Clay Min. Bull. (1964), 5, 338. THE IN OF S1TU SOME FORMATION KAOLINITE AND DEVELOPMENT MACROCRYSTALS L. R. M O O R E Department of Geology, University of She)field Read 8th November 1963 ABSTRACT: Tonsteins, which are kaolinite-rich rocks with an amorphous groundmass containing much organic material, occur widely in European Coal Measure deposits. The nature of these rocks and their peculiar fabric is considered in detail and evidence is adduced which suggests that they were derived from soils and that the original organic components (micro-organisms and fungi) played a significant part in the formation of the kaolinite macrocrystals. INTRODUCTION Rocks referred to as Tonsteins are well known within the European Coal Measure Basins; they occur within the coal seam or in the accompanying fireclay or roof shales. The term merely signifies an argillaceous rock, but a structural significance has become implicit in that it indicates a well-consolidated homogeneous rock, often with conchoidal fracture and distinct from thinly bedded or fissile shale bands which may have a similar relationship to the coal seam. These rocks vary in colour from dark brown or black, to grey or white, and are usually thin (1-3 in.) but very exceptionally may reach a thickness of 3 or 4 ft. An account of their nature and occurrence (Moore, 1963) has also reviewed the literature concerning their study. The importance of Tonsteins follows from the remarkable regularity of their occurrence at definite horizons in the succession of Coal Measures rocks and hence their value in correlation within a coalfield, or as a means of correlation between disconnected coal basins. Their recognition, apart from physical characteristics, also depends upon a content of kaolin-type minerals, first noted by Termier (1923) who referred to the presence o f the mineral 'leverrierite.' This distinctive mineralogical characteristic led to an impetus in their study and SchiJller & Grassrnan (1949) identified both "leverrierite' and kaolin, whilst Grim (1953) later suggested the term 'leverrierite' should be discontinued and referred to kaolin alone. The 338 Kaolinite macrocrystals 339 habit of the kaolin present led to a mineralogical classification (Schtiller, 1951) in which the rounded forms or boules characterized the 'Gruppen' type of Tonstein, whereas prismatic and vermiform kaolin macrocrystals served to identify the 'Kristal' Tonstein. Upon this basis, and in conjunction with consideration of other mineralogical constituents, the Tonstein bands are separately identified and used in stratigraphic subdivision. Many workers attracted by the mineralogy, physical characteristics and widespread lateral occurrence of these rocks have considered the problems of genesis. Thus, the ash of forest fires, finely degraded felspathic materials deposited as sediments (Termier, 1923; Pruvost, 1934), and kaolin derived f r o m weathered fireclays (Teichmtiller, Meyer & Werner, 1952) have been considered. Other authors (Stach, 1950; Petraschek, 1942) sought the source in volcanic ash, whilst Scheere (1955) believed that, under certain physico-chemical conditions in shallow water environments, kaolin would be formed from fine-grained sediments consisting of mica- or illite-type clay minerals, Schtiller (1951) and Hoehne (1954) thought the rocks originated from alumina-rich aqueous solutions or gels deposited within the peats. Although Tonsteins occur rarely, their distribution is widespread within the Carboniferous and Permo-Carboniferous coal-bearing rocks of the northern and southern hemispheres (Moore, 1963). Their frequent occurrence within coals, or in close association with a coal seam, suggests an origin connected with the process of peat formation, development, and possibly with erosion. This relationship is substantiated in records of their presence within Tertiary coals. The chemical composition of these rocks (Pruvost, 1934; Scheere, 1955; Hoehne, 1951) shows a significant range; those most typically developed and with the physical characteristics enumerated above are often very pure and consist mainly of silica and alumina. In general terms the SiO2 may range from 35 to 50% with A1203 30 to 45%. The high SiO2 and A1203 is characteristic, and although MgO, CaO, Na20, K20 are invariably low each may range from less than 1% to 2-3%. The iron content is variable, but often low, whilst fractional percentages of MnO, and P205 may be present and TiO2 is frequently around 2-3 %. The amount of H20 is generally in the range 10-15% and the organic matter content is very variable. The analyses of some of the purer Tonsteins are directly comparable with kaolinites such as that from Murfreesboro, Arkansas, U.S.A., which contains 97-2% kaolin. Despite the apparent homogeneity, the lack of bedding and the conchoidal fracture, minor structures, such as included lenses or wedges of darker or lighter coloured material, are often visible in hand specimens. Flow structures, sometimes emphasized by broadly folded curves of included organic material, indicate an originally plastic medium. 340 L. R . Moore In thin section a pale yellow or brown groundmass is present. This may form, e.g. in Tonstein from Erda, a very high proportion of the rock with extensive and relatively continuous distribution and little other mineralogical content than kaolin macrocrystals, although there is invariably some organic material. In other Tonsteins, e.g. Graziella, the groundmass is more restricted or patchily developed. Included within it or separating individual areas are larger masses of organic matter and a range of minerals which may variously include quartz, mica, clay minerals, pyrite, anatase and kaolin macrocrystals. The groundmass, particularly that of the former type, consists of small rounded ill-defined floccules (seen best with partially crossed nicols)and carries small dark cells (1 t0 or colonies of such cells which resemble bacterial colonies; in places larger cells or chains