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INVERSION BETWEEN SPHALERITE. and WURTZITE.TYPE STRUGTURES Ln the SYSTEM Zn-Fe-Ga-S

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INVERSION BETWEEN SPHALERITE. and WURTZITE.TYPE STRUGTURES Ln the SYSTEM Zn-Fe-Ga-S 949 The CanadianMineralogist Vol. 34, pp. 949-958(1996) INVERSIONBETWEEN SPHALERITE. AND WURTZITE.TYPESTRUGTURES lN THESYSTEM Zn-Fe-Ga-S TETICHIUENOI Depamnentof EarthSciences, Fukwka Universiry of Education,729 Akama" Munakata, Fukwl<a 81 141 , Japan STEVEND. SCOTT Departmentof Geology,University of Toronto,Toronto, Ontario MSS 38 I SHOJI KOJIMA Institute of Mineralogy, Petrology and Economic Geolagy, FamJty of Science, Tohoku University, Aoba, Sendai 980-77, Japan ABSTRACT The inversion between sphalerite and wurtzite in the system Zn-Fe-Ca-S was investigatedby dry synthetic phase- equilibrium experiments.In the projection diagrams of the ZnS-FeS-CaS pseudoternaxysystem at 900" and 800'C, the (Zn,Fe,Ga)r-$ solid solution extendsover an extensiveregion from the ZnS composition toward both FeS- and GaS- compositions.At 900'C, this solid solution has the sphalerib structure along the ZnS-FeS join, consistsof a mixture of sphalerite+ wurtzite wherethere is a small amountof GaScomponent, and adops the u/urtzitestructure where there is a greater proportionof the GaSand FeScomponents. A mixed sphalerite+ wurtzite type occursin the GaS-richportion of the ZnS-GaS join and slightly extendingtoward the FeS composition.At 800'C, there is a similar distribution of polymorphswithin the solid-solutionfield, exceptthat the mixed sphalerite+ wurtzite field is more extensiveand includestle entire ZnS-CaSjoin. Heating experimentsshow that the inversion from the sphalerite structure to the wurtzite structure for a sample having composition (ZnS)7e(GaS)3soccurs near 875oC.Reaction rates of this inversion are slow in both directions; the inversion temperaturedepends on the bulk composition(especially the concentrationof cations)and the sulfur fugacity. Keywords:inversion, sphalerite, wurtzite, systemZn-Fe-Ga-S, solid solution,phase equilibrium, dry synthesis. Somuerns Nous avons6tudi6 I'inversion enfe la sphal6riteet la wurtzit€ dansle systbmeZn-Fe-Ga-S au moyen de syntlbsesb sec. Dansles sectionsisothermes du sy$emepseudoternaire i 900oet i 800oC,la solutionsolide (Zn,Fe,Ga)1_rSs'6tend sur un large intervalle de composition,de ZnS vers FeSet GaS.A 900'C, cettesolution solide adoptela structurede la sphaldriteentre ZnS et FeS,un m6langedes structures de sphal6rite+ wurtzite oi la compositioncontient un peu de GaS,et la structurede la wurtzite of les compositionscontiennent davantage de GaSet de FeS.On trouve aussiun champde stabilitf des structues sphal6rite+ wurtzite dans le secteurenrichi en GaS entre ZnS et GaS, qui s'6tetrdl6gdrement dans la direction de FeS. A 800oC,nous trouvonsune r6partition semblabledes structuresdans le champde solution solide, sauf que le domainee sphaldrite+ wurtzite a une plus grande6tendue et inclut I'intervalle ZnS-FeS au complet. Un chauffagede la composition(ZnS)ro(GaS)r6 mdne dl'inversion de la structurede la sphaldriteh la structurede la wurtzite prds de 875"C. Les taux de r6action sont lents dans les deux directions.La tempdraturede l'inversion ddpendde la compositiondu m6lange,particulidrement la concentrationdes cations' et la fugacit6 du soufre' (rraduit par la Rgdaction) Mots-cl6s:inversion, sphaldrite, wurtzite, systbmeZn-Fe-Ca-S, solution solide, dquilibre de phases,synthdse I sec. I E-nnil adlress.'