• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    Al-Fe-P三元系的熱力學(xué)優(yōu)化

    2013-10-18 05:27:14曹戰(zhàn)民王昆鵬牛春菊杜廣巍喬芝郁
    物理化學(xué)學(xué)報(bào) 2013年1期
    關(guān)鍵詞:北京科技大學(xué)材料科學(xué)工程學(xué)院

    曹戰(zhàn)民 謝 偉 王昆鵬 牛春菊 杜廣巍 喬芝郁

    (1北京科技大學(xué)鋼鐵冶金新技術(shù)國家重點(diǎn)實(shí)驗(yàn)室,冶金與生態(tài)工程學(xué)院,北京 100083;2北京科技大學(xué)材料科學(xué)與工程學(xué)院,北京 100083)

    1 Introduction

    Phosphorus has known to be an essential metalloid element in forming an amorphous phase exhibiting useful engineering properties,such as,the Invar effect,1corrosion resistance,2and catalysis.3The Al-Fe-P ternary system has drawn more and more attention due to that amorphous phase formation has been found in the Al-Fe-P system by using a melt-spinning technique.4The evaluation of the glass-forming ability(GFA)of alloys is of great importance by judging in advance whether amorphous phases could be formed at given conditions.The successful evaluation5-7of GFA of some alloys indicates that the expressions of the Gibbs energies of the phases are very powerful in qualitatively analyzing the composition dependency of the GFA.The Al-Fe-P system is also a fundamental ternary system of the Fe-based and P-containing multi-component alloys,which are very important for the advanced metallurgy and materials.Knowledge of the thermodynamic properties of the Al-Fe-P system is significant for the development of Fe-based and P-containing multi-component alloys by providing information regarding the phases that are present at service temperature,their compositions and volume fractions and so on.Therefore,the interest in this system is increasing,as shown by a recent publication,8in which,however,the researchers only gave a description of the Fe rich side and merely accounted for one isothermal section at 723 K during the calculation.

    Thus,our study was aimed to give a thermodynamic optimization of the Al-Fe-P system over the whole composition range based on all available experimental information in the literature by using CALPHAD(CALculation of PHAse Diagram)approach with Thermo-Calc software package.9The optimized self-consistent thermodynamic parameters of the Al-Fe-P system are expected to be helpful for both the better understanding of the composition dependency of the GFA in the Al-Fe-P system and the development of the Fe-based and P-containing multi-component alloy thermodynamic database.

    2 Information on the binary and the ternary systems

    2.1 Al-P system

    The Al-P system was extensively investigated by many researchers.White et al.10released the existence of only one intermediate phase,AlP,which was further confirmed by Panish and Ilegems11,12during the study of the Ga-rich corner of the Ga-Al-P ternary system.Tu et al.13confirmed the existence of AlP again in the investigation of the 723 K isothermal section of the Al-P-Zn ternary system with the help of combined techniques of optical microscopy,scanning electron microscopy coupled with energy dispersive X-ray spectroscopy(SEMEDS),and X-ray diffraction(XRD).Kischio14reported the melting point of AlP to be(2803±50)K without experimental detail.Czochrallski15established a possible upper limit to the solubility of P in γ-Al of 0.0007 at mole fraction of P.

    Several researchers experimentally measured the heat of formation of AlP using different methods and large difference existed among the experimental results.Kischio14obtained ΔfH295K(AlP)=(-82630±1050)J·mol-1·atom-1from the heat of dissolution of AlP in aqueous HCl and the known formation of the products.Wang and Zaheervuddin16measured the heats of combustion of AlP and equal mol mixtures of Al and red P.Adjusting their results to white P as reference state,ΔfH298K(AlP)=(-69500±4600)J·mol-1·atom-1was obtained.Maria et al.17measured the partial pressures of Al and P2vapor equilibrium with AlP,from 1270 to 1800 K using the Knudsen effusion method in combination with mass spectrometry,and ΔfH298K(AlP)=(-59000±6700)J·mol-1·atom-1was obtained.A second law fit to Maria′s experimental results17was carried out by McAlister18and ΔfH298K(AlP)=(-57600±17700)J·mol-1·atom-1with statistical error was yielded.Martosudirdjo and Pratt19reported ΔfH(AlP)=(-74000±900)J·mol-1·atom-1using precipitation calorimetry in liquid Sn at 582 K.

    Tu et al.13gave a description of the Al-P binary system during the thermodynamic analysis of the Al-P-Zn ternary system.Unfortunately,their description could not reflect the phase relation of AlP with other phases correctly when extrapolating the parameters into the Al-Fe-P ternary system.Therefore,the thermodynamic parameters of the Al-P system were re-optimized in this work.

    2.2 Al-Fe and Fe-P binary systems

    In the Al-Fe system the equilibrium phases are the liquid,the α-Fe solid solution based on body-centered cubic(bcc)Fe,the γ-Fe solid solution based on face-centered cubic(fcc)Fe,the AlFe formed through ordering of α-Fe,Al13Fe4,Al5Fe2,Al2Fe,Al5Fe4,and the γ-Al based on fcc Al.Many researchers,including Kaufman and Nesor,20Saunders and Rivlin21and Seierstein22,optimized the Al-Fe binary system.The assessment by Seierstein22is the first consistent description of the Al-Fe phase diagram and has been successfully extrapolated to the related ternary system by many researchers.23-25Thus,the parameters optimized by Seierstein22have been adopted in present assessment,except that the thermodynamic parameters of Al2Fe phase have been slightly modified to ensure the Al2Fe phase be stable in the Al-Fe-P ternary system.The optimized parameters are shown in Table 1,and the calculated Al-Fe phase diagram is shown in Fig.1(a).

