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Natroapophyllite, a New Orthorhombic Sodium Analog of Apophyllite I

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Natroapophyllite, a New Orthorhombic Sodium Analog of Apophyllite I American Mineralogisl, Volume 66, pages 410-423, l98I Natroapophyllite,a new orthorhombic sodiumanalog of apophyllite I. Description,occurrence, and nomenclature HtRou.lnu MATSUEDA Institute of Mining Geology Akita University, Akita 010, Japan YesuNoRr Mrun-e.' eNo JoHN RucrrDce Department of Geology, University of Toronto Toronto, Ontario MsS IAI, Canada Abstract Natroapophyllite NaCaoSirO2oF' 8H2O, a sodium analogof apophyllite,has beenfound in white skarn at the SampoMine, Okayama,Japan. Electron microprobe analysisof the min- eralgives SiO252.79, CaO25.4l, NarO 3.05,K2O 0.33,F 2.27,HrO (by difference)l7.ll weight percent;(-O=F' : 0.96).Optical and crystallographicparameters are: a: 1.536(2),B : 1.538(2),y: l.5tA(2),2V(meas.):32(l)",r<v;a:8.875(4), D:8.881(6),c: 15.79(l)A, spacegroup Pnnm,Z : 2; D obs. : 2.50,D calc.: 230 g/cm3. The crystal structure,refaed (R : 0.056)by least-squaresmethods from 563 ditruseX-ray reflectionscollected with an automatic single-crystaldifractometer, has rings of SiOotetra- hedra. Ca- and Na-polyhedra are more distorted in natroapophyllite compared with apo- phyllite becauseof the substitutionof Na for K. TGA showsdiscontinuous water loss of 16 weight percent, similar to apophyllite. DTA and IR data suggestthat natroapophyllite has hydrogen atoms in three di-fferent structural environments. A pseudosolid-solution series exists between natroapophyllite and fluorapophyllite which bridges the orthorhombic-tetragonalsymmetry change.Crystals are shown which display continuousand discontinuouszoning. Introduction and Rucklidge, 1979).The Na-rich examplesare in- The nomenclatureof the apophyllite group is com- variably orthorhombic and fluorine-rich, and the proposed plex. Fluorapophyllite and hydroxyapophyllite have name natroapophyllitehas been for this so- recently been defined by Dunn et al. (1978) as the dium analog of the orthorhombic apophyllite de- valid names for the end members of the tetragonal scribed originally by Sahama (1965) and Belsare apophyllite series,in which K is the major alkali cat- (1969).It is not the sodium analog of ordinary tetra- given ion. Orthorhombic varietiesof apophyllite have also gonal apophyllite. The name natroapophyllite, been described.Sahama (1965) gave details of an or- in allusion to its compositionalrelation to apophyl- thorhombic fluorine-rich apophyllite KCa.AlSi, lite, was approvedby the IMA Commissionon New 1976. OroF'8HrO, which containedsignificant Al. Minerals and New Mineral Names in October, prefixes would Although Na may substitute for K in apophyllite Other additional for natroapophyllite to a small degree,samples in which Na predominates be in order, e.9.,ortho- and fluor-, but in the absence over K have only recentlybeen described (Matsueda, of non-orthorhombicor other than fluorine-rich nat- 1975,1980; Miura et al., 1916;Miura, 1977;Miva roapophyllite, it seemsunnecessary to burden the lit- erature with more complex names than natroapo- phyllite, orthorhombic I On leavefrom Departmentof MineralogicalSciences and Ge- which is defined as being the ology, Faculty of Science,Yamaguchi University, Yamaguchi753' sodium end member of the apophyllite group miner- Japan. als with the formula NaCaoSi'OroF'8HrO. 0003-004x/8I /030+04 l 0$02.00 410 MATSUEDA ET AL.: NATROAPOPHYLLITE Fig' l. Optical micrographsof natroapophyllitefrom the Sampo Mine. (a) Compositecrystals of typical natroapophyllite(SA-lb) and fluorapophyllite(SA-la). SA-l samplesare up to 0.15 x I mm. (b) Compositenatro- (SA-2a)fluorapophyllite (SA-2b) crystalsand intermediatecompositions (SA-2c, d, e). Sampledescriptions, physical properties, and generationby the granite intrusion (Matsueda,1980). morphology The white skarn was formed by fluorine metasoma- tism of ferrobustamite and wollastonite-andradite The four samplesdescribed here have SA-numbers skarns (Matsueda, 1980). In transmitted light the referring to the Sampo Mine, some l0 km west of grains of natroapophyllite are invariably rimmed by Takahashi City in Okayama Prefecture.The Sampo apophyllite (Fig. l), which suggeststhat a pseudo Mine is one of the typical contact metasomaticore solid solution exists between apophyllite and nat- deposits of the Chuhgoku Province and was em- roapophyllite, in which there is a transition from te- placed at the contactof Paleozoiclimestone and slate tragonal to orthorhombic symmetry.This would rep- with Late Cretaceousgranite (Matsueda, 1973, 1980). resent a range of chemical variation beyond the Natroapophyllite occursin associationwith zeophyl- solid-solution series fluorapophyllite to hydroxy- lite, cuspidine,apophyllite, and calcite in the 'hrhite apophyllite reportedby Dunn et