Metallurgical Society of CIM Annual Volimie Featuring Molybdenum incorporating Vol. 16, Nos. 1-4, 1977, of the Canadian Metallurgical Quarterly J.M. Toguri, Editor G. C. Weatherly, Assistant Editor THE CANADIAN INSTITUTE OF MINING AND METALLURGY| | i THE METALLURGICAL SOCIETY OF CIM P, Tarassoff — President 8. H. Melbourne — Ist Vice-President W. Smith — Treasurer Itzkovitch — Seeretary THE PUBLICATIONS COMMITTEE J. D. Boyd — Chairman R. A. Bergman, G. R. Hoey, D. A. R. Kay, ALD. Pelton, M. ¥. Solar, G. Van Weert THE ANNUAL VOLUME 3. M, Toguri — Editor G. C. Weatherly — Assistant Editor Board of Review: G. E. Agar, J. D. Boyd, J. EB. Dutrizac, G. R. Hoey, H.W, King, C. R. Masson, L.R, Morris, R. Sridhar, F, Weinberg 4J.L. MeGerrigle — Production Editor ‘The Canadian Institute of Mining and Metallurgy, Suite 400, 1180 Sherbrooke St. West, Montreal, Quebec, H8A 2M8 ‘The Annual Volume of The Metallurgical Society of CIM is published by The Canadian Institute of Min- ing and Metallurgy as a contribution to the science and technology of metallurgy. La traduction des résumés est faite par le départe- ment de métallurgie de |'Bcole ‘Polytechnique, Montréal. Price: CIM Members $15; Others $25. NOTE TO AUTHORS Submission of Manuscripts ‘The editors invite manuscripts, written discussion and other comments. These should be addressed to the Editor, Professor J. M. Toguri, Department of Metallurgy and Materials Science, University of Toronto, Toronto MSS 1A4, Ontario, Canada, All submitted manuscripts will be reviewed by at least two referees whose findings will be trans- mitted via the Board of Review to the Editor. The Editor, acting on the advice of the referees, is responsible for the ultimate acceptance or rejection of the manuscript. Written discussion of papers should be submitted within two months of the publication date, and will be forwarded to the author of the paper for reply. Discussions and replies will be publ'hed together, ‘Manuscript Requirements Three copies must be submitted, typed double- spaced on 814- by 10-In, paper, with a generous margin, ‘The abstract, together with the title of the paper, names of authors and their affiliations, showld be Presented on the first page of the manuscript Abstracts should be no more than 150 words. Titles should be kept to minimum length. ‘Tables should be typed on separate sheets, A list of figures, with numbers and captions, should be submitted ‘with the manuseript, wo References are to be indicated in the text in order ‘of appearance by a parenthetical number. They should be listed on a separate page in the numerical order in which they are used in the text, using accepted abbreviations. The form will be: (3) Smith, J. F., Jones, C. L, and Brown, H. W., Je Inst. Metals. 88: 172 (1961). Formulae should be numbered in order of appear- ance along the right-hand margin, Important: Symbols should be clarified by mar- ginal notes. The following should be identified: zero and capital letter 0; lower case letter “ell” and figure one. Line drawings and photographs, no larger than 8% x 11 inches, but capable of reduction, should be submitted in quadruplicate, They should include one master set for reproduction; that is, glossy photographs and/or original line drawings. ‘The re- maining three sets may be copies suitable for read- ing. All wording to-be reproduced with the figures should be printed upon them, except for figure number and caption. Each should be identified on the reverse with figure number, title of paper and name of author. In cases where there might be doubt, the top of the photograph or figure should be marked. Photomicrographs