    The Fe-P system is composed of the liquid,the α-Fe solid solution based on bcc Fe,the γ-Fe solid solution based on fcc Fe,Fe3P,Fe2P,FeP,FeP2,FeP4,and P(red and white P).A critical assessment of the Fe-P system has been carried out by Okamoto,26Ohtani27and Tokunaga28et al.However,in all these evaluations the valuable thermodynamic properties in the Fe-P system measured by Zaitsev et al.29using differential scanning calorimetry and Knudsen effusion method with mass-spectrometric analysis of the gaseous phase were omitted.Most recently,a thermodynamic re-optimization of the Fe-P system has been carried out by Cao et al.,30and satisfactorily reproduced most experimental phase diagram and thermodynamic properties.Hence,the parameters assessed by Cao et al.30with minor modification were used in present work.The modified parameters and calculated phase diagram of Fe-P system are shown in Table 1 and Fig.1b,respectively.

    2.3 Al-Fe-P ternary system

    Because of the high volatilization of P,the Al-Fe-P ternary phase diagram has been studied only for the Fe rich corner of this system.Vogel and Klose31studied the phase equilibria in the Fe-Fe2P-AlP-Fe50Al50region of the Al-Fe-P ternary system using differential thermal analysis(DTA)and metallographyanalysis.The vertical sections of w(P)=6%,9%(mass fraction)and w(Al)=10%,25%were determined.The isothermal section at room temperature and the liquidus surface in the Fe-Fe2PAlP-Fe50Al50region were also investigated experimentally.There was found that the AlP-Fe2P and AlP-Fe50Al50sections are the quasi-binaries of the simple eutectic type.Kaneko et al.32investigated the phase relationships between phosphide-phase and iron-phase in the Al-Fe-P system by chemical and X-ray examinations and the obtained results agree with those reported by Vogel and Klose.31Limited thermodynamic properties relevant to the Al-Fe-P system are reported.Yamada and Kato33,34determined the activity interaction coefficients of phosphorus in the Fe-P-i system at 1873 K using a Knudsen cell-mass spectrometer combination with the computation from the ratio of the intensities of P+and Fe+peaks,and=4.6±0.7 was obtained.Based on the Miedema model and Toop equation Ding et al.35thermodynamically predicted the activity interaction coefficients between alloying elements and P in liquid Fe at 1873 K and the value of predictedis 8.78,which is much larger than the measured mentioned above.On the basis of the above mentioned information,the phase equilibria in the Al-Fe-P ternary system were reviewed in references.36-38

    Table 1 Optimized thermodynamic parameters for the binary and ternary systems

    Most recently,Wu et al.8investigated the phase equilibrium in the Al-Fe-P system when the P content was below 20%(mass fraction)with SEM-EDS and XRD and released an isothermal section at 723 K of the Al-Fe-P system at low phosphorus contents.And up to now,no ternary phase has been found in this ternary system.

    3 Thermodynamic models

    The thermodynamic models adopted here for the phases of the Al-Fe-P system are summarized in Table 1 and briefly introduced below.

    3.1 Pure elements

    3.2 Solution phases

    The solution phases are modeled by the substitutional solution model and their Gibbs energies are described by the following expression:

    where the three terms assume different forms according to the nature of the phase.Substitutional solutions are represented by only one sublattice where all the atoms mix randomly.In the binary case(A,B)1,the three contributions to the Gibbs energy are:

    Fig.1 Calculated binary phase diagrams

    In the case of ternary solutions,the expressions ofrefGφandare easily derived from the binary ones.As for the excess Gibbs energy,it is obtained by combing the binary excess Gibbs energies according to the Muggianu extrapolation formula40and adding a ternary excess term:

    and the L functions have the form shown in Eq.(4).

    This model has been adopted for the following phases:liquid,α,γ,and Al5Fe4(see Table 1).

    3.3 Ordered/disordered phases

    The ordered AlFe phase with bcc_B2 structure is modeled as(Al,Fe)0.5(Al,Fe)0.5in the Al-Fe system.22In order to represent the Gibbs energy of the ordered/disordered transitions using a single function,the disordered α-Fe phase with bcc_A2 structure is described by(Al,Fe)1.Ansara et al.41,42have derived an equation which allows the thermodynamic properties of the disordered phase to be evaluated independently.This is done by resolving the Gibbs energy into three terms as following:

    in which yi′is the site fraction of i(i=Al and Fe)in the first sublattice,and yi″in the second one.(xi)is the Gibbs energy of the disordered α-Fe phase.The second term(yi′,yi″)is described by the sublattice model and implicitly contains a contribution from the disordered state.The last term(xi)represents the contribution from the disordered state to the ordered one.When the site fractions are equal,i.e.yi′=yi″,the last two terms cancel each other.The ordered AlFe phase with bcc_B2 structure and the disordered α-Fe phase with bcc_A2 structure are modeled as(Al,Fe,P)0.5(Al,Fe,P)0.5and(Al,Fe,P)1in the Al-Fe-P ternary system,respectively.Due to lack of the experimental information on the ordered/disordered transition in the Al-Fe-P ternary system the ternary interaction parameters are assumed to be zero.

    3.4 Intermetallic compounds

    Stoichiometric compounds are represented with as many sublattices as the number of component elements,with only one atom type in each sublattice.In the binary case the model is(A)u(B)1-uand the Gibbs energies are given by

    The Eq.(7)was adopted to describe the Gibbs energies of the stoichiometric compounds that were lack of heat capacity data:Al5Fe2,Al2Fe,FeP2,FeP4,and AlP(see Table 1).

    For Fe3P,Fe2P,and FeP phases,the heat capacity data are available in a wide temperature range29and their Gibbs energies are given by

    Table 2 Lattice stability parameters used in the present optimization39

    where ΔfH298Kand S298Kare the enthalpy of formation and the entropy at 298 K,and Cpis the heat capacities at constant pressure.

    In Seierstein′s study,22non-stoichiometric compound,Al13Fe4,was modeled with three sublattices:(Al)0.6275(Fe)0.235(Al,Va)0.1375in order to account for its binary solubility range.The Gibbs energy is given by

    where the superscript?denotes the third sublattice of the presented model,is the site fraction of i in the third sublattice,Va is the vacancy in the third sublattice.andare the Gibbs energy of the two end members(Al)0.6275(Fe)0.235(Al)0.1375and(Al)0.6275(Fe)0.235(Va)0.1375.