al. (1978)and Dunn skarn" on the 9th level, No. I Yoshiki Ore Body of and Wilson (1978). the mine. Other associatedminerals include andra- Natroapophyllite samplesSA-l to 3 in Table I oc- dite, xonotlite, wollastonite, a clinopyroxene in the cur as minute prismatic euhedral to subhedral crys- diopside-hedenbergiteseries, magnetite, quartz, and tals up to 0.15x I mm (Figs.I and2), brownish-yel- native bismuth, all of which occur in banded zones low to yellowish-brown (in SA-l and 3) or colorless betweenthe granite and marble contacts.Natroapo- to white (in SA-2). The luster is vitreousto pearly. A phyllite was found in the white skarns close to the typical exampleof natroapophyllitein SA-l is zoned marble contact(Matsueda, 1973, 1980). The fluorine- with fluorapophyllite, and the two phases are re- bearing silicates zeophyllite and apophyllite crystal- ferred to in Table I as SA-lb and SA-la, respec- lized during a hydrothermal alteration stage,which tively. Compositecrystals exhibit {100} prisms trun- occurred after the thermal metamorphism and skarn cated by the {l I l} dipyramid striated perpendicular 4t2 MATSUEDA ET AL: NATROAPOPHYLLITE Table l. Occurrences,parag€nes€s, compositions, and optie axial anglesof fluorapophyllite and natroapophyllite from the Sampo Mine SpeciEen No. Occurrence Paragenesis Alkalj- contenE* 2V(neas.) Kt SA- la Whlte skarn Zeophyllite, calcite, . o8Nto.ozc"4. t3 '1 I SA- Ib (9L No.1 Yoshiki ore Body) andradite, f luorite, cuspidine Ko.o6Nto.9oc"4.13 Ko -?l SA-2a .03*"0. 86c"4. 08 Kr >>0 SA-2b . olNto.02c"4 . 09 Druse in white skarn llagnetite, andradite, SA-2c Ko. >0 (9L No.1 Yoshiki Ore Body) fluorite 4oN"o.z8ct4 . oo 1 SA-2d Ko.85Nto. roca4. 16 Kt SA-2e . ogN"o.o3c"4. ol Ko. =30 SA-3a o7N"o.75c'4. r2 White skarn Fluorite, xonotolite, SA-3b Ko.45Nuo.5lct4. 1 (9L West No,I Yoshiki Ore andradite, magnetite, cuspidlne l2 SA-3c Body) *o.95Nto.03c"4. zo j.n >0 sA-4 Spherical skarn marble t3 (10L l{rest. No.l Yoshiki Fluorite, andradite "o.9oNto.o3ct4. Ore Body) * Atonic z'atios of aLkali ions on the basis of Si = 8.00. to the c axis (Fig. la). SpecimenSA-2 is subdivided to that offluorapophyllite (Figs. I andz) because,as 2a-2e for varying compositionsin the rangenatro- to shown below, the crystals are compositeswith the fluorapophyllite.It exhibits well-developedfl I U di- rims being K-rich fluorapophyllite and the cores Na- pyramids with {100} prisms which give the samplea rich natroapophyllite.Optical measurementcould be "fish-eye" appearance(Figs. lb and2\. The external morphology of the crystalsis sinilar 'fish Fig. 2. Scanningelectron micrographs of natroapophyllite(SA-2a). (a) Subhedralcrystals of SA-2 showing eye' appearance.(b) Euhedral crytsalsof SA-2. MATSUEDA ET AL.: NATROAPOPHYLLITE %.\ Oo(41) @ o(41)o ox) si (1) Qc'rzl ,a Ca(l) .J O o(41)OI !"-els' Fig. 3. The Si6O2ssheet in natroapophylliteprojected on (001). mademost reliably on specfunenSA-l in which the K amountsof calcite and fluorite is 2.50,and the calcu- and Na phasesare easily distinguished. The Na-rich lated value is 2.30. Natroapophyllite is slightly sol- component is colorless in thin section and distinctly uble in l: I HCI and 1: I HNO3. biaxial with 2V(meas.): 3211;o,r 1 via : 1.536(2), B : 1.538(2)and y : 1.54r'r(2\.The K-rich com- Chemistry ponent is uniaxid with the propertiesof normal fluor- The chemical compositions of the natroapophyllite apophyllite, ar : 1.536and e : 1.539(see Table l). and fluorapophyllite crystals were determined with Biaxial examples of the K-rich component are also the JXA-5A electron microprobe analyzer at Kytrshtr noted in Table l, but the detaileddescription of these University. The analyses, which were performed at phaseswill be reservedfor a separatepaper. l5kV acceleratingvoltage and l5nA samplecurrent, Cleavageis perfect on {001} and poor on [ll0]. are shown in Table 2, along with a list of the stan- The Mohs hardnessis 4 to 5, and the streak is light dards used.Water was determinedby difference.No gray. The mineral does not fluoresce in UV radia- other elements besides those listed were detected in tion. An IR spectrumof natroapophylliteis shown in either form of apophyllite from the Sampo.Mine. Part IL The powder usedfor this was carefully sepa- Wet-chemical analysis of somewhat impure material rated from the K-rich fluorapophyllite parts of the including a small amount of apophyllite from the crystals. The spectrum shows two sharp peaks at same locality was performed by Dr. K. Ishibashi of 3560 and 3420 cm-' and one broad peak at 3020 Fukuoka University, using weight loss on ignition. cm-'. Thesecorrespond to two strong and one weak The resultsare HrO(+) : 15.83and HrO(-) : 0.14 hydrogen bonds (see Part II). The specific gravity, weight percent.An analysisof the most Na-rich spec- measuredby the suspensionmethod in Thoulet's so- imen (SA-lb) with 3.05 weight percent NarO
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