将Miedema模型与实验数据相结合得到适于Miedema模型的O和S的参数(O:电负性7.04、电子密度6.03、摩尔体积4.59;S:电负性5.8、电子密度3.24、摩尔体积6.97),计算了141种O的二元化合物和145种S的二元化合物生成焓其平均绝对误差(MAPE)分别为36.8%、32.4%.结合Ding导出的三元系相互作用系数计算模型,计算了1873 K时Fe基熔体中O和S与其它元素之间的相互作用系数.与实验数据的比较表明,除个别元素外,计算值与实验值之间误差不大且变化趋势比较一致.将误差较大的Nb、Ag、Pt的电负性参数由原来的4.05、4.35、5.65修正为4.31、4.17、5.57,使用Miedema模型的计算精度有很大的提高.
参考文献
[1] | J.In-Ho,Sergei A.Decterov,A thermodynamic model for deoxidation equilibria in steel,Metall.Mater.Trans.B,35B,493(2004) |
[2] | Y.Shinya,K.Yoichi,K.Zensaku,Activity coefficient of oxygen in copper-tellurium melts,Metall.Trans.B,17B,171(1986) |
[3] | O.Shinya,K.Zenzaku,Thermodynamic study of oxygen in liquid elements of group Ib to VIb,Transactions of the Japan Institute of Metals,22(8),558(1981) |
[4] | Jean L,Michele N.Interactions between metal and slag melts:Steel desulfurization,Metall.Mater.Trans.B,73,493(2011) |
[5] | CHEN Xingqiu,YAN Xinlin,DING Xueyong,Enthalpies ofpormation for compounds:a century and comes of age for density functional based computations,Journal of Rare Earths,22,1 (2004)(陈星秋,严新林,丁学勇,化合物生成焓:一百年和密度泛函基量子机制的原子模型新时代,中国稀土学报,22,1(2004)) |
[6] | DING Xueyong,FAN Peng,LUO Lihua,AlloyMelts Thermodynamic Model,Prediction and Software Development (Shenyang,Northeastern University Press,1998)p.30(丁学勇,范鹏,罗利华,合金熔体热力学模型、预测值及其软件开发(沈阳,东北大学出版社,1998)p.30) |
[7] | X.Y.Ding,P.Fan,W.Wang,Thermodynamic calculation for alloy systems,Metall.Mater.Trans.B,30B,271 (1999) |
[8] | F.R.de Boer,R.Boom,W.C.M.Matttens,Cohesion in Metals:Transition Metal Alloys (Netherlands,North-Holland Physics Publishing,1989) |
[9] | Xing-Qiu Chen,R.Podloucky,Miedema' s model revised:The Parameters Φ* for Ti,Zr,and Hf,Computer Coupling of Phase Diagram and Thermochemistry,Calphad,30,266(2006) |
[10] | J.Neuhausen,B.Eichler,Extension ofMiedema's macroscopic atom model to the elements of group 16(O,S,Se,Te,Po),Paul Scherrer Institut,2003 |
[11] | Mitsutaka Hino,Kimihisa Ito,Thermodynamic Data for Steelmaking (Japan,Tohoku Printing Co.Ltd,2010) |
[12] | S.P.Sun,D.Q.Yi,Y.Jiang,An improved atomic size factor used in Miedema' s model for binary transition metal systems,Chem.Phys.Lett.,513,149(2011) |
[13] | A.R.Miedema,On the heat of formation of solid alloys Ⅱ,Journal of the Less-Common Metals,46,67(1976) |
[14] | S.V.Meschel,X.Q.Chen,O.J Kleppa,Philip Nash,The standard enthalpies of formation of some intermetallic compounds of early 4d and 5d transition metals by high temperature direct synthesis calorimetry,Calphad,33,55(2009) |
[15] | X.Q.Chen,W.Wolf,R.Podloucky,P.Rogl,Comment on "Enthalpies of formation binary Laves phases",Intermetallics,12,59(2004) |
[16] | Jerome Assal,Bengt Hallstedt,Ludwig J.Gauckler,Thermodynamic assessment of the silver-oxygen system,J.Am.Ceram.Soc.,80(12),3054(1997) |
[17] | Ihsan· Barron,Translated by CHENG Nailiang,NIU Sitong,XU Guiying,Thermochemical Data of Pure Substances (Beijng,Science Press,2003)(伊赫桑·巴伦著,程乃良,牛四通,徐桂英译,纯物质热化学数据手册(北京,科学出版社,2003)) |
[18] | P.A.G.O'Hare,G.K.Johnson,Thermochemistry of inorganic sulfur compounds Ⅶ.Standard molar enthalpy of formation at 298.15K,high-temperature enthalpy increments,and other thermodynamic properties to 1100K of titanium disulfide,TiS2,The Journal of Chemical Thermodynamics,18(2),189(1986) |
