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F. J. Wicks E. J. W. Whittaker Canadian Mineralogl*t VoL 13, pp.227-243(1975) A REAPPRAISAL OF THE STRUCTURES OF THE SERPENTINE MINERALS F. J. WICKS Mineralogl Depa.rtment' Royal Ontario Museum, Toronto, Canada E. J. W. WHITTAKER Departrnent of Geology & Mineralogy, Oxford Unlversity, Oxford, England ABSIRACT and compression,it is suggestedthat it is the cona' pression of the octahedral sheet that buckles the The three theoretical stacking schemes for tri- Mg plane so that the Mg atoms occupy two posi- octahe&al l:1 layer silicates developed independent- tions at different levels. This disturbance of the ly by fteadman, Z'tpgin' and Bailey all assume structure in turn tilts the tetrahedra in the way ideal hydrogen bonding between successive layers, that is observed. In chrysotile the curvature only with polytypes developed through shifts of :tal3, partly relieves the mismatch, and evidence is pre- !b/3 or zero, and rotations of 180o or zero. The sented for a similar buckling itr this structure, three systems contain 16 distinct polyty?es, and though to a smaller extent, This postulated buckl- Bailey's nomenclature is extended to provide sym- ing explains some hitherto obscure features of the bols for each one. If lizardite is redefined to in- structure. Antigorite appearsto overcompensatethe clude all serpentines with flat-layer structures, these mismatch in the direction of curyature, but it has can be designated as lizardite followed by the ap- an anomalouslythick octahedral sheet which is propriate polytype symbol. still unexplained. The above system cannot be applied to the chry- sotilo structures because the sbifts between the layers show that the normal hydrogen bonding INrnooucrroN position is not achieved. The layer stacking de- pends on tle fact that the basal oxygens form two sets, differing in e, and tle lower one lies rn the Because of their frequent sub-microscopis, groctves between, and the upper one over the ridges fine-grained texture and close chemical relation- formed by, the underlying hydroxyl rows. This ships, an adequate classification of the ser- stacking principle leads to a series of polytypes for pentine minerals was delayed until structural which an analogous nomenclature is proposed. information became available, and this was using subscript c to denote their essentially cylin- itself delayed by the unusual curved layersosu- drical character. Thus clinochrysotile, orthochry- perlattices and disordered stackings that occur sotile Zvyagin's clinochrysotile be- and l-layer these minerals. It was not until 1956 that come 2Ma, 2Or"1 ar.d lM"r. The term in chrysotile by Whit- parachrysotile is retain_ed to describe the cylindrical work on the structures of chrysotile structure with a 9.2A fiber axis. The alternating taker (1952, 1953, L954, I955a, b, c, d, l'956a, wave structure of antigorite, with layer inversions b, c, 1957) and by Jagodzinski & Kunze (L954a, and interconnections between successive layers at b, c) and of antigorite by Zussman (1954) and the inversions, destroys the possibility of systematic Kunze (1956, 1958, 1959) was advanced suf- hydrogen bonding and makes the stacking depen- ficiently for a viable classification to be put for- dent on the primary bonding at the interconnections, ward (Whittaker & Zussman 1956). polytypes so that it cannot be discussed in terms of This classification divided the serpentine min- of either kind. into three structural groups based on A review of the substitution in natural and syn- erals rylin- (chrysotile), thetic chrysotiles and lizardites indicates that there drical layers cornrgated layers is a compositional overlap between curved and flat- (antigorite) and flat layers (lizardite). Chryso- layer structures. Thus, as all flat-layer structures tils was further sub-divided into three varieties, caq b€ regarded as polytypes of-lizardite and all clinochrysotile, orthochrysotile and parachryso- oylindrical structures with a 5.3A fiber axis can tile. Antigorite was soon found to occur with be regarded as polyty?es of chrysotile, lizardite and a range of superlattice periods (comrgation chrysotile are polymorphs. Compositional data for wave-lengtls) from 16-110A as well as the parachrysotile poly- are lacking. Antigorite is not a original 43A @rindley et aI. 1958; Chapman & morph of the other serpentines because it has an Zussman 1959; Kunze 1961). Sub-division of (though slightly) different composi- essentially only the flat-layer serpentines was necessitated by tion. of varieties with a 1-layer cell Because the mismatched tetrahedral and octahe- the discovery dral sheets in lizardite are respectively in tension and a 2-layer cell @ucklidge & Zussman 1965), 227 228 THE CANADIAN MINERALOGIST a 6layer cell (Zussman & Brindley 1957; Zuss- The purpose of the present paper is to discuss man, Brindley & Comer 1957; Olsen 196l; tho differences between the internal structure of Miiller 1963; Krstanovii & Pavlovid 1967), a the layers of the main divisions of the serpen- 6- (pseudo 2-) lryer and a G (pseudo 3-) layer tine minerals, and to relate them to one another cell (Gillery 1959; Bailey & Tyler 1960), a 3- and to other trioctahedral 1:1 layer silicates in layer cell (Coats 1968) and a 9-layer cell (Jah- terms of structure and crystal chemistry, and anbagloo & Znltai 1968)4. It has since become in this connection to develop further the dis- evident from the work of Zvyugn (1967) that a cussion of Olsen (1961) and Radoslovich fourth variety of chrysotile, L-layer clinochryso- (1963b). The relationships of these structural tile, must be added to the three chrysotiles of features to the chemical differences that have Whittaker & Zussman's classification. been treated previously by Faust @ Fahey OnIy two serpentine varieties have come to (1"962r, Page (1958), and Whittaker & Wicks light whose relationship to the three-fold classi- (1970) are also discussed.However, before pro- fication has been in doubt. One h the splintery ceeding to this discussionit is desirable to con- serpentine @ovlen-type) found by Krstanovis sider the relationships of the layer stacking of the & Pavlovii (1964) which they suggestedto have serpentine minerals to the polytype classifica- a modified clinochrysotile structure. More re- tions of Steadman (1964), Ztyagln (1967) and cently Middleton (1974) has investigated this Bailey (1967a, 1969) for 1:1. layer silicates. further and found Povlen-type clinochrysotile to Some sonfwion has been introduced into the be composed of chrysotile-like layers. He has literature by attempts to fit the serpentines into also found a Povlen-type orthochrysotile whose these classifications, which are not in fact di- structure he has interpreted as an intergrowth rectly applicable to the serpentine structures. of chrysotile and lizardite-like layers. The other serpentine variety is an unusual serpentine from THEoRETTcALPor,yrypns the Tilly Foster mine, New York (Aumento 1967,) which may be o very intimate mixture of Three theoretical stacking schemes for tri- clinochrysotile and antigorite. octahedral l:1 layer silicates have been de- veloped in recent years by (i) Steadman (1964), (i) Zvyagin, Mischenko & Shitov (1966) and Zvyagin (1967) and. (iii) Bailey (1967a, t969). *Jahanbagloo & Zo.ltai (1968) analyzed what they The terminology developed by the called a bexagonal Al-serpentine with a 9-layer tri- various auth- gonal structure and a composition of (Mgr.o"Al."n- ors differs and so do their basic assumptions, Fe.sr)(Si!.a7Al.$)Ou(OH)n.However, as this composi- so that the same series of polyty,pes is not de- tion is closer to the amesite end of the lizardite- veloped in each system, although there is con- amesite solid-solution eries this qrecimen will be siderable overlap (Table 1). The full details of called amei{te .9? in this paper. the procedures are given in the original papers TABLE I. A CMAiISOII OF POLTYPES Sbatun (1964) ZvFgln (1967) Bailey (1969) [email protected] Layers lnter- h€dml [xlendd SF@ ln Unlt hyer Strlcture Group Struchre S!ructurc ilodifi- Group Poljdse hlley hup CelI Shlfts X@b€r fl@r Nmber Typ€ catlon Xmnclature hla/3 17 tl 1 Bl[Atil1t4 &2a/3 t8 z 41 Nl a1 P3t 3 a./3 19&20 3&4 3T 3T 3Tt C@2, 2 al3+r tt l1 I c20 B 20r 2Or n9! n.l 2 at3+r 2&3 equlvalent & 2h 2 al3rr 4 4" 2i2 az ''l ot 5 5 al3+r 5&6 5H 6H 6Ht P3l0 I ilone I I A]TCIT'IT B3bl3 2&3 | &2 3T 3R 3R P3lc 2 b/3 a 3 2rnzl P63@ 2 flon*r 9 vIr I D 2ts D 2Ht 2Ht P6: 2 b/3+? l0 & ll ll 2&3 2H 2H2 2HZ k 6 b/3+r 16 v1 l fr 6R 6Rr 86 ilone,r/3 4&5 lfflnitles rlth 6&z P33 ttane,.b/3 6&7 &lley Group C 312 B 6 ltondr t2 & 13 .tflnltles !ilh bl3rr P6" 6 llon+r _ t4 I t5 Bijley Grolp ! 6lz b/3+r liere fu strlciure nders according b stedfun or zvyagln arc glven on one llne, they corrcspond to enanfiomrohs A REAPPRAISAL OF THE STRUCTURES OF THE SERPENTINE MINERALS and a Cetailed comparison of the methods is -----n? given in Wicks (1969). ? 9---o a; '- For purposes of generating th,e various poly- o; oMs' 'ho i i types, the three systems assume an ideal tetra- -.. hedral sheet with hexagonal symmetry, linked O .,P @t O A through the apical oxygens without distortion to an ideal trioctahedral sheet with trigonal sym- €*, A fr+ tr- ,O metry (Fig. 1). Stacking of successivelayers is a o'fez o '/ o then assumedto occur in such a way that hydro- gen bonding always develops between every ba- of @*,,,,Qo i sal oxygen of a given layer and the outer hy- "ig--- ----o--- o--- o--- -- --€ droxyls of the adjacent layer (see Fig. 2 of Bailey 1969).
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