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Synthesis and Fluorine.Hydfoxyl Exchange in the Amblygonite Series

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Synthesis and Fluorine.Hydfoxyl Exchange in the Amblygonite Series Caiwdian Mineralogist Vol. 14, pp. 357-363 (1976) SYNTHESISAND FLUORINE.HYDFOXYLEXCHANGE IN THE AMBLYGONITESERIES SPENCER E. LOH,|, ^rxn WLLIAM S. WISE Departmentof Geologicalsciences, university of california, santa Barbara, ca 9|106 ABSTRACT Souurernr, The amblygonite series includes the solid solution La s6rieamblygonite consiste en une solution solide between the end members, amblygonite, LiAIPO;F, entre les p6les extr6mes,I'amblygonite (LiAlpO4F) and montebrasite, LiAIPO4OH. The moit comrrion et la mont6brasite (LiAIPO4OH). La compositionla composition range. is between Ambl6 and Amb5o, plus courante que I'on retrouve dans les pqmatites where this series occurs in Li-rich pegmatites. richesen Li se situe entre Amble et Ambrol Ih com- The end members and four intermediate composi- positions limifss st quatre compositions interm6_ tions were synthesized by standard hydrothermal diaires ont 6t6 synttr6tis6espar voie hydrothermale d tochniques at 600'C and 2 kbar water pressure. All 6@'C et 2 kbar de pressiond'eau. Tous les six para_ six ell param€ters vary linearly across the com- mdtresde l4 maills varient de fagon linGaire. positional I-es ai_ range. Amblygonite cell dimensions arg mensionsde la maille de I'amblygonite sont, a 8.103, a p 5.103, b 7.221, c 5.5064, a L14"22" 98.54'. b7.22L,c 5.506[, aLl422t, p 98.b4',^y 6ZTfz'iww t 67'02'; and montebrasite, a 5.185, b 7.161, c mont6brasite,a 5.185,b Z.t6I, c 5.OOA, 5.040A, a ll2"I8" B 97"51" .t 67"52'. These !t c 112"18r, cell P 97%It, Les paramOtresae cescomposGs dimensions indicate that the unit cells of the pure purement!.97"52'. Li litliques sont un peu plus petits que-ceux series are slightly smaller than those of the des natural min6raux naturels. Les indices de r6-fraction mineral se.ries. Refractive indices are €ssen- coincident tially identical essentiellementavec ceux des min6raux with comparable natural minsrals. naturels. Les Equilibrium compositions compositions d'6quilibre de la phase . of ttre amblygonite phase amblygonite dans la r6action in the exchange reaction : d'6changeLiAlirO4F LiAlpO4F + ffrb *HzO:LiAIPO+OH*HF ont LiAIPO4OH $ HF were approached 6t6 ipproch6s des from both sides, deux c0t6s i faide des membres extrbmes using pure synthetic end members as starting syntl6- ma- tiques purs commemat6riaux de d6part. Les compo- terials. Gas compositions were controlled bi solid gazeuses The sitions ont 6t6 contr6l6espar des solutions F"flg=. results, z6-5 for several levels of Jnr, can tamponssolides. the equilibrium Les r6sultats,,Aab pour les diff€rents F"jl^t" constant in the fonn, log niveaux de/gp, peuvent K.-319:' : 4.58 (+O.22) : (Jnr/uzo) 6tre adaptdsd la constanre : los + log d'6quilibrep{ log Klongff: -4.58 (+0.22) : [(l - re*),/ra-rl which allorrs calculation gas loc of Ay/Ia2Q * loe - ,cA-)/ra^b] ce qui permet compositions for natural amblygonite compositions [(1 le calcul gazeusespour les-composi- beyond therangeof tJrebuffers. If AGIAZ' 0 and -des_compositions LG,/L P 5O, tions d'amblygonitesnaturelles au deli des soluiions as in the LiF-LiOH exchangereaction, tampons. Si :a thenlog I( : - f000/?("K). AG"/AI 0 et LG"/LP = 0, comme dans la r6action d'6change : - Equilibrium constants at pegmatitic alors log K OCf/ temperatures ?('K). Les constantesd'6quilibre, are very small, indicating strong i dis temp6ratures fractionation of pegmatitiques, sont trds petites indiquant F into-the amblygonite phase. Isothermal ainsi un crystalliza- fractionnementde F dans la phaseamblygonite. tion of amblygonite will cause a decrease in La tle f cristallisation isothermique de I'amblygonite abais- content of the gas, and crystal zoning will be toward montebrasite sera le contenu en F du gls, et la zor^;tlondu cristal compositions. Znung with increases sera dans of F content la direction d'une augmentationen mont6- result from (l) increases in fo, ac_ brasite.Une zonationqui comFanying increases in gas pressure d6montreune augmentation caused by en F r6sultera (1) d'une haussesen qui silicate phase crystallization and/or (2) /rc,, ac@m- by decreas_ pagne I'augmentation de la pressiongazeuse caus6e ing temperature leading to smaller' e[uilibrium par constants. la cristallisation de silicates et/oa (2) d'un abais- sement de la temp6rature menant i des constantes d'6quilibre plus petites. (fraduit par le journal) INTRoDUCTToN 'rPresent Arnblygonite series address: Department of Geological polytechnic Sciences, Virginia Institute & State A continuous, isomorphous series exists be- Univ., Blacksbury, VA 24061. tween the end members,amblygonite, LiAlpO4F, 357 358 TTIE CANADIAN MINERALOGIST mole o/o F 40 60 vt o(, c E (,5 (, a o C' c wt. 7o F Frc. 