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Mineralogy of the Zippeite Group 433

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Mineralogy of the Zippeite Group 433 C anadian M ine raloei.st Vol. 14, W, 429436 (1976) MINERALOGYOF THEZIPPEITE GROUP CLIFFORD FRONDEL Department of Geological Sciences,Hamatd University, Cambidge, Massachusetts JUN ITO James Franck Instilute, University ol Chicago, Chlcago, Illinois RUSSELL M. HONEA 1105Bellatre Street,Broomtield, Colorado ALICE M. WEEKS Department of Geology, Temple University, Philadelphia, Pennsylvania ABsrRAcr en trois groupes, chimiquement et aux rayons-X, selon qu'ils contiennent: K ou NHa, Na, ou un The ill-defined mineral zippeite and a number cation divalent. De nombreuses solutions solides of zippeite-like minerals, hitherto supposed to be existent entre pOles i cations divalents, mais non hydrated uranyl sulfates, are found to contain one K et Na. Le compo# correspondant au p6le Na or another of various monovalent or divalent ca- est orthohombique avec a 8.80, b 68.48, c 14.55L; tions in addition to uranium. They correspond to tous ces min6raux possddent une m0_me pseudo- syntletic phases with the formula l"(UOr6(SOrg maille avec 4 -8.8. b -17.1, c -7.2L. (OH)ro.yHgO, where A is K, Na or NHa (with La nature chimique de la zippEite type de Joa- .r-4 and y-4) or Co,Ni,Fe2+,Mna+,Mgln (with chimsthal (J. F. John 1821) n'est pas connue. Un r=2 and y-16). All are structurally related but min6ral analogue, d6crit par R. Nov6dek (1935) et three subgroups are indicated by X-ray and ch€m- provenant de la m0me localit6, est identifi6 corrme ical evidencel the K and NHa members, the Na potassigueet est consid6r6 comme n6otype. D'autres member, and the divalent cation members. Extensive phases naturelles ont 6t6 identifides; ce sont les solid solutions exist between the divalent cation zipp6ites de sodium (la plus commune), de cobalt, members but not with the K and Na members. The de nickel, de maen6sium et de zinc. Un min6ral Na member is orthorhombic with 8.80. a , 68.48. alt6r6 repr6sente probablement la zipp6ite de fer. c 14.55A; all of the members relaied to are an Les efforts faits pour synth6tiser les zipp6ites de orthorhombic pseudocell -8.8, -17.L, with a 6 Ca et de Cu ont 6t6 vains. c -7-24. Clraduit par la R6ddction) The chemical identity of tle type zippeite of J. F. John (1821) from Joachimsthal is not known. A INTRoDUCTIoN similar mineral described by R. Nov6Cek (1935) The fint uranium sulfates found in nature from the same locality is identified as tle K mem- ber and is taken as the neotype. Other identified were recognized by the German chemist J. F. natural phases include sodium-zippeite (the com- John in 1821.. At that time the only otler known mon member), cobalt-zippeite, nickel-zippeite, mag- uranium minerals were the species subsequently nesium-zippeite and zinc-zippeite, An altered min- called uraninite, torbernite and autunite. John eral probably representing the iron member also described and qualitatively analyzed an emerald occurs. Efforts to synthesize the Ca and Cu mem: green uranvitriol and a yellow earlhy basisches group bers of the failed. schwefelsiiures uranoxyd from Joachimsthal, SorvrvrernB Czechoslovakia. The uranvitriol later was de- scribed crystallographically and named johan- La zipp6ite, min6ral mal d6fini, ainsi qu'un cer- nite by Haidinger (1830). The yellow earthy tain nombre de min6raux analogues, 6taient consi- sulfate was named zippeite* by Haidinger (1845) d6r6s jusqu'ici comme des sulfates d'uranyle hydra- but without further description. t6s; ils s'avdrent contenir, outre l'uranium, I'un ou I'autre de diff6rents cations monovalents ou diva- Minerals attributed to zippeite have since Ients. Ces min6raux correspondent aux phases syn- th6tiques l"(JOr)0(SOJa(OH)ro.)HzO, of I est Il Na ou NHa (avec r=4 et y=4) ou bien Co, Ni, *A memorial of Frantiiek X. M. TipW GlSt- Fe2+, Mnz+, Mg Zn (avec x=2 et y=16). IIs sont 1863), Czech mineralogist, is given by Kettner tous apparentes par leur strucfure, mais se classent (l963). 429 Downloaded from http://pubs.geoscienceworld.org/canmin/article-pdf/14/4/429/3445649/429.pdf by guest on 25 September 2021 THB CANADIAN MINERALOGIST been found at numerous losalities but their This included members found here to be iden- study has been attended by nany difficulties. tical with various natural zippeite-like rninelals. In part this has been caused by the very fine- The latter have been named zippeite (the K grained and admixed uature of the material and member of the group), sodium-zippeite' cobalt- by the quite limited samples available for zippeite, nickel-zippeite, mapesium-zippeite and analysis. The main source of trouble, holvever, zinc-zippeite. These names have the approval bas been the long-standing belief that the min- of the Commission on New Minerals and Min- eral was a hydrated uranyl sulfate. It is now eral Names of the I.M.,\ fouud that the earlier analyses were incomplete, and that the minerals and