    No ternary intermetallic compounds have been reported in previous study and all binary intermetallic phases were treated to have zero ternary solubility in the Al-Fe-P system in present work.

    4 Optimization results and discussion

    The binary and ternary interaction parameters have been optimized using the PARROT module included in the Thermo-Calc software package.9The phase diagram data and experimental thermodynamic information were used as the input to the program.Each datum value was given a certain weight by our personal evaluation of the datum source and considering the consistency between the phase diagram and the thermodynamic properties.The interaction parameters have been evaluated by trial and error method during the course of the optimization until most of the selected experimental information is reproduced within the expected uncertainty limits.As a result,a complete list of the thermodynamic parameters describing the Al-Fe-P system is summarized in Table 1.Computed phase equilibria are compared to the selected experimental information reviewed in Sections 2.1 and 2.3.And a brief discussion is given as below.

    4.1 Al-P binary system

    The calculated phase diagram of Al-P system is shown in Fig.1(c).The evaluated melting point of AlP is 2803 K,which agrees well with the experimental value(2803±50)K.14As mentioned in Section 2.1,there are large differences among the experimental values of enthalpy formation of AlP determined by different researchers.The calculated ΔfH298K(AlP)=-74.0 kJ·mol-1·atom-1,is close to the value measured by Wang and Zaheervuddin.16

    4.2 Al-Fe-P ternary system

    By using the present optimized parameters of the Al-P system along with the reported parameters of the Al-Fe22and Fe-P30systems,and based on the vertical section and isothermal section diagram information,the Al-Fe-P ternary system is further optimized.The parameters of the Al-Fe and Fe-P system were slightly modified in order to fit the experimental data better.

    Fig.2 (a)Isothermal section diagram of the Al-Fe-P system at room temperature determined by Vogel and Klose31 and redrawn by Schmid-Fetzer and Tomashik38 and(b)calculated isothermal section diagram at room temperature in this work

    Fig.3 Calculated vertical section diagrams compared with the experimental data31

    The experimental and calculated isothermal section diagrams at room temperature are shown in Fig.2.It is easy to see that most of the phase relations have been well reproduced.The representative calculated vertical section diagrams with experimental data are illustrated in Fig.3.Although there is,in general,a satisfactory agreement between the experimental data reported by Vogel and Klose31for the phase diagram,some differences still exist,e.g.a relative discrepancy on the liquidus line between the calculated and the experimental data was observed.Actually,great care has been taken to reduce these discrepancies in our assessment,but it was found that it is difficult to fit these experimental data very well.It is still necessary to get more new experimental data to solve this problem.Additionally,some of the equilibria with respect to the bcc phase are inconsistent with the measured vertical sections by Vogel and Klose,31e.g.in our assessment,bcc phase is respectively in equilibrium with Fe2P and liq+Fe2P in the dashed regions,as shown in Fig.3(d),rather than AlP and liq+AlP reported by Vogel and Klose.31

    It was worthy to point out that we calculated the isothermal section diagram of the Al-Fe-P system at 723 K and compared with the latest experimental data,8which was published after the present assessment had been finished,and a good agreement between them was obtained,as shown in Fig.4.It proved that the thermodynamic parameters gained in our optimization are reliable.

    Fig.4 Calculated isothermal section diagram of the Al-Fe-P system at 723 K compared with the experimental data8

    Fig.5 Calculated liquidus projection of the Al-Fe-P system

    Table 3 Present calculated values for the invariant reactions in the Al-Fe-P system with the experimental data31

    Taking into account the available information on the binary and ternary systems,the complete liquidus projection for the whole Al-Fe-P system are illustrated in Fig.5.The calculated and experimental invariant temperatures and the corresponding compositions for the various invariant reactions are summarized in Table 3.Although the temperatures are generally in good agreement with the experimental values,there are still some differences in the compositions.Invariant reactions E7 and E8 are very near to the binary subsystems,so these two invariant reactions cannot be visible in Fig.5.Necessary experiments are also needed to validate the liquidus projection in the Al-Fe-P system.

    5 Explanation on the glass-forming ability

    Fig.6 Calculated driving force(DF)surface projection at 973 K superimposed with iso-DF lines and the experimental glass compositions denoted by Inoue4

    The driving force(DF)criterion5,6is based on the assumption that the phase having the highest driving force is most like-ly to form first.Considering that the formation of an amorphous phase would be favored when the nucleation and growth of crystalline phases are retarded,then the composition with the highest glass-forming ability can be the one with the lowest driving force of formation of crystalline phases.In order to analyze the composition dependency of the glass-forming ability,the initial crystallization driving force,which can be regarded as a representation of the nucleation ability of the crystalline phases,was employed in this work.The initial driving forces of all crystalline phases under every specified liquid composition at 973 K were first calculated and then the maximal values under each composition were chosen to construct the DF surface projection,as shown in Fig.6.Iso-DF lines and the experimental glass compositions are superimposed on it.All the experimental data are in the region where the driving forces are lower than 0.9.This is in accordance with the driving force criterion:alloys having lower driving forces possess higher glassforming abilities.This proves that the driving force criterion can be used as an index to predict the composition field most likely having the best glass-forming ability before any experiments.

    6 Conclusions

    Based on the available experimental information on the Al-P and the Al-Fe-P systems as well as the published assessment of the Al-Fe and the Fe-P binary systems,a critical assessment of the Al-P binary and the Al-Fe-P ternary system was carried out and a consistent thermodynamic description for describing all the phases in the Al-Fe-P system was obtained.The phase diagrams of the Al-Fe-P system over the entire composition range,including the vertical sections for w(P)=6%,9%,and w(Al)=10%,25%,the isothermal section at room temperature as well as the liquidus projection was constructed from present thermodynamic calculation.Most reported compositions of amorphous phase lie in the regions with low initial driving forces for the crystalline phases,which soundly proves the reasonability and reliability of the present thermodynamic description.

