fe2O3 T = 1300 C [Brown, Navrotsky, 1994] from measured cation distributions from G mix [Ghiorso,1990] and measured H mix from calculated G mix and measured H mix mole fraction FeTiO 3
28 Corundum in MgO-TiO 2 -Ti 2 O 3 and MnO-TiO 2 -Ti 2 O 3
29 Conclusions The liquid phase in all subsystems was evaluated using associate species model (two cations per species). All systems were assessed using experimental phase diagram information. 12 binaries and 10 ternary systems were described. The 39 stoichiometric phases containing Ti were incorporated. The solubility ranges of 14 solid solution phases containing Titanium were described using available experimental data.
30 Thanks for your attention
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