[19] | Herve Toulhoat,Pascal Raybaud,Slavik Kasztelan,et al.Tansition metals to sulfur binding energies relationship to catalytic activities in HDS:back to Sabatier with first principle calculations,Catalysis Today,50(3-4),629(1999) |
[20] | Suraj Deore,Alexandra Navrotsky.Oxide melt solution calorimetry of sulphides:Enthalpy of formation of sphalerite,galena,greenockite,and hawleyite,Am.Mineral,91,400(2006) |
[21] | A.Zubkov,T.Fujino,N.Sato,K.Yamada,Enthalpies of formationof the palladium sulphides,The Journal of Chemical Thermodynamics,30(5),571(1998) |
[22] | C.Toffolon,C.Servant,Thermodynamic assessment of the Fe-Nb System,Calphad,24(2),97(2000) |
[23] | S.V.Meschel,O.J.Kleppa,The standard enthalpies of formation of some intermetallic compounds of transition metals by high temperature direct synthesis calorimetry,J.Alloys Compd.,415,143(2006) |
[24] | A.Bolcavage,U.R.Kattner,A reassessment of the calculated NiNb phase diagram,Journal of Phase Equilibria,17(2),92(1996) |
[25] | Letitia Topor,O.J.Kleppa,Standard enthalpies of formation of PtTi,PtZr,and PtHf,Metall.Trans.A,19A,1827(1988) |
[26] | Q.T.Guo,O.J.Kleppa,Standard enthalpies of formation of Ni3V,Ni3Hf,Pd3Hf,and Pt3Sc and systematics of ΔHfo for Ni3Me (Me=La,Hf,Ta),Pd3Me(Me=La,Hf,Ta),and Pt3Me (Me=Sc,Ti,V or Y,Zr,Nb) alloys,J.Phys.Chem.,99,2854(1995) |
[27] | Q.T.Guo,O.J.Kleppa,Standard enthalpies of formation of some holmium alloys,Ho + Me (Me=Ni,Ru,Pd,Ir,Pt),determined by high temperature direct synthesis calorimetry,J.Alloys Compd.,234,280(1996) |
[28] | J.H.Zhu,C.T.Liu,L.M.Pike,P.K.Liaw,Enthalpies of formation of binary Laves phases,Intermetallics,10,579(2002) |
[29] | K.Fitzner,W.G.Jung,O.J.Kleppa,Thermochemistry of binary alloys of transition metals:the Me-Sc,Me-Y,and Me-La (Me=Ag,Au) systems,Metall.Trans.A,22A,1103(1991) |
[30] | S.V.Meschel,O.J.Kleppa,Thermochemistry of some binary alloys of Samarium with the noble metals(Cu,Ag,Au) by high temperature direct synthesis calorimetry,J.Alloys Compd.,416,93(2006) |
[31] | S.V.Meschel,O.J.Kleppa,Thermochemistry of some binary alloys of silver with the lanthanide metals by high temperature direct synthesis calorimetry,J.Alloys Compd.,376,73(2004) |
[32] | Q.T.Guo,O.J.Kleppa,Standard enthalpies of formation of Ni3Ta,Pd3Ta,Pt3Nb,Pt3V,Pt3V by high-temperature direct synthesis calorimetry,J.Alloys Compd.,205,63(1994) |
[33] | Q.T.Guo,O.J.Kleppa,Standard enthalpies of formation of terbium alloys,Tb+Me (Me=Ni,Ru,Rh,Pd,lr,Pt),by high-temperature direct synthesis calorimetry,J.Alloys Compd.,221,50(1995) |
[34] | S.V.Meschel,O.J.Kleppa,Standard enthalpies of formation of some 3d,4d and 5d transition-metal stannides by direct synthesis calorimetry,Thermochimica Acta,314,205(1998) |
[35] | N.Selhaoui,O.J.Kleppa,Standard enthalpies of formation of scandium alloys,Sc+Me (Me=Fe,Co,Ni,Ru,Rh,Pd,Ir,Pt),by hightemperature calorimetry,J.Alloys Compd.,191,155(1993) |
[36] | N Selhaoui,O.J.Kleppa,Standard enthalpies of formation of scandium alloys,Sc+Me (Me=Fe,Co,Ni,Ru,Rh,Pd,Ir,Pt),by hightemperature calorimetry,J.Alloys Compd.,191,145(1993) |
[37] | Q.T.Guo,O.J.Kleppa,Standard enthalpies of formation of terbium alloys,Tb+Me (Me=Ni,Ru,Rh,Pd,Ir,Pt),by high-temperature direct synthesis calorimetry,J.Alloys Compd.,221,45(1995) |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%