    (1)Fukamichi,K.;Kikuchi,M.;Hiroyoshi,H.;Masumoto,T.Anomalous Thermal Expansion,ΔE Effect,Invar and Elinvar Characteristics of Some Fe-based Amorphous Alloys.In Rapidly Quenched Metals III;Cantor,B.Ed.;The Metals Society:London,1978.

    (2)Masumoto,T.;Hashimoto,K.;Naka,M.Corrosion Behavior of Amorphous Metals.In Ra pidly Quench ed Metals III;Cantor,B.Ed.;The Metals Society:London,1978.

    (3)Yokoyama,A.;Komiyama,H.;Inoue,H.;Masumoto,T.;Kimura,H.M.S cripta Met.1981,15,365.

    (4)Inoue,A.;Kitamura,A.;Masumoto,T.Mater.Sci.1983,18,753.doi:10.1007/BF00745573

    (5)Kim,D.;Lee,B.J.;Kim,N.J.Intermetallics 2004,12,1103.doi:10.1016/j.intermet.2004.04.001

    (6)Kim,D.;Lee,B.J.;Kim,N.J.Scripta Mater.2005,52,969.doi:10.1016/j.scriptamat.2005.01.038

    (7)Bo,H.;Wang,J.;Jin,S.;Qi,H.Y.;Yuan,X.L.;Liu,L.B.;Jin,Z.P.Intermetallics 2010,18,2322.doi:10.1016/j.intermet.2010.08.002

    (8)Wu,C.J.;Huang,W.M.;Su,X.P.;Peng,H.P.;Wang,J.H.;Liu,Y.CAL PH AD 2012,38,1.doi:10.1016/j.calphad.2012.03.005

    (9)Sundman,B.;Jansson,B.;Andersson,J.O.CALPHAD 1985,9,153.doi:10.1016/0364-5916(85)90021-5

    (10)White,W.E.;Bushey,A.H.J.Am.Chem.Soc.1944,66,1666.doi:10.1021/ja01238a018

    (11)Panish,M.B.;Ilegems,M.Prog.S olid State Chem.1972,7,39.doi:10.1016/0079-6786(72)90004-0

    (12)Ilegems,M.;Panish,M.B.Crys.Growth 1973,20,77.doi:10.1016/0022-0248(73)90117-6

    (13)Tu,H.;Yin,F.C.;Su,X.P.;Liu,Y.;Wang,X.M.C ALP H AD 2009,33,755.doi:10.1016/j.calphad.2009.10.003

    (15)Czochrallski,J.Z.Metallkd.1923,15,273.

    (16)Wang,C.C.;Zaheervuddin,M.Inorg.Nucl.Ch em.1963,25,326.doi:10.1016/0022-1902(63)80071-8

    (17)de Maria,G.;Gingerich,K.A.;Piacente,V.Chem.Phys.1968,49,4705.

    (18)McAlister,A.J.Alloy P hase Diagrams 1985,6(3),222.doi:10.1007/BF02880402

    (19)Martosudirdjo,S.;Pratt,J.N.T h ermochim.A cta 1974,10,23.doi:10.1016/0040-6031(74)85019-7

    (20)Kaufman,L.;Nesor,H.CA LPHA D 1978,2,325.doi:10.1016/0364-5916(78)90020-2

    (21)Saunders,N.;Rivlin,V.G.Z.Metallkd.1987,78,795.

    (22)Seierstein,M.The Al-Fe System.In COST 507,T hermoch emical Database for Light Metal Alloys;Ansara,I.,Dinsdale,A.T.,Rand,M.H.Eds.;Office for Official Publications of the European Communities:Luxembourg,1998.

    (23)Zhang,L.J.;Du,Y.CAL PHAD 2007,31,529.doi:10.1016/j.calphad.2007.03.003

    (24)Du,Y.;Schuster,J.C.;Liu,Z.K.;Hu,R.X.;Nash,P.;Sun,W.H.;Zhang,W.W.;Wang,J.;Zhang,L.J.;Tang,C.Y.;Zhu,Z.J.;Liu,S.H.;Ouyang,Y.F.;Zhang,W.Q.;Krendelsberger,N.Intermetallics 2008,16(4),554.doi:10.1016/j.intermet.2008.01.003

    (25)Guo,C.P.;Du,Z.M.;Li,C.R.;Zhang,B.L.;Tao,M.C ALP H AD 2008,32,637.doi:10.1016/j.calphad.2008.08.007

    (26)Okamoto,H.B ull.Alloy Phase Diagrams 1990,11,404.doi:10.1007/BF02843320

    (27)Ohtani,H.;Hanaya,N.;Hasebe,M.;Teraoka,S.;Abe,M.C ALP H AD 2006,30,147.doi:10.1016/j.calphad.2005.09.006

    (28)Tokunaga,T.;Hanaya,N.;Ohtani,H.;Hasebe,M.ISIJ International 2009,49(7),947.doi:10.2355/isijinternational.49.947

    (29)Zaitsev,A.I.;Dobrokhotova,Z.V.;Litvina,A.D.;Mogutnov,B.M.Chem.S oc.Faraday Trans.1995,91(4),703.doi:10.1039/ft9959100703

    (30)Cao,Z.M.;Wang,K.P.;Qiao,Z.Y.;Du,G.W.A cta Phys.-Chim.Sin.2012,28(1),37.[曹戰(zhàn)民,王昆鵬,喬芝郁,杜廣巍.物理化學(xué)學(xué)報(bào),2012,28(1),37.]doi:10.3866/PKU.WHXB201111172

    (31)Vogel,R.;Klose,H.Arch.Eisenhuttenwesen 1952,23(7),287.

    (32)Kaneko,H.;Nishizawa,T.;Tamaki,K.Nippon Kinzoku Gakkai-shi 1965,29(2),159.