should be submitted so that they may be reproduced ‘size as’, and the correct magnification retained. If the degree of magnifica tion is not indieated in the photomicrograph, this information should be ineluded in the eaption, ‘The editor will insert all illustrations as close as possible to the first mention in the text. Original line drawings will be returned to the author.TRANSACTIONS, The Thermodynamics of Dilute Liquid Nickel Alloys G.K. Sigworth, Assistant Professor, Department of Metalluray and Materials Science, CarneaedMelion University, Pittsburgh, Pennsylvania 4. Elliot, Professor of Metalluray, Massachusetts Institute of Technology, Cambridge, Massachusetts G. Vaughn, Graduate Student, and GLH Geiger, Professor, Department of Metallurgical Engineering, University of Arizon Tucson, Arizona Abstract The published data on the thermodynamics of liquid nickel-base alloys, have" been reviewed. "Recommended Tormodyamie watuts are tebulstad for binary end ter- nary alloye, and ealeulated values of deosidation con Mtante are. piven for selected elements. Les données publiges sur la thermodynamique des allia- ‘gerd ave de nickel liquide sont paseées en revue. Les Qaleurs thermodynamiques a conecilicr vont tabulees pour Tce altiager binaires cf ternatres et lea valeurs. ealcules dep constantes de désozydation sont données pour divers ements, Introduction CONSIDERABLE INFORMATION on the thermo- dynamic behaviour of elements in liquid nickel has been reported in the Iiterature. Unfortunately, these data are often widely scattered and presented in a variety of ways. Some systems have been reviewed by Hultgren and co-workers” in their survey of the thermodynamic properties of binary metallic all There is also thermodynamte information in the surveys on binary phase diagrams,”, but no single compilation has been made. In this paper, the avail~ able thermodynamic data have been reviewed and summarized, and recommended thermodynamic values are given for elements dissolved in nickel-base alloys. Although data in the literature appear in several forms, only two are used in reporting the results of this study. ‘They are composition in atom fraction, with the pure sub- stance as the reference and standard states, and composi- tion in weight per cent, with the infinitely dilute solution as the reference state and a hypothetical 1 per cent solu- tion as the standard state. By convention, the activity coefficient @,/X, = x1 when X, 0, and a,/%, 1 when %, “> 0. As some publications do ‘not employ these standard and reference states, it has been necessary jn many instances to make a conversion from the data as reported in the literature, Should the reader wish to alter the standard state or composition coordinate employed in this paper, a brief treatment of the method for making the conversion is available in an earlier compilation’. A more ‘generalized treatment of the subject! is also available. 108 ‘Table 1 shows the selected values for the standard free energy of solution of elements in dilute liquid nickel. Notes regarding the calculation of tabulated values appear with the table, Tables 2 and 3 show selected Gibbs free energy interaction coefficients for nickel-based alloys. The interaction coefficient was introduced by Wagner," first used by Chipman," and later extended formally by Lupis and Elliot." Using the notation of Lupis and Elliott,” ret == me Edt Bote + 2 dpa on + oc ® i< ‘The solvent, liquid nickel, has een designated as component 1 in the n-component system, and the pure substance is used as the reference state. Third and higher-order terms are usually