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STUDIES of URANIUM MINERALS (VII): ZEUNERITE* Junrrn Worssfnonrnr

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STUDIES of URANIUM MINERALS (VII): ZEUNERITE* Junrrn Worssfnonrnr STUDIES OF URANIUM MINERALS (VII): ZEUNERITE* Junrrn WorssFnoNrnr Assrnlcr X-ray study by the Weissenberg method on zeunerite from Tintic, Utah, gave a space groupPafnmm-Da,Tandcelldimensionsao:7.73A,rs:f.33A,withae:rs:1:1.238.The unit cell contents are Cu(UODz(AsOr)z 8HzO. The calculated specific gravity is 3.79; the measured specific gravity of Schneeberg material is 3.64. Study of synthetic zeunerite indicated the existence of two and possibly three hydrates, one with 16 to 10HzO, one with 8 to 5H2O, and possibly a still lower hydrate. fn this respect the synthetic material is similar to autunite and torbernite, both of which have been found in the fully hydrated form and as lower hydrates, meta I and meta II. Natural zeunerite corresponds in water content and o-ray structure to meta-autunite I and to synthetic zeunerite with 8H:O. Variation in water content afiects both the optical and the fluorescent properties of the material, Zeunerite, from the Weisser Hirsch mine near Schneeberg,Saxony, was named and first describedby Weisbach (1872, 1873, 1877). Since then the mineral has been reported (Hintze, 1931) from at least seven other localities. The only available analysis of the Schneeberg material, made by Winkler (1873), established the composition as Cu(UOr)r(AsOr)zSHzO. The mineral occurs as pale-greento emerald-greentetragonal crystals which usually are rectangular tablets flattened on {001}. The crystal habit closely resembles that of the isostructural mineral torbernite, Cu(UOz)z(PO4)28-12}J2O. The poor quality of the available crystals of zeunerite from Schneebergprobably was responsiblefor the deviation in the later morphologicalmeasurements of Schrauf (1872) from those of Weisbach. Schrauf's elements, which correspond in unit and orientation to the r-ray cell found by the presentauthor, are a:c:l:1.250. An angle table based on his elements is given in Table 1. Crystals from Schneeberg,described by JeZek (1922) as zeunerite, were probably torbernite; the figures he reported for indices of refraction (Table 2) and specificgravity (3.28) are lower than those found by others for zeunerite. An *-ray study by the Weissenberg method (copper radiation) was made of zeunerite crystals from the Centennial Eureka mine, Tintic, Utah. The mineral occurs as tiny tablets associatedwith secondary copper arsenatesin oxidizedlimonitic vein material. The forms c{001}, rnlll}l, P{021}, s{023}, and u{111} were identifiedon the crystalsby goniometric measurements; the poor qualitv of the reflections did not + Published by permission of the Director, U. S. Geological Survey. Contribution from the Department of Mineralogy and Petrography, Harvard Univer- sity, No. 325. 249 250 JUDITH WEISS FRONDEL warrant the derivation of new morphological elements. Rotation, zero- Iayer, and second-layer photographs were taken about the c axis, and rotation and zero-layer photographs were taken about the two possible choices of horizontal axes. The space group was determined as Pafnmm:Dnr,7,it being assumedthat the point symmetry is tetragonal holohedral. No r-ray evidence was found for less than tetragonal sym- metry. The unit cell dimensions are ao:7.13 A, co:8.83 A, with ootco:t:1.238. The unit cell contents are Cu(UO):(AsOr)z SHrO. Beintema (1938) in his work on the structure of meta-autunite I, sug- geststhat only half of the holes in the structure into which the Ca atoms TLnr.e 1. ANcr,n Tlsr,r lon Neruner- ZeuNlt rn oic : l:I.25O;ps;rs: 1 .250: 1 o 001 0"00' 90'00' 90'00' a 010 0"00' 90 00 90 00 45 00 n Ol3 000 2237 90 00 74 13 f o43 000 5902 90 00 s2n+ .po2r 000 68 12 90 00 48 58 i 041 000 78 4r+ 90 00 46 06 Doubtful:m ll0, g 012,s 023,y Ol1,v lll. can be fitted are actually occupied by Ca atoms' This explanation may also serve here and account for the fact that the chemical formula gives only one Cu atom per unit cell although the space group demands that there are two equivalent positions for the Cu atom in each unit cell. The calculated specificgravity for the composition is 3.79. The specificgrav- ity of Schneebergmaterial was redetermined as 3.64. This is