    (33)Yamada,K.;Kato,E.Tetsu-to-Hagane(J.Iron Steel Inst.Jap.)1979,65(2),273.

    (34)Yamada,K.;Kato,E.Trans.Iron Steel Inst.Jap.1983,23(1),51.doi:10.2355/isijinternational1966.23.51

    (35)Ding,X.;Wang,W.;Han,Q.Acta Metall.S in.1993,29(12),B527.

    (36)Raghavan,V.The Al-Fe-P System(Aluminium-Iron-Phosphorus).In Phase Diagrams of Ternary Iron Alloys,Part 3,Ternary Systems Containing Iron and P hosphorus;Indian Institute of Metals:Calcutta,1988.

    (37)Raghavan,V.Alloy P hase Dia grams 1989,5(1),32.

    (38)Schmid-Fetzer,R.;Tomashik,V.A.L andolt-B R nstein-Group IV P hysical Chemistry 2008,11D1(1),172.

    (39)Dinsdale,A.T.CAL PHAD 1991,15,317.doi:10.1016/0364-5916(91)90030-N

    (40)Muggianu,Y.M.;Gambino,M.;Bros,J.P.Chim.Ph ys.1975,72,83.

    (41)Ansara,I.;Dupin,N.;Lukas,H.L.;Sundman,B.J.Alloy.Compd.1997,247,20.doi:10.1016/S0925-8388(96)02652-7

    (42)Dupin,N.;Ansara,I.;Sundman,B.CAL PH AD 2001,25,279.doi:10.1016/S0364-5916(01)00049-9

