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Crystal Chemistry of the 2*Ivl2* 6Z$Oc

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Crystal Chemistry of the 2*Ivl2* 6Z$Oc American Mineralogist,Volume 70, pages 171-181,1985 2*Ivl2* crystal chemistry of the 6z$oc)zl sheet:structural principles and crystal structures of ruizite, macfallite and orientite Pe,ul B. Moonn, JrNcnue,u SuBNI eNo Tereuenu Anerr2 Department of the GeophysicalSciences The University of Chicago Chicago, Illinois 60637 Abstract The crystal structures of ruizite, CarMn]*1OH)2[Si4Oil(OH)2].ZH2O,monoclinic, a=9.064,b:6.171,c:11.9764,F:91.38',spacegroupC2lm,Z:2,R:0.084for1546 independe-ntFo; macfallite,CazIr,tnS*(OH)3[SiO4Si2O7], monoclinic, a : 10.235,b = 6.086, c:8.9704, F:ll0.75",spacegroupP2ylm,Z:2,R=0.l84for2437independentFo;and orientite,Ca2Mn2+Mn]+(OH)4[Si3Oro], orthorhombic, a : 9.074, b = 19.130, c : 6.121A, spacegroup Bbmm, Z : 4, R : 0. 156for 1238independent Fo, havebeen approximately determined. Structure disorder (domains, intergrowths) and/or solid solution probably affect these structures; and true single crystals of these and related compounds are very infrequently encountered. Ruizite, macfallite, orientite, lawsonite, sursassite,ardennite, pumpellyite, santafeite and bermanite all are based on the same fundamental building block, a sheet 3tttti*16(fO izl, Q : anion not associatedwith a tetrahedron,n : vacancy.This sheet is basedon a layer of the spinel structureprojected down [ 11]giving the 3tM1*d2OO4)21 sheet with maximal two-sided plane group symmetry lp3mll, as found in chloritoid. Ordered vacancies lead to the fundamental building block in this study with plane symmetry lc2lml. Alternatively, the chain component of the fundamental building block (f.b.b.) is IttvtS*(Or)u(d2l where { usually is OH-. A variety of interchain tetrahedral polymers can occur and many explain the disorder in these structures. Introduction Structural principle Although many of the mineral crystal structures are The underlying principle is a two-sided plane, a section presently known, the principles behind them are rarely of the familiar arrangementof spinel, Al2(MgOa),normal applied, and a holistic structural genealogy is woefully to [ll]. In our model, the symbol M refers to cationic lacking. Much of the inability to evolve a structural speciesin octahedral coordination (in this case Al3+.;and genealogystems from the difficulty of applying graphical T refers to the cationic speciesin tetrahedralcoordination enumeration to these problems, and the problem of (in this caseMg2+). For spinel, a : 8.14, this arrange- choice:just which part of the structure should be empha- ment has t1 %rt a 5.7A and h : 13 sized?We chooseto demonstratethat a fragment-in this h :9.94.It is an orthogonalcell and hasbeen extensive- case a two-sided slab.-is common to several crystal ly exploited for structures derived from spinel by selec- structuresof minerals, and may afford a unifying genealo- tive site orderings. This arrangement is a sheet with gy among these compounds.The list is by no means composition 3[tr,trOr(too)2], maximal point symmetry exhaustive: the compounds selected were those with $ZtmY witn two-sided plane group piZlm. The nearest reasonablyrefined crystal structure parameters. Briefly, orthohexagonalmonoclinic subgroup of this would have the compounds occur in regimes of low to intermediate point symmetry lZlm\ and two-sided plane group c2lm. temperature, and low to high (cf. lawsonite) pressure. Table I outlines the crystal chemical characters of these 6 x 9A sheet structures. called such becausetheir axial translations approximate these integers. Of the ten ' representativestructure types, only the structure of san- X-ray Laboratory, Graduate School, Wuhan College of 'tafeite Geology,Beijing, China. is unknown. It is inferred to belong to this group 2 Department of the Geological Sciences, University of Illi- and an approximateformula is given. Earlier, we attempt- nois, Chicago, Illinois 60680. ed to solve its structure but it appears to be twinned, in 0003-.004)vE5/0I 02-0 I 7 I $02.00 t7l t72 MOORE ET AL: STRUCTURES OF RUIZITE, MACFALLITE AND ORIENTITE Table l. Crystal-chemicalcharacters ofthe 6 x 9A sheet structuresr Specles g(i) b(i) !-(l) g spqceGrcup t,/tl Trc-slded Dlam Reference l{a0z(T0r ) z '1.740 Chlori told Fe(tI )rAl(0H)rlAt 30r(si04)rl 5.47 18.19 l0l,57' CZlc p3ml Theoreti cal lt't.Oz(TOr)zl,splnel ap = 8.'