probably low, as the crystals contained minute air holes and some inclusions of limonite and the available sample was too small to give an accurate re- sult. The true specificgravity is probably nearer to the calculated value than to that obtainedby this measurement. The r-ray powder pattern data of the Tintic material is given in Table 3. Zeunerite from Schneeberg yielded identical patterns. The presenceof arsenicin all the specimensexamined was verified by qualita- tive tests. The indices of refraction, newly measuredon this material to- gether with the previously reported measurements,are summarizedin Table 2. The observedvariation in the indices of refraction suggeststhat the composition of zeunerite varies in some respects' Possibly there is isomorphous substitution of (PO+) for (AsO+) causing a reduction in the STUDIES OF URANIUM MINERALS VII: ZEUNERITE 251 indices of refraction toward those of torbernite; no analvtical work has been done to determine whether this is so. Hallimond (1916, 1920) has shown that torbernite forms three differ- ent hydrates: torbernite, meta-torbernite f, and meta-torbernite II. Beintema's work (1938) gave similar information for the isostructural mineral autunite. The water content of each hydrate is in part zeolitic and variable between limits depending on the humidity and temperature. The present study of synthetic zeunerite has shown the existenceof at Tnnr,n 2. Oprrcar, Dere ron N,rrunar, ,tNl Svxtrmtrc ZnuNrmrr Ail uniaxial negative (-) nO nE Natural zeunerite From Schneeberg* 1.647 From Schneeberg+ r.647 From Schneeberg* 1.642 From Schneeberg* 1.640 From Eureka mine, Tintic, Utah* 1.647 From Eureka mine, Tintic, Utah+ 1.643 Majuba Hill, Nevada* 1.645 Hintze (1931) 1.651 1.635 Millosevich (1912) 1.629 Jezek (1922) 1.585 1.576probably torbernite Larsen and Berman (1934) t.643 r.623 Synthetic zeunerite With 16HrO r.602 With 10HrO I.610 with 8H2o 1. 645-1 .648 with sHro 1.654 + In the Mineralogical Museum, Harvard University. least two, and possibly three, hydrates of the copper uranium arsenate' The synthetic material was prepared according to Winkler's (1873) method: freshly precipitated copper carbonate was dissolved in excess arsenic acid, and to this solution uranium nitrate was added, which pre- cipitated the hydrous copper uranium arsenate in distinct but small crystals, less than 0.01 mm. in diameter. Two Penfield water determina- tions on the fully hydrated material gave 16 molecules of water. After standing in air overnight, the material had dehydrated to 10HrO and apparently had reached equilibrium. Heating in an oven caused no further loss of water until 65o C was reached. At this temperature the material dehydrated to 8HzO'and stayed in equilibrium up to 85'C. 252 JUDITH WEISS FRONDEL Tarr,n 3. INrrnpr,.q.x.q.nSpacrxcs lnou X-Rav Powonn P,trrnnNs (A) Cu/Ni radiation:1 5418 A. Synthetic zeunerite Natural zeunerite Fully hydrated (16HrO) Dehydrated to SH:O 8HrO J* 10.65 10 8.76 8.93 10 6.86 5 6.56 1 5.04 8 5.95 1 2 5.47 5 5.54 6 3.59 9 5.04 4 5.04 3 .39 7 r'. tq 3 4.35 .t 3.18 z 4.15 1 3.07 I 3.71 9 3.72 9 2.93 4 3.55 7 J.JO 7 2.86 4 3.28 8 3.30 8 2.73 J 3.12 1 ) qa. A 2.99 J 3.01 2.47 4 2.75 2 2.77 2 )47 1 2.67 2.7r 2 2.38 L 4 2.59 ? 2.31 2 Z.JL 4 7<) + 2.27 J 242 J 2.42 2.19 / 229 1 2.30 I 2.O8 2.24 2 2.26 2 1.985 1 2.18 2 2.19 2 |.926 o 2.15 2 2.15 2 1.873 2 2.08 J 2.09 4 r.797 1.994 J 2.01 4 1.768 I 1.922 I 1.937 1 1.734 1 1.841 1 1.855 1.704 2 1.784 J r.797 J I .658 1 |.746 1 1.749 2 1.642 4 1.689 I 1.695 1.610 3 1.637 2 1.656 4 1.590 I 1.600 2 1.605 3 1.563 1.566 o |.570 I.JJJ r.486 1.512 1 1.451 1.429 J 1.423 1.429 z 1.382 J 1.400 1.406 2 1.365 J 1.375 1.382 3 I.JJZ 1 1.354 1.358 2 I.JIJ 2 7.324 1.329 2 1.298 I 1.281 1.290 t-275 1.262 1.265 1.248 z 1 111 1.247 1.222 I t.224 1.225 1.211 2 1.208 1.209 1.202 2 1.175 2 1.176 t.tgl 1 1.160 I 1.161 I 1.181 1 1.127 1.130 I 1.168 n 1.118 1.143 2 I .088 1.092 I 1.118 I t.077 1.094 z 1.065 I 1.086 z 1.060 1 * Intensities estimated visuallv. STUDIES OF URANIUM MINERALS VII: ZEUNERITE 253 From this temperature up to 1050 C the material lost water slowly but continuously and finally reached equilibrium with 5H2O. This hydrate, however, is not stable under atmospheric conditions; after standing in air for one day it had rehydrated to SHrO.
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