1. Histogram of the compositions of natural memben of the ambly' gonite series from data compiled by Loh (1975). and montebrasite, LiAIPOcOH. Genqrally, the Ginzburg 1950; Gallaghet 1967; Connolly & name amblygonite or amblygonite series has O'Hara fgZg; ff"i*ich & Corey 1955; Cern6 been used to representany member of the series. et al- 1972). Neither pure amblygonite nor montebrasite has C,ern6et al. (1973) presenteddetailed physicat The highest reported been found in nature., properties on twenty analyzed latural -ambly- mole %) fluorine content is 11.8 vtt. Vo Q2 lonite minerals. Specific gravities, -refractive from Saxony (Moss ef aI. 1969) and the lowest indices, and differential thermal behavior all is 0.85 wt. % Q mole Vo) from Siberia (Vlasov show gradual changes with F-content. X-ray 1966). Figure 1 illustrates the compositions of powdei diffraction methods provide- efftcient all the reported occurrences of amblygonite and ind accurate means for the indirect determina- montebrasite, 80Vo of which have less than tion of F content. T:he 2A(CuKa') values for the 50 mole Vo fluoine. Sodium is the most com- (131) reflection (Moss et aL 1969) shory line.ar mon minor element replacing lithium, in changes with the fluorine content in amblygonite amounts averaging near 0.5 mole Vo. mineials. The determination line was refined by The members of tlis series occur chiefly in eernd et al. (1973). lithium- and phosphate-rich granitic pesmatites, commonly as ellipsoidal nodules or crude crys- Purpose of the studY tals up to 0.5 m in a paragenesissimilar to that has been done of spodumene(Moore 1973). The perfect {100} Since little experimental work cleavage and milky-white colot often lead to on this minglal-ssrigs, pure end members and confusion with the feldspars. The minerals most intermediate members of the amblygonite series commonly associated with amblygonite a,re have been synthesized to investigate some of spodumene, apatite, lepidolite, tourmaline, and the physical properties and to test the complete- other lithium phosphate minerals. Amblygonite o.r. of th" solid solution. Comparison of proper' has also been found in high-tempetature veins ties of the synthetic and natural minerals will and greisen with cassiteriteo topz, and mica. help to further define the mineral series espe- The minerals of the amblygonite series have ciaily for the end members. More important is been found at the famous pegmatite localities the determination of the relationship between of Varutrask, Sweden; Karakhstan and Siberia, the F content of the amblygonite and the lm of USSR; Montebraso France; Rhodesia; Black the pegmatite magma. In this paper we p,resent Hills, South Dakota, Eight Mile Park, Colorado; the properties of a series of synthetic amblygon- Pala, California; Newry, Hebron, Buckfield, ites.-and we show that most amblygonites crys- and other localities in Maine; and Tanco Peg- tallize from fluids with very low lr-less tlan matite, Bernic Lake, Manitoba (Quensel 1956; 0.005 bars. SYNTHESIS OF TIIE AMBLYCONITE SERIES 359 TABLEl. CoMPUTEDoENSITIES, CELL DII4ENSIoNS, Cu{dl(131) At'lDMEASURE0 I-REFRACTM INDEX 0F SYNTHETIC AMBLYGONITE,MONTEBM5ITE, AND lTS INTERMIDIA1EI.{EMBER5L nnt amb20 amb40 amb6o ambgo amb a (i) 5.r85(6) 5.r75(?) 5.r67(r) 5.r5l (3) 5.134(2) 5.130(3) b (i) 7.r6r (e) 7.164(21 7.r7r (3) 7.175(6) 7.213(6') 7.221 (5\ c (i) 5.o4o (5) 5.042(2) 5.047(2) 5.045(4) 5.056(3) 5.056(4) o ll2" 18(6)' 112.37(2), il2.57(2), r13023(4)', r14" 3(4)', 1r4. 22(4)', 6 97'5l(8)' e8' o(2)' e8" 3(2), e8" r5(4)' e8" 42(41' e8. 54(5)' 't2(2)' | 67.5217)' 67o 46(21', 67" 42(z)' 67" 30(3)' 67. 67" 2(3)' v (i)3 roo.q(z) 15e.8(6) 15e.3(7) 158.1(r) 157.6(r) 157.r(r) densitv (caIc.J r'uzu 3.041 3.058 3.089 3.108 3.t 26 i;i;:i' 52.22" 52.42" 52.58" 52.84" 53.07. 53.23' i:ll:ll 52.23" 52.40. 52.57" 52.85" 53.07" 53.?4" 1-index 1.643 (l) 1.634 (l) 1.622 (1) 1.612 (l) 1.603 (l) 1.592(1) SyNtnnsrs or Mntvtusns oF THE Complete X-ray powder patternsz were ob- AMBLycoNrrn SrnIEs tained for each composition, and the unit-cell using the U.S. Geolo- Experimental procedure dimensions were refined gical Survey's FORTRAN IV computer pro- The end members and four intermediate gram W7214 (see Table 1). Linear regxessions compositions of the amblygonite series were of each parameter are given in Table 2 with prepared from mixes of the proper proportions the compositions expressedboth as mole Vo F of LiF, LiOH.HIO, and AlPOa.l Approximately and wt. 7o F, which may be compared directly 30 mg of mix and 15 mg of water were sealed to those developed by Cern6 et aI. (1973). The in 2 cm long and 3 mm diameter gold tubes. values of 20(l3L) for each composition and The synthesizingruns were conducted at 600"C and 2000 bars water pressure in standard, ex- 2Copies ternally heated, cold-sealpressure vessels.Tem- available from the authors.
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