    猜你喜歡
    北京科技大學(xué)材料科學(xué)工程學(xué)院
    《北京科技大學(xué)學(xué)報(bào)(社會(huì)科學(xué)版)》
    理論縱橫(2024年1期)2024-01-11 07:56:12
    中海油化工與新材料科學(xué)研究院
    《北京科技大學(xué)學(xué)報(bào)(社會(huì)科學(xué)版)》
    理論縱橫(2022年6期)2022-12-06 04:27:50
    福建工程學(xué)院
    福建工程學(xué)院
    《北京科技大學(xué)學(xué)報(bào)》(社會(huì)科學(xué)版)
    理論縱橫(2022年1期)2022-02-16 07:26:06
    材料科學(xué)與工程學(xué)科
    福建工程學(xué)院
    福建工程學(xué)院材料科學(xué)與工程學(xué)科
    福建工程學(xué)院
    有码 亚洲区| 国产又色又爽无遮挡免| 两个人的视频大全免费| 久久久久精品久久久久真实原创| av又黄又爽大尺度在线免费看| 日韩成人av中文字幕在线观看| 久久久色成人| 欧美成人午夜免费资源| 成人高潮视频无遮挡免费网站| 两个人的视频大全免费| 久久99热这里只有精品18| 国产视频首页在线观看| 天堂俺去俺来也www色官网| 国产伦精品一区二区三区四那| 国产精品.久久久| 日产精品乱码卡一卡2卡三| 精品久久久久久久久av| 少妇 在线观看| 男女无遮挡免费网站观看| 亚洲国产日韩一区二区| 日本wwww免费看| 国产高清国产精品国产三级 | 又黄又爽又刺激的免费视频.| 成人午夜精彩视频在线观看| 成人毛片60女人毛片免费| 国内少妇人妻偷人精品xxx网站| 中文资源天堂在线| 激情 狠狠 欧美| 日韩三级伦理在线观看| 亚洲一级一片aⅴ在线观看| 成人黄色视频免费在线看| 久久99精品国语久久久| 亚洲真实伦在线观看| 久久久久久久久久久免费av| 国产黄片美女视频| 热99国产精品久久久久久7| 亚洲国产精品成人综合色| 久久这里有精品视频免费| 美女被艹到高潮喷水动态| 联通29元200g的流量卡| 国产午夜福利久久久久久| 国内揄拍国产精品人妻在线| 毛片一级片免费看久久久久| 成人亚洲精品av一区二区| 国产又色又爽无遮挡免| av免费观看日本| 欧美性感艳星| 欧美 日韩 精品 国产| 高清视频免费观看一区二区| 2022亚洲国产成人精品| 久久人人爽av亚洲精品天堂 | 简卡轻食公司| 日日摸夜夜添夜夜添av毛片| 97人妻精品一区二区三区麻豆| 舔av片在线| 简卡轻食公司| 久久久久久久久久成人| 国产一区二区在线观看日韩| 校园人妻丝袜中文字幕| av线在线观看网站| 国产老妇女一区| 菩萨蛮人人尽说江南好唐韦庄| 欧美日韩视频高清一区二区三区二| 少妇 在线观看| 欧美高清成人免费视频www| 老司机影院毛片| 亚洲av.av天堂| 性插视频无遮挡在线免费观看| 久久99热6这里只有精品| 尾随美女入室| 国内揄拍国产精品人妻在线| 看十八女毛片水多多多| 汤姆久久久久久久影院中文字幕| 久久久国产一区二区| 国内精品宾馆在线| 人妻 亚洲 视频| 国内少妇人妻偷人精品xxx网站| 色吧在线观看| 好男人在线观看高清免费视频| videos熟女内射| 五月开心婷婷网| 精品人妻视频免费看| 国产av国产精品国产| 中文字幕制服av| h日本视频在线播放| 91aial.com中文字幕在线观看| 国产亚洲最大av| 亚洲精品成人av观看孕妇| 国产成人午夜福利电影在线观看| 日韩av在线免费看完整版不卡| 一级a做视频免费观看| 欧美xxxx性猛交bbbb| 久久这里有精品视频免费| 亚洲精品自拍成人| 亚洲精品久久午夜乱码| 最近最新中文字幕大全电影3| 成人免费观看视频高清| 一本—道久久a久久精品蜜桃钙片 精品乱码久久久久久99久播 | 国产色婷婷99| 日本与韩国留学比较| 亚洲最大成人av| 天堂俺去俺来也www色官网| 精品视频人人做人人爽| 国产免费一级a男人的天堂| 一级a做视频免费观看| 午夜激情福利司机影院| 久久久久久久久久成人| 丰满人妻一区二区三区视频av| 国语对白做爰xxxⅹ性视频网站| 精品人妻一区二区三区麻豆| 中文字幕av成人在线电影| 久久影院123| 婷婷色av中文字幕| 精品国产一区二区三区久久久樱花 | av网站免费在线观看视频| 亚洲国产欧美人成| 麻豆乱淫一区二区| 成人亚洲精品一区在线观看 | 亚洲av免费在线观看| 王馨瑶露胸无遮挡在线观看| 80岁老熟妇乱子伦牲交| 精品久久久久久久久亚洲| 国产免费一区二区三区四区乱码| 国产日韩欧美在线精品| 亚洲成人精品中文字幕电影| 国产免费一区二区三区四区乱码| 又爽又黄a免费视频| 国内精品美女久久久久久| av又黄又爽大尺度在线免费看| 亚洲aⅴ乱码一区二区在线播放| 91精品国产九色| av天堂中文字幕网| 久久人人爽人人爽人人片va| 韩国高清视频一区二区三区| 最近中文字幕2019免费版| 日韩av免费高清视频| 亚洲精品成人av观看孕妇| 日韩,欧美,国产一区二区三区| 精品久久久久久久久亚洲| 最后的刺客免费高清国语| 男女无遮挡免费网站观看| 亚洲电影在线观看av| 在线观看一区二区三区| 啦啦啦在线观看免费高清www| 一本—道久久a久久精品蜜桃钙片 精品乱码久久久久久99久播 | 午夜福利视频精品| 国产片特级美女逼逼视频| 午夜精品国产一区二区电影 | 人妻夜夜爽99麻豆av| 男女边摸边吃奶| 久久99热这里只有精品18| 国产亚洲最大av| av国产久精品久网站免费入址| 三级国产精品片| 成人一区二区视频在线观看| 老司机影院毛片| 大码成人一级视频| 久久精品久久久久久久性| 成人亚洲精品一区在线观看 | 男女边吃奶边做爰视频| 内地一区二区视频在线| 亚洲一区二区三区欧美精品 | 最近中文字幕2019免费版| 一级a做视频免费观看| 国产一级毛片在线| 麻豆久久精品国产亚洲av| 亚洲精品色激情综合| 精品久久久精品久久久| 亚洲人成网站在线播| 熟女av电影| 夫妻性生交免费视频一级片| 亚洲欧美精品专区久久| 日韩av免费高清视频| 欧美xxxx黑人xx丫x性爽| 