[email protected] 950 TTIE CANADIAN MINERALOGIST Ixrnolucrron investigatorsto reproducethe 1020'C inversion have been unsuccessful,and both sphalerite and wurtzite Sphalerite is a cubic (3C) phase with the space have been synthesized over a wide range of grovp F43m, and wurtzite is a hexagonal(2//) phase temperatures(Scott & Bames 1972). In the system with the space group C6mc. Yaious schemesof Fe-Zn-S (Kullerud 1953,Barton & Toulmin 1966), stacking of the 3-layer cubic and 2-layer hexagonal the inversion temperaturewas found to decreasewittr structuresresult in polytypism in pure ZnS (Smith increasingFeS contentin the (Zn, Fe)S solid solution, 1955, Scott & Barnes 1972). However, synthetic to valuesas low as 850" - 875'C at 56 mol.7oFeS, phasesin the system Zn-Fe-Ga-S contain only the the maximum amount of Fe in this solid solution. end-member3C sphaleriteand 2H wurtzite structures. Scott & Barnes(1972) argued, on the basisof rapid The former is the low-temperaturephase, and the latter reaction-kinetics in hydrothermal systems, that is the phase stable at high temperature. Ga- and wurtzite was not metastably formed in all low- Fe-bearingcompositions of zinc sulfide are therefore temperature ores (e.g., Mississippi-Valley-type phasesof $eat interest to investigate3C-2H stability deposits) and insisted that natural wurtzite must be relations. In this paper, we investigatethe inversion stableunder conditions far below 1020'C.Moreover" between sphalerite-typeand wurtzite-type structures, on the basis of their dry synthesisand hydrothermal based on new experiments, on the results of our experiments, they proposed that the inversion previous phase-equilibriumstudies on portions of the temperatureis a function of sulfur fugacity, with system Zn-Fe-Ga-S (Ueno & Scott L99L, L994, sphalerite being the S-rich phase (Zn1-"S), and 1995), and on heating experimentsof sampleswith wurtzite, the S-poor phase(ZnSl_r). They found that composition(7'S)zo(GaS):0. tlte inversion of sphaleriteto wurtzite proceedsmuch According to the previouswork (Allen & Crenshaw more slowly than the reversereaction, which would l9l2), the inversion temperaturefor pure ZnS is likely lead to sphaleriterather than wurtzite stability near 1020oCat I atm. However, attempts by some where the two phases coexist at low temperatures. TABI! 1. DOERIMEMATRESULTS FoR fiE SYSIEMZIS'FcS'CIS AT 900'C Mol.