synthetic compounds METHoDS oF SYNTHESIS hitherto loosely grouped around the name zip- peite contain one or another of various mono- Zippeite-type phases were precipitated fron valent or divalent cations in addition to the acid solutions containing uranyl sulfate to- uranyl ion. gether with sulfates of K, NII+ Na, Co, Ni, The earlier ilrrrmary accounts of natural and Fe'+, Mn2+, Mg or Zn. Precipitation was ef- synthetic so-called zippeite by Nov6Cek (1935), fected at room temperature by the addition of Traill (1952) and Frondel (1958) constitute a NILOH (or NaOI{) to solutions containing composite description of a group of related sub- divalent cations and of KOH, NaOH or NIIIOH stances.They believed tle mineral to be a hy- to solutions containing the corresponding mono- drated uranyl sulfate. This situation gave rise valent sulfates. Experimentation established to complications during the 1950's, a period of that the phases are pri:cipitated in acid solutions active study of tle mineralogy of uranium, when over a wide range of molar ratios and con- supposed uranyl sulfates falling within the range centrations. Control of pH is essential. In gen- of properties attributed to "zippeite" were found eral, if a dilute alkaline solution is slowly added at many places. Some of these substances were dropwise with vigorous stirring, bringing the tentatively referred to by new names, such as pH up to 4.O4.2, a precipitate will form on the meta-zippeite, meta-zippeite-I, meta-zip- standing for hours or days. Under these condi- peite-Il aud beta-zippeite mentioned by Gruner tions only a small proportion of the dissolved et al. (1954) and othen. A few occurrencesbe- cations is precipitated. If the precipitation is ef- came known informally by the name of the fected at somewhat higher pH, becquerelite or mine in which they were found, such as "Happy other phases in either crystalline or amorphous Jack zippeite" and 'Ilcky Strike zippeite". form may coprecipitate. With regard to the identity of the original The rapid addition of the alkaline precipitant, mineral from Joachimsth4l,Nov6dek (1935) did depending on its normality and the vigor of not succeed in finding type specimens of John's stirring, may locally give a relatively high pH material and based his description and micro- with accompanying immediate precipitation of chemioal analyses of zippeite on certain non- becquerelite. This may then redissolve slowly. type specimens from the same locality. He The rather divergent ratios of UOa to SOg re- thought that the rather variable material repre- ported in some analyses of synthetic material sented a series of hydrated uranyl sulfates. may be due to admixture of becquerelite. Uranyl Frondel (1958) obtained three of tlese speci- sulfate solutions that are nearly saturated with mens*, found them to be similar to a syn- the monovalent or divalent sulfates, and that thetic compound reported to be a hydrated have an initial pH below 3, generally yield satis- uranyl sulfate, and described this material as factory results. zippeite-proper with the composition 2UOg' The use of NaOH in precipitating the divalent SOa'5HzO. cation and K members often results in the co- Following the recognition early in the present precipitation of the Na mernber. This precipitates study that certain synthetic zippeite-like pre- fust and may then be followed, on standing, by parations contained K as an essential sonstituent, the divalent cation compound. The Na msmber two of Nov6dek's specimens and the earlier is commonly admixed in natural material. analyzed synthetic compound were re-analyzed The particle size of the precipitates tends to and found to be a potassium uranyl sulfate. An increase with time when left in the mother extensive program of phase synthesis was then solution, but crystals large enough for single- undertaken that led to the recognition of a crystal study could not be obtained even after large group of structurally related compounds. several months. In general the particle size in- creases with decreasing pH at the level' of precipitation and with increasing dilution. Zip- *Kindly supplied by Dr. Karel TuCek of the Na- peite-type phases genfsining Ca or Cu could tional Museum in Prague. not be synthesized. Downloaded from http://pubs.geoscienceworld.org/canmin/article-pdf/14/4/429/3445649/429.pdf by guest on 25 September 2021 MINBRALOGY OF TIIE ZPPEITE GROUP 431 Gnoup DEscRIprroN X-ray methods failed because of the very poorly crystallized nature of the precipitates. Extensive The composition and properties of the mem. mutual substitution between the various divalent bers of the zippeite group are summarized in cations is indicated in natural material. this section. Details of the individual members are given in following sections. X-ray crystallography Chemicql composition X-ray study indicates that all of the mem- bers have identical or very closely related The 8 chemical analyses of natural and syn- structures.
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