97精品久久久久久久久久精品| 一级av片app| 精品视频人人做人人爽| 夫妻性生交免费视频一级片| 欧美日韩在线观看h| 国产男女内射视频| 国产精品嫩草影院av在线观看| 国产亚洲av片在线观看秒播厂| 永久免费av网站大全| 国产精品女同一区二区软件| 亚洲在线观看片| 亚洲激情五月婷婷啪啪| 性插视频无遮挡在线免费观看| 亚洲av成人精品一区久久| 1000部很黄的大片| 最近中文字幕高清免费大全6| 免费黄网站久久成人精品| 永久免费av网站大全| 久久综合国产亚洲精品| 在线观看一区二区三区激情| 久久精品国产自在天天线| 国产精品熟女久久久久浪| 久久亚洲国产成人精品v| 国内揄拍国产精品人妻在线| 国产精品99久久99久久久不卡 | 国产亚洲精品久久久com| 国产欧美日韩精品一区二区| 国产一区二区三区av在线| 日韩免费高清中文字幕av| 国产精品不卡视频一区二区| 九九久久精品国产亚洲av麻豆| 亚洲综合精品二区| 亚洲国产日韩一区二区| 狂野欧美激情性xxxx在线观看| 超碰97精品在线观看| 亚洲成人av在线免费| 激情五月婷婷亚洲| 国产在线一区二区三区精| 在线观看av片永久免费下载| 亚洲欧美清纯卡通| www.av在线官网国产| 2018国产大陆天天弄谢| 亚洲av在线观看美女高潮| 亚洲精品亚洲一区二区| 好男人在线观看高清免费视频| 尾随美女入室| 久久久久久国产a免费观看| 国产精品久久久久久久久免| 神马国产精品三级电影在线观看| 免费观看无遮挡的男女| 欧美高清成人免费视频www| 国内揄拍国产精品人妻在线| 午夜爱爱视频在线播放| 免费观看在线日韩| 色播亚洲综合网| 亚洲在线观看片| 亚洲自拍偷在线| 亚洲综合精品二区| 国内精品美女久久久久久| 国产黄a三级三级三级人| 美女视频免费永久观看网站| 神马国产精品三级电影在线观看| 97热精品久久久久久| 亚洲欧美成人精品一区二区| 欧美精品国产亚洲| 国产乱人偷精品视频| 欧美亚洲 丝袜 人妻 在线| 18禁裸乳无遮挡免费网站照片| 国产午夜精品一二区理论片| 亚洲自偷自拍三级| 国产久久久一区二区三区| 午夜福利高清视频| 欧美成人一区二区免费高清观看| 国产成人一区二区在线| 丰满乱子伦码专区| 成年女人在线观看亚洲视频 | av黄色大香蕉| 深夜a级毛片| 久久久久精品性色| 国产免费福利视频在线观看| 国模一区二区三区四区视频| 精品酒店卫生间| 青春草亚洲视频在线观看| 老师上课跳d突然被开到最大视频| 91午夜精品亚洲一区二区三区| 日日摸夜夜添夜夜爱| 国产成人午夜福利电影在线观看| 亚洲自偷自拍三级| 在线观看人妻少妇| 精品国产乱码久久久久久小说| 最近手机中文字幕大全| 白带黄色成豆腐渣| 激情 狠狠 欧美| 国产 一区 欧美 日韩| 国产乱人视频| 免费观看的影片在线观看| 一级毛片aaaaaa免费看小| 亚洲av成人精品一二三区| 成年免费大片在线观看| 亚洲成色77777| 在线观看国产h片| 亚洲人成网站高清观看| 日日啪夜夜撸| 国产 精品1| 99精国产麻豆久久婷婷| 国产亚洲午夜精品一区二区久久 | 日韩中字成人| 美女高潮的动态| 白带黄色成豆腐渣| 久久久久精品久久久久真实原创| av在线播放精品| 欧美3d第一页| 成人欧美大片| 波野结衣二区三区在线| 高清日韩中文字幕在线| 午夜福利视频1000在线观看| 国产色爽女视频免费观看| 午夜福利高清视频| 舔av片在线| 欧美成人精品欧美一级黄| 三级经典国产精品| 高清日韩中文字幕在线| 精品人妻熟女av久视频| 亚洲无线观看免费| 国产亚洲5aaaaa淫片| 69av精品久久久久久| 青春草国产在线视频| 日韩欧美 国产精品| 亚洲国产精品成人综合色| 欧美变态另类bdsm刘玥| 一级毛片电影观看| 午夜视频国产福利| 国产亚洲午夜精品一区二区久久 | 日韩三级伦理在线观看| 99热这里只有是精品50| 少妇人妻久久综合中文| 丝瓜视频免费看黄片| 欧美日韩在线观看h| 久久人人爽人人片av| 交换朋友夫妻互换小说| 午夜爱爱视频在线播放| 国内少妇人妻偷人精品xxx网站| 久久6这里有精品| 人人妻人人爽人人添夜夜欢视频 | 欧美xxⅹ黑人| 久久久久九九精品影院| 国产男女超爽视频在线观看| 欧美成人一区二区免费高清观看| 成人高潮视频无遮挡免费网站| 麻豆国产97在线/欧美| 又爽又黄a免费视频| 免费播放大片免费观看视频在线观看| 成年免费大片在线观看| 亚洲精品久久久久久婷婷小说| 国产精品熟女久久久久浪| 国产有黄有色有爽视频| 婷婷色综合www| 国产成人精品福利久久| 国产免费视频播放在线视频| 岛国毛片在线播放| 性插视频无遮挡在线免费观看| 伦精品一区二区三区| 国产高清国产精品国产三级 | 免费观看av网站的网址| 免费观看的影片在线观看| 成人亚洲精品一区在线观看 | 免费观看无遮挡的男女| 久久久久久久久久久免费av| 色播亚洲综合网| 色5月婷婷丁香| 精品久久国产蜜桃| 免费人成在线观看视频色| 高清日韩中文字幕在线| 久久久久久久亚洲中文字幕| 五月玫瑰六月丁香| 中文字幕免费在线视频6| 亚洲欧美日韩无卡精品| 最近2019中文字幕mv第一页| 亚洲精品aⅴ在线观看| 禁无遮挡网站| 三级男女做爰猛烈吃奶摸视频| 18禁在线播放成人免费| kizo精华| 黄色怎么调成土黄色| 国产伦理片在线播放av一区| 久久ye,这里只有精品| 国产伦精品一区二区三区四那| 日日撸夜夜添| 又爽又黄a免费视频| 亚洲国产精品专区欧美| 国产在线一区二区三区精| 欧美bdsm另类| 久久久久久久久久久丰满| 99久久精品热视频| 99热这里只有精品一区| 亚洲综合色惰| 久久久久久久亚洲中文字幕| 日韩av免费高清视频| 久久精品熟女亚洲av麻豆精品| 国产伦精品一区二区三区视频9| 女人十人毛片免费观看3o分钟| 国产精品麻豆人妻色哟哟久久| 男女下面进入的视频免费午夜| 久久人人爽人人片av| 亚洲精品久久久久久婷婷小说| 亚洲成人久久爱视频| 永久网站在线| 国产淫片久久久久久久久| 91久久精品电影网| 狂野欧美白嫩少妇大欣赏| 成人毛片a级毛片在线播放| 亚洲精品日本国产第一区| 人妻夜夜爽99麻豆av| 性插视频无遮挡在线免费观看| 亚洲人成网站在线观看播放| 久久久精品欧美日韩精品| 尾随美女入室| 