%sp TABTI 9. D@ERIMEN{IAIRESUL]5 FOR'TllE SvtlEM Zis-&S€as AT 900'C T039 ZnS+FeS+GaS 't913 Run no. Haatlng TM7 ZnS+GaS Sp(Wz){€a T050 FeS{GaS 24 x+Z+Y T064 FeS+9GaS 21 GaS+Z+Y T028 ZnS+2GaS 29 Sp(wz)+GaS+Ga 63.7 T065 sFes+7cag 21 GaS+Z+Y T040 zns+Fes+Gas 29 \lz+Y t@o TFes+gGag 21 X+Po+Y T048 ZnS+GaS 31 Sp(wz)+GaS+Ga 42.7 T067 9FeS+GaS 21 X+Po+Y T051 FeS+GaS 30 Z+X+Y T068 TZnS+3GaS 23 Vtz+Ga T059 FeS+gGaS 33 GaS+Z+Y TNAO gznS+GaS 2 w2(sp){Ga 48.1 T060 SFoS+7GaS 33 GaS+Z+Y T061 TFoS+3GaS 30 X+Po+Y T150 ZnS+FeS+2GaS gFeS+GaS T151 ZnS+FeS+4GaS V+GaS+Y 1@2 33 X+Po+Y 'l't52 T070 TZnS+3GaS 35 Sp(Wz)+Ga s0.4 ZnS+Fe8+6GaS ViGaS+Y '1071 gZnS+GaS Tt6e ZnS+F6S+8GaS 1q GaS+V+Y 35 Sp(Wz)+Ga T154 2ZnS+2FeS{€aS 20 Wz+Y T168 ZnS+FeS+2GaS 44 T155 42nS+4FeS{GaS 20 Wz+Y T169 ZnS+FeS+4GaS 44 V+GaS+Y T156 ZnS+2FoS+GaS 20 W2+Y '1171T170 ZnS+FoS+8GaS 47 GaS+V+Y T157 ZnS+4FeS+GaS 20 VVz+Po+Y 2ZnS+2FeS+GaS 44 w2+Y 1172 44 94.2 Tt58 ZnS+6FeS+GaS W2+Po+Y 4ZnS+4FoS+GaS Wz(Sp)+Y 20 T179 ZnS+2FeS+GaS 44 \ T159 ZnS{€Fes{€aS 2+Y 20 Po+Wz+Y f174 ZnS+4FeS+GaS 47 \ry'z+Po+Y T 160 Wz(Sp)+Y 46.3 2ZnS+FoS+2GaS 20 1175 ZnS+SFsSiGaS 47 Po+Wz+Y T161 4ZnS+FeS+4GaS 20 8p(Wz)+Y 7176 2ZnS+FeS+2GaS 47 wz(Sp)+Y 41.4 I toz 2ZnS+FoS+GaS W2+Y 1177 4ZnS+FeS*GaS 47 Sp(WZ)+Y 83.0 42nS+F6S+GaS 22 UVZ+Y T17A 2ZnS+FeS+GaS 44 VVz+Y T164 62nS+FoS{€aS 22 1j1.12+Y T179 4ZnS+FeS+GaS 47 Wz(Sp)+Y 26.0 I toc SZnS+FoS+GaS 22 V\ts(Sp)+Y 11.4 T180 SZnS*FaS+GaS 44 Sp(Ufz)+Y 51.7 't1d7I too ZnS+2FeS+2Gas 22 Wz+V+Y T181 ZnS+2FeS+2GaS 44 W2+V+Y ZnS14FoS+4GaS Vfz+V+Y 1162 ZnS+4FeS+4GaS 44 T186 22nS+gGaS 2 Sp(Wz)+Ga T199 ZnS+FeS+6GaS 40 GaS+V+Y TI OA i ZnS+FeS+gGag 18 T200 zns+Fes+3cas 40 V+Y+GaS T196 gznS+9FeS+22GaS 18 r20'l gzns+9Fes+22cas 40 T197 I lZnS+l 1FeS+1 SqaS 18 \r{z+Y Im2 1lZnS+11FeS+18GaS 35 V+Y+Vy'z T198 SZnS+gFeS{4GaS \ /z+Y 18 '1210T20g SZnS+€FoS+4GaS 35 V+$lz+Y T205 ZnS+9FeS+10GaS V+X+Y ZnS+gFeS+1oGaS 40 V+X+Y T206 ZnS+7Feg+12GaS 20 V+GaS+Y r21'l'1212 ZnS+7FoS+l2GaS 40 GaS+V+Y r207 ZnS+5FeS+14GaS 20 GaS+V+Y ZnS+sFeS+14GaS 40 GaS+V+Y T208 ZnS+3FeS+l6GaS 20 GaS+V+Y f21S ZnS+gFeS+16GaS 40 GaS+V+Y Sp:Sphalerite, !12: Wuraito, Y: AlloyY,X: PhasoX,Z:Phas€Z Sp: Sphalerite,VVz: Wuruite, Y: AlloyY,X: PhasoX, Z: PhassZ U: PhaseU,V: PhaseV,Po: Pynhotite, Zn: zinc, S: sulfur, Ga: gallium U: PhaseU,V: Phassv Po: Pynhotite,Zn: zlnq S: sulfur,Ga: galllum Sp(VJz):Mhed phasesh whlchsphalerite predominalos Sp(Wz): Mixsd phases in whlch sphalorite predominates Vvz(Sp):Mhsd phasesin whichwurbite prodomlnates V\'z(Sp):Mil€d phas€s in which wurEito predomlnatos INVERSION BETWEEN SPTIALERNEAND WIJRTZTE 951 Kojima & Ohmoto(1991) disagreed and proposed, on In addition to kinetics, the incorporationof several the basis of hydrothermal synthesesand the natural elementsis known to profoundly affect the temperature occunenceof wurtzite, that hydrothermalwurtzite is a of the sphalerite-wurtziteinversion. In hydrothermal metastablemineral formed by rapid precipitationfrom experimentsin the system ZnS-MnS, Talusor.et al. highly supersaturatedsolutions. Kojima (1991) carried (L977) showed that the inversion temperature out wufiite-sphalerite inversion experimentsusing a decreasesto 350oCat a composition(ZnS)TaQvInS)26. solution-mediatedmethod in the temperaturerange In hydrothermal syntheses in the ternary system from 200'to 350oC"and found that the inversionrate ZnS-MnS{dS at 500'C and 1000 atm.
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