neglected, because the accuracy of the available date rarely permit their caleulation with any degree of certainty. When the ‘composition coordinate is weight per cent, the Taylor series expansion corresponding to eq. (2) is: Sem it Brim. iP 3, rte iwt, illo. % HI + 0 (56%) @ directly from experimental measurements are in bold- face type. (Others have been calculated by using the conversion equations of Lupis and Elliott”) ‘The temperature given indicates the experimental tem- perature used in the original determination of thermo- dynamic properties, A temperature range indicates that more than one temperature was employed in the original experiments, and that the values tabulated are valid for that range of temperature. The numbers of the references providing the results shown in the tables are in bold-face type. When the authors have found it necessary to caleulate (or recalculate) inter- action coefficients from the data given in a study, an asterisk follows the corresponding reference number. ‘The free-energy data in Table 1 and information on thermochemistry of oxides"** have been used to calculate deoxidation equilibria, The results are shown in Table 4. It is necessary to discuss the values given for the interaction coefficients in Ni-i-C alloys in Table 8. The caleulated interaction coefficients have been deter- mined for carbon-saturated solutions. They differ from the other coefficients in that they are deter- mined at unit carbon activity; hence, X: #1. The free energy interaction coefficients are defined after Lapis: ye thn | o The Metallurgical Society of CIMTABLE 1 — The Gibbs Free Energy of Solution of Fements in Liquid Nickel @ (0) (oy | ® aden sat ® Etemeat, askire) afm tomy caller. som) Teo) | eterences Gonsuted Mo ome yons2e7 | — mam gai | oan sama a iw a ist? baa ae sais [Pew szm | Beason HS i a ais | zen ma — Siem) tn 13 2%) e Jom—sor | n= sogsr ‘se soe. .a0 &, o> SaaS [ee Bam ae “i ef) @ Hho |alletZans — S ep o8 ait a ist ios 3.3, xs) os a 2867 09 ast om | oma se oS Scien | Mo ENB ees & Se Bel ae aa B toward ra ig Btoosaer [Mtoe sr baw [RAE og, RSS os a) rn — ager sy ® = tte 1Stamo Bs me ae Esa Sadao (See oe % ER [ER eR |S EE 1 om «samy 10 war hi Preven | Bay | } é os eran = i ¢ . Salt Der woz | byrne ts - - — 169704 0.336T | 1500-1700, 83-90, 91, 92, 93, 94, | 95, 96, 136 “4 ego ge-ago |p tis is (eet Bi |By,s B " Mae'r ead? | Bag aces = gto — ot Selig | |e |B, 07-tio, far-lie oe res sum, | room | aw 258 ‘.o0019 ‘24300 — 1 93Ty=) (= 26300— lasetye) | 1550-1700 15-17 20,107,116, 117-122 a feo —2ay | eer ierys | er B oy a Citta |B! 5 Bs ae aasryiny | asa sora» | eo wa, i ae} Gee sames |g Ha Str Ce amen | ed rg |i | Bh (9) For the standard state shown i the fest column, Gases ae alone atmosphere pessre Vals in parenhese ae for unelable standard Siterat ere (©) See te tet for an explanation athe standard and reference states used. Values in paentheses are considered tobe uncertain, (©) Principal raerenes used in data election are in boar ype. (Q) Regular salut esumed forthe que phase, Cais om ncn by. () Cakuatd tram exe sly, TABLE 2 — Free Energy Interaction Coefficients in Binary Nickel Alloys Element, ad A a @ (0.09 ae oz) oe (ons) ct a {a 40.008) & ® o o oe 1 ew aoa cu a ® ore Fe 40 ° ans ¥ i ds ° " a ° ° 03 6 § seme st2 | Comnet+es | usa one ‘Annual Volume, 1977 105‘TABLE 3 — Free Energy Interaction Coefficients in Ternary Nickel Alloys eG Alloys tome] a (3a o0@ | mee oop Gah mi | be Sot ain, 2 8 tt am ‘ & |g 005 ftihy [tly Tk & — |=0% = anet tom) |) | L169 or ae = ba Cit) {Eto | on 1609 co dog none em | Qa 10 fe | a | ees gs |i {3.100 a |e ania Voom =| 46 iso \2 & |S oe {ory cap cd 3 i jaar 2a {om | (as tet 2 fin | Bat soni fom | toy | in ws te es Petey | Eo) | tan asoo faa : 52 aoe om a0 19 z by 3 {ow {im (tm | to z a 4 ‘ns ep (on, | to 2 Site ine fa) | faa Isat in Site aan omy {ios} Teo \z s 383 ast ai) (aoe isan ar a a oo comp oy fis 2 ie 2 tos, G0 on} {sit zg i ety te Som [oi tn \2 Y = Be = ams 0) om eta kar w are = not Com = [om etn z hh is ao ‘ame way? tee 3 3) The values for dilute solutions have been 1m data in references 2 ar 150. The val 3° Elementi | a oa Retereees e @ 0 ra fe ti $ Hea te | 3 ie i (2 3 std Senet ck ee a | ro) elereces i ° 0), fae ae i cis) | zeta ia i |e Sass Ito 07, es, 10 | ! | Part, EH Alloys & a ee nt e Te) |__Reterences u 24 2 | ona omen [025 7si0 1700 | 67, a | 3 o ons a as | te Bi & on ° oo 4 oar Teton | 36,6408, i, & om <2 ong =oaor | — ane 1st0 Biss & (an os oon © =e roc | Be 7o,70° fe 8 “e foe Q =ar 10 3 is, { ae mo | 338 ° oon 0 | os sono [a Me |= 20 ° “aoe | os {son 2 § ua ‘ aus 2 come = |=B Wstasco | 67,68 ¥ in ta a3 | oat ‘eso @ ¥ 55 . tt Soon, \ts isa | Be 108 ‘The Metallurgical Society of CIM.rep Relerences Time fu wae | Tee) Relrecee | ssa "su & ere ry os 1333 Fa & a ‘ Sse | eo 8 & oz nos on itis Te fe 26 =a ou feanzam | 89,74, 2 me |=i6 a8 ont reget | 9,120, q oh: oo C02 Taoism |e aa w =i we Cie 18) | sats * rae @ |=s3t |i i Elementi] 2d o & Te) References Au — 24 BI lo 1550 re ets Cosy 10 & IY aa ae Q 10 & har oras 20 ° 19 & ia is = te Sox Gots | Isoa4600 fe ea a ons ame Zan 109 : as a t 1809, § Ss 50 ‘Zoo | Zone 1600, 3 5 at) i cu 8 =z 1800, 5.07, i = co ite tata v aa Zs Call a =i 1800 Bar Part H, NELS Alloys Hemest,i| at lee a o| oe Teo) Refeenes x ies 72 jou fo yan 10 Pi & as ¢ Sour 3 {09 130 in! & a oy a 0 fos {sto 3 & a o {dna 0 te isn w fe LL | 0.005, fo 1.005, 1540-1600 99, 101, 108. i Bs ay 0 © noms | ols ie |= Ky ae 29 oe a fs sa ine th i 38 oe 3 ae sn s and General Remarks ue dof “- ~ o It must be emphasized that data tabulated in this 3% In,Pac=1 Several conversion relationships are also given by Lupis," but the most important in the context of this paper is given below: 4 Ke he 14 Xe +2 KOE ‘The mole fraction of carbon at carbon saturation, Ke, is known, but the other interaction coefficients are not known. It therefore has been necessary to assume they are zero, of $i has been assumed to be equal to e:. The cal~ culated values in Table 3 reflect this assumption. ‘These values are considered to be rough estimates and are, there- fore, shown in parentheses. Annual Volume, 1977 study are offered for the convenience of the reader fas survey values. Many assumptions have been em- ployed in this study, and much subjective judgment hhas been exercised by the authors in selecting data. Also, it has not been practical to indicate the accuracy of thermodynamic values tabulated herein. For these reasons, the reader is encouraged to examine the original studies. It may be useful to consider a few of the pitfalls inherent in this survey. A careful examination of all information on the Ni-S system, for example, will show data in Tables 1 and 2 to be valid only for low concentrations (less than about 2 atom per cent) 107TABLE 4 — Calculated Deoxidation Equilibria in Nickel Alloys. |_-wK aN +0 o0ya5/T— te so7 | 448 x 10 25 0 Wee T— 7 | 30x 1 e +0 350877 + 206 | 922% 10> G& $0 eos e503 | 216% 108 & +o aT 6815 | 0087 Zoe 30 Bau war | 8343 10 Fe to 7st — 401 |B Me =o wong T— 738 | 32> 108 mm $0. Uist T— 652 | Te te si +20 BOT — i796 | G18 x Loe t o2 saigT— ws | 805% 1 2v +30 = arate | 148310 te $20 = wows) | amt 155 | 938K ID “These oxides frm spinels with nickel oxide at low aly concentra tons) At high sulphur contents, one should use the results of Meyer and co-workers.’ In other words, the values selected here for dilute nickel-base alloys would apply to melting operations, but would not apply to matte smelting or to calculations of the Ni-S phase diagram, One will also find a discrepancy between the NI-O phase diagram and the thermodynamic values, tabulated in this study. The error could be eaused by any of the following (a) the values for the free energy of solution of oxygen in Table 1 are too negative: () the interaction coefficients, «§ and cf, are non-zero; (¢) the published value for the free energy of formation of nickel oxide **® isin error. In spite of this difficulty, the selected values for oxygen are in accord with published deoxidation equilibria for Al, Mn, Si, Ti and V, and are felt to be rellable for dilute solutions. A final comment is needed. The information avail- abe on the thermodynamics of solution of many ele- ments in nickel is sparse. Experimental work on B, ©, Ca, Mg, Mo, Ti, W and Zr would be desirable, References (DR, Hultgren, PD. Desai, D. T. Hawking, 3. Giviser and'K. K. Kelly. Selected Values of’ The Thermodynamic Propertice of Binary Alloys, Amer, Soe. Metals, Metals Park, Ohio, 107%, (a) M. Hansen and K.’Anderko. Constitution of Bingry Atioys, nd. ed, MeGraw-Hil, New York, (b) R_P. Eliott, Constitution of Binary. Alloys, First ‘Supplement, MeGraw-Hil, New York, 1958 (e) FA. Shunk, Constitution ‘of ‘Binary ‘Aitoys, Third Supplement, MeGraw-HiMl, New York, 1968 (8) GK, Sigworth and J. F- Elliott, Can. Met, Quart 49: 455 “G974) @ (4) 3." "Bulott and_J. Chipman, Proc. of Int. Symp. ‘on Met. Chem. Sheffield, 1951, p. 121, Tron Steet co) ett, London, ar ha Tagner. Thermodynamics of Alloye, p. 61, Ad Mison Wesley, Reading, Mass, 1902 (6) J. Chipman,’ J. Tron Steel Institute, London, 180 91 (1958), (7) CH. P. upis and J.P, Elliott. Acta Afet, 142 530; 1019. (1960). (8) CHP. Lapis and J. F, Eliott, J. Iron Steet Tstiiute, London. 203° 79 (1908). () CWP. Lapis and. J. F, Elliott, Trane, Met, Soe, AuMie. 2357 257; 829 (1965). (10) CHP. Lupis and’ J. F. Elliott. Acta Met, 15: 108 265, (1967). (11) GOH, P. Lapis. Liquid Metale, Chemistry and Physics 8. Beer, ed, pp. 1-88, Marcel Dekker, New ‘York, 1973. (12) HEP. Tupi, Atet. Trans, 5: 1919 (1974). (13) F. Vacket, B, Desre and E, Bonnier. Comptes Rendu Abad, Sel, Paris, 260: 4633 1043. (1980). (14) W."G. ‘Dyubanoy, A. Ya. Stomaxn and A. F. Filippov, Fev. Vyssh. Ucheb, Zaved., Chern. Met. 1972 (3): 68. (15) V.'V. Averin, P. A. Cherkasoy and A. M. Samarin, Tealei.” po" Zharoprochn.. Splavam, Akad.” Wank SSE, net, Mat 9" 20418 (1902): (18) V. V,Averin, PA. Chetkasoy and’A. M. Samarin Ty. inet, Mer. im, AA, Boikova, Akad. Nok SSSRNo. 15: 58:67, (1968), (17) VV. “Avorin’ and. PLA. Chersskov. Biz Khim. Oinavy “Met. Protsesiov,” Komis, po. Fiz-Khim. Osnovam Proivv. Stati, Sb. Statel, 1064: 70-85, (18) V, Mi, Sandakov, Yu. 6. Esin and P. V. Geld, Zh, Piz, Khim. 5: 1798.00 (97), (29) J. Golonka and J. Daiemianke. Prace Inst, Hutnie- uch 21; "261-278 (1968). (20) A.'Ya: Stomakhin and A. Yu. Polyakov. fev. Vyssh. Voheb., Zaver. Chern, Met, 109113): 110-121 (21) W. Oclgen ‘and W. Middel, Afite, Kaiser Withelm Inst, Blsenforseh, 19: 1-26 (1831). (22) F."iorber,W. Gelsen, and H. Lichtenberg. ibid: Ta1.a60. (28) A. Neckel, 1, Brdelyi, G. Sodeck and B, Buschmann, Gang Met. Quart, 13: 819-081 (974). (24) Avi Biswas and E, J. Grimsey. Inet. Min, Met, Trans. 92 2500-2550. (197). (25) You."O, Hsin, V. M. Baev, P. 'V. Gel'd and ML S. Petrushsky. Izv. 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