免费观看无遮挡的男女| 99精国产麻豆久久婷婷| 在线 av 中文字幕| 亚洲一区二区三区欧美精品 | 久久国产乱子免费精品| 国产爽快片一区二区三区| 国产精品秋霞免费鲁丝片| 精品人妻一区二区三区麻豆| 国产亚洲91精品色在线| 国产精品人妻久久久久久| 最后的刺客免费高清国语| 亚洲国产高清在线一区二区三| 六月丁香七月| 亚洲电影在线观看av| 成人无遮挡网站| 亚洲经典国产精华液单| 禁无遮挡网站| 午夜福利网站1000一区二区三区| 黄色视频在线播放观看不卡| 亚洲精品,欧美精品| 国产精品伦人一区二区| 久久久成人免费电影| 高清毛片免费看| 成人国产av品久久久| 哪个播放器可以免费观看大片| 欧美丝袜亚洲另类| 久久精品久久久久久噜噜老黄| 中文字幕制服av| 久久国产乱子免费精品| 亚洲精品一区蜜桃| 2018国产大陆天天弄谢| 亚洲无线观看免费| 国产黄片视频在线免费观看| 成人免费观看视频高清| 男插女下体视频免费在线播放| 国产熟女欧美一区二区| 热99国产精品久久久久久7| 国产高潮美女av| 国产老妇伦熟女老妇高清| 国产乱人视频| 亚洲伊人久久精品综合| 久久久a久久爽久久v久久| av又黄又爽大尺度在线免费看| 国产成人精品婷婷| 九九爱精品视频在线观看| 国产有黄有色有爽视频| 国产精品精品国产色婷婷| 51国产日韩欧美| 亚洲经典国产精华液单| 欧美一区二区亚洲| 中文在线观看免费www的网站| 久久99蜜桃精品久久| 毛片女人毛片| av专区在线播放| 国产一区亚洲一区在线观看| 亚洲久久久久久中文字幕| 男女啪啪激烈高潮av片| 久久国内精品自在自线图片| 特级一级黄色大片| 精品久久久久久电影网| 特大巨黑吊av在线直播| 欧美精品一区二区大全| 好男人视频免费观看在线| 九草在线视频观看| 国产精品三级大全| videos熟女内射| 久久久成人免费电影| 乱系列少妇在线播放| 午夜福利在线观看免费完整高清在| 免费观看无遮挡的男女| 免费大片黄手机在线观看| a级毛片免费高清观看在线播放| 精品一区二区三卡| 偷拍熟女少妇极品色| 国产成人freesex在线| 少妇猛男粗大的猛烈进出视频 | 97热精品久久久久久| 免费观看在线日韩| 狂野欧美激情性bbbbbb| 精品人妻视频免费看| 伊人久久国产一区二区| 亚洲国产欧美人成| 熟女av电影| 色播亚洲综合网| 久久女婷五月综合色啪小说 | 午夜免费观看性视频| 我要看日韩黄色一级片| 免费大片黄手机在线观看| 亚洲欧美清纯卡通| 蜜臀久久99精品久久宅男| 久久久久久久大尺度免费视频| 亚洲熟女精品中文字幕| av在线老鸭窝| 18禁在线播放成人免费| 久久女婷五月综合色啪小说 | 久热这里只有精品99| 久久精品综合一区二区三区| 亚洲天堂国产精品一区在线| 亚洲综合色惰| 免费看不卡的av| 日日摸夜夜添夜夜爱| 大话2 男鬼变身卡| 啦啦啦啦在线视频资源| 亚洲综合色惰| 亚洲精华国产精华液的使用体验| 欧美激情在线99| 精品国产一区二区三区久久久樱花 | 国产av国产精品国产| 亚洲第一区二区三区不卡| 麻豆精品久久久久久蜜桃| 少妇人妻 视频| 大又大粗又爽又黄少妇毛片口| 91久久精品国产一区二区三区| 亚洲无线观看免费| 亚洲色图综合在线观看| 1000部很黄的大片| 啦啦啦啦在线视频资源| 国产精品国产三级国产av玫瑰| 男女无遮挡免费网站观看| 日本av手机在线免费观看| 亚洲国产高清在线一区二区三| 国产黄色视频一区二区在线观看| 成人黄色视频免费在线看| tube8黄色片| 欧美性感艳星| 夜夜看夜夜爽夜夜摸| 最近手机中文字幕大全| 久久99蜜桃精品久久| 中文在线观看免费www的网站| 有码 亚洲区| 免费大片黄手机在线观看| 亚洲四区av| 日韩av不卡免费在线播放| 亚洲精品国产av蜜桃| 免费不卡的大黄色大毛片视频在线观看| 真实男女啪啪啪动态图| 欧美另类一区| 黄色日韩在线| 丝袜脚勾引网站| 哪个播放器可以免费观看大片| 亚洲人成网站在线播| 亚洲综合色惰| 日韩成人伦理影院| 97热精品久久久久久| 亚洲精品久久久久久婷婷小说| 干丝袜人妻中文字幕| 亚洲av免费在线观看| 小蜜桃在线观看免费完整版高清| 久久久久久久精品精品| 免费观看在线日韩| 91精品国产九色| 一级片'在线观看视频| www.av在线官网国产| 午夜爱爱视频在线播放| 久久久久精品久久久久真实原创| 国产日韩欧美亚洲二区| 亚洲av男天堂| 午夜精品一区二区三区免费看| 深夜a级毛片| 男女边吃奶边做爰视频| 欧美老熟妇乱子伦牲交| 青青草视频在线视频观看| av专区在线播放| 色吧在线观看| 国产精品精品国产色婷婷| 最近最新中文字幕大全电影3| 又粗又硬又长又爽又黄的视频| 亚洲图色成人| 美女国产视频在线观看| 内地一区二区视频在线| 亚洲欧洲国产日韩| 啦啦啦啦在线视频资源| 黄片无遮挡物在线观看| 麻豆精品久久久久久蜜桃| 国产亚洲5aaaaa淫片| 亚洲av不卡在线观看| 亚洲综合色惰| 亚洲在线观看片| 七月丁香在线播放| tube8黄色片| 一级片'在线观看视频| 另类亚洲欧美激情| 亚洲av欧美aⅴ国产| 亚洲精品第二区| 哪个播放器可以免费观看大片| 麻豆乱淫一区二区| 亚洲精品成人久久久久久| 高清在线视频一区二区三区| 亚洲美女视频黄频| 亚洲国产成人一精品久久久| 菩萨蛮人人尽说江南好唐韦庄| 国产乱人偷精品视频| 2018国产大陆天天弄谢| kizo精华| 少妇猛男粗大的猛烈进出视频 | 亚洲欧洲日产国产| 色网站视频免费| 热re99久久精品国产66热6| 一级片'在线观看视频| 亚洲av二区三区四区| 国产亚洲一区二区精品| 久久久国产一区二区| 波野结衣二区三区在线| 欧美3d第一页| 亚洲怡红院男人天堂| 91精品一卡2卡3卡4卡| 国产精品嫩草影院av在线观看| 亚洲欧美精品专区久久| 精品久久久噜噜| 国产综合精华液| 成人亚洲欧美一区二区av| 亚洲人与动物交配视频| 免费看a级黄色片| 卡戴珊不雅视频在线播放| 久久精品熟女亚洲av麻豆精品| 国产成人精品婷婷| 精品视频人人做人人爽| 啦啦啦中文免费视频观看日本| 伦理电影大哥的女人| 中文乱码字字幕精品一区二区三区| 大陆偷拍与自拍| 免费黄色在线免费观看| 亚洲欧洲国产日韩| 波多野结衣巨乳人妻|