| A tr = 9:21 \2-fJlL=W lPill, c2ln] |.732 ' czln MzBz(TOt) r Lawsonlte 4 cafA'lz(0H)z(Slz0r)].H20 5.80 8.83 13.20 Cmm 1.522 c2/n Sursassite 2 iln(il)rlAlr(0H)3(St0{)(sir0?)l 8.70 5.f9 9.78 108.87 P2 ln I.503 P2ln '1.499 Ardennlte 2 iln(II)+Mgr(0H)rtAl {(0H)+(Aso.) (st0r)r(st r0to)l 8.71 II E' Pnm Pzln 4 Pumpellylte 4 Carr'rglAlr(0H)r(sl0r)(Sir0z)l 8.81 5.94 19.t4 97.60 Az/n 1.483 Pzlil orienti te 4 caro(Hr0)rlr4n(III)z(Oft)u(si r0ro)l 9.01 19.13 6.12 Bbm 1.482 bzln o ihcfal I i te 2 carllln(Itl)3(0+r)r(si0r)(siz0z)l 10.23 5.09 4.97 t10,75 P2tln 1.473 PZln Ruizite 2 cartr,|n(tII)r(0H)z(str0rr(0H)z)l.2Hz0 9.05 6.t7 11.98 91.38 Czln 1.158 czln Santa fe i te 4 a. [hrca(0H)zll.tn(IIr)r(0H)s(v0+)a].H20 9,25 O.JJ 30,00 C222r(pseudo ?) 1.461 cz Bemnite 4 iln(II)(H,0)rtrh(III)z(0+l)z(P0r)zl 6.22 8.93 ra 25 C222r(pseudo) 1.436 cz tspecles are arranged according to decreasing trltr ratJo. Cell edges of the f.b.b. are underllned. The spacegroups of bemnlte and posslbly santafelte are the trlnred groups. The tm-sided plane refers to the f.b.b. 'ln the structures. lHarrlson and Brlndley (1957). zRumnova and Sklpetrcva (1959). 3lGlllni and flerllno (1982). 4Donnayand AllEnn (1968). scottardi (1965). 5Thls TSun study. and $leber (1958), wlth !and gaxes lnterchanged. sKampf and t'loore (1976), after transfomtlon a = [l0l], l = [lOi], c = [OI0]. ilote B" 90.250, much the same fashion as bermanite. The actual space repeatswas not required. This adds somecredence to the group of bermanite is P21, but twinning usually leads to M2nd2GO4)2unit as a fundamental building block. The the C2221spacegroup (Kampf andMoore, 1976).Ruizite, direction normal to this sheet is the basis of a variety of formerly proposed as Pztlc by Williams and Duggan tetrahedral polymerizations, as we shall see. (1977), is C2lm for our crystal from Kuruman, South Figure 2a is a construction of the idealized Cllm sheet Africa. The "theoretical" structure, which is included in showing the important symmetry operations. Note that the M3@2(TO+)z (d : arbitrary symbol for an anion) all populated octahedraare basedon the unit M(Or)+(d)2, subgrouping, would be a slab of the spinel stmcture where @ are in trans arrangement with respect to the normal to the [111]direction. The spacegroup P3ml for this two-sided plane includes the orthogonal component of CZlm as a subgroup. The sheet of cubic close-packing is the basisfor the ratio tzltt : tfltt : 1.732. An outline of the P3ml, ar = 6A, arrangementis presented in Figure 1. This sheet consists of rows of populated octahedra alternating with rows of insular octahedra and the tetrahedra. Chloritoid actually pos- sessesthis slab as the [AlrOz(SiO+)z]unit and distortions lead to monoclinic or triclinic symmetry, but the tzltt ratio is close to V3. If rows of populated octahedra alternate with rows ofoctahedral voids and the tetrahedra,then the formula M2!6(TO4)2 obtains, where ! is a vacancy. This arrangement is an ordered subgroup of P3zl. Its maximal space group is CZlm. The most pronounced distortion in these structures arises from cation-cation repulsion effects across the shared edges-and a subse- quentdiminution in the t2ltl ratio. lf a = 9A and b : 6A, then t2lt1: 1.50,close to the average1.482 for the nine structure types of M2!+2(TO4)2. The range is 1.545 to 1.428for these compounds.No attempt was made to x transform the cell criteria in Table l. Rather, the 6 9A Fig. l. Sheet of 3[M3dr(To+)z] showing some of the axes were underlined and the ratio was derived directly symmetry elementsin space groupPlml and the unit cell outline from knowledge of the structure and orientation of the with a1,a2- 6A.Some symmetry elements m,7,2,21 andaxial octahedralchains. All the structures approximatethe 6 x glides are shown and are slightly offset to ease visualization of 9 module, and division or multiplication of these axial the sheet. MOORE ET AL: STRUCTURES OF RT]IZITE, MACFALLITE AND ORIENTITE r73 Fig. 2a. sheetof 3[Mrf]hToq)) showinsm,10),1e),2,2, anda-axial glides in spacegroup C2lm, the ordered subgroup of Fig. 3. The hypotheticalstructure built of cis-M@2Oao P3nl. This is the fundamentalbuilding block for the structures octahedra.The symmetry elements m,I areshown and the space in the text. The axesare approximatelya : 94, b : 64. groupis P2lm.The axes are approximately a = 4.5Aand b: 64. octahedralcenter. Monoclinic same-cellsubgroups of this lar orbital for /Mn3* in high spin configurationforces the spacegroup include trans arcangement,but this does not rule out the crs arrangementfor some isotropic cation, say Al3+. Alm --> C2 --->P2, P2r In every structure involving Mn3+ (orientite, macfal- l\ ..+pm lite, ruizite, bermanite), a common feature of polyhedral I r- distortion appears: the polyhedron is elongate with PZlm, P2llm 4Mn3*-O ca. l.%A and 2Mn3*-O ca. 2.21A, with t6l14n3+-6= Often, it is more convenient to project the structure down 2.024 average(Table 2).
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