of cells and fungal hyphae are present. The groundmass is predominantly amorphous and isotropic and is colloidal in nature. Rotation under crossed nicols presents a patchy clouded effect with a suggestion of linear arrangement which might be due to streaming double refraction (Baver, 1956). The original consistency was that of a gel, paste or aggregate of plastic material composed largely of alumina and silica together with an organic content of degraded humic material and included micro-biological remains. This resembles the composition of a mixed organicinorganic soil colloid and by processes which include dehydration and separation of the mixed colloid the kaolin macrocrystals develop within the groundmass. GENESIS OF SOME TONSTEINS The study of a large number of European and British specimens has shown that a feature common to all is intense aerobic microbiological degradation of the organic matter. The microbiological details have been described (Moore, 1963) for the German Erda Tonstein. This evidence is important in assessing the conditions under which the rocks were formed and provides information on the chemical composition of the rocks and of the processes leading to the kaolinite content. The recognition of micro-organisms simulating bacteria, fungi and actinomycetes, and analogous to those of a soil population, when taken in conjunction with other physical and chemical properties leads to the conclusion that these rocks were formed as soils. By analogy with modem tropical soils of comparable chemical and kaolinitic mineralogical constitution the method of formation might have been as podzol or 'lateritic type soils' (Mohr & Van Baren, 1954; Van der Merwe, 1949) or by other processes already described (Moore, 1963). Mohr & Van Baren (1954) describing podzolization processes in tropical forest Kaolinite macrocrvstals 341 profiles, referred to the formation of a mottled clay in the A horizon. This mixed colloidal kaolinite-iron-oxide hydrate complex was loose, spongy and pervious to air and water in the non-dispersed state. With leaching of the iron, kaolin and kaolinitic materials remained and the consistency became plastic, tough and impervious. Many authors including Robinson (1949), Mohr & Van Baren (1954), Joffe (1949) and Baver (1956) have described soil colloids containing the trihydrate gibbsite, kaolinite and related minerals as forming important constituents of podzols and lateritic soil types. A consideration of literature on the environment of kaolin formation is instructuve in indicating the conditions necessary for the formation of kaolinite-rich soils. Ross (1943) stresses the stability of kaolin as an end product associated with other stable minerals, and indicates that it is formed in conditions where leaching is effective and where strong oxidation of organic matter by an active soil microflora working in a humid climate produces humic acids. Mohr & Van Baren (1954) consider humic acids play a major r61e since they not only control pH but are also effective in removing bases. Keller (1956) has discussed the influence of various environments on the formation of clay minerals. With regard to kaolinite he considers the environment as a 'chemical microclimate' controlled by factors such as the biota, concentration of active ions, oxidation potential, temperatures of the reacting system, relationship to ground water and the nature of the water environment, e.g. lacustrine or marine. Kaolin formation requires excess H+ and the removal of Ca2+, Mg/+, Fe3+, Na+ and K+ (in fact all cations other than aluminium and silicon) from a permeable substrate with strong leaching by water that must not be stagnant. The high AI:Si ratio leads to the removal of silica which is stabilized in solution by Na+ and K+, and iron if present must be removed from the system by oxidation to oxide or sulphide. The conclusions of Nord & Vittucci (1947) and Nord & Schubert (1961) are pertinent in considering the part played by microbiological organisms in these processes. They studied the chemical nature of the microbiological attack on cellulose by fungi and showed the enzymatic action to be one of hydrolysis which by stages resulted in acetic, oxalic and related acids from simple decomposition. Mohr & Van Baren (1954) state that bacteria, actinomycetes and fungi are all concerned in the mineralization of organic matter. Bacteria are principally concerned with initial breakdown of organic matter whilst the fungi convert the material into new compounds which remain in the soil. The micro-organisms require only limited air or oxygen but are nevertheless also dependent upon the presence of some calcium, magnesium and potassium as essential metabolic elements. The same authors referred to the effect of pH on microbiological 342 L. R. Moore activity, and state that below a critical value of pH 4.5 bacterial activity ceases, the optimum range lying between pH 5.5 and pH 7.5. Fungi, however, are dominant members of a soil microflora at pH 3"5-5.5 and can flourish under extremely acid conditions. These authors conclude that the critical pH value of 4-5 which limits bacterial activity is normally indicative of a low level of mineral plant foods, such as calcium, magnesium and potassium, and below such a limit organic matter accumulates and peat formation occurs. This critical pH value is also significant in other ways for in sub-aquatic soils Mohr & Van Baren observed the constitution of the soil colloid to be kaolin plus silicic acid. This fact is in accord with the experimental evidence of Mason (1960), who noted a marked change in the relative solubilities of alumina and silica at a pH of about 4, at which value alumina is readily soluble and silica only slightly soluble. Within the pH range 5-9 the solubility of silica increases and alumina becomes practically insoluble and remains to form lateritic soils and bauxites. At a pH of 4.5-5.0 iron forms complex soluble compounds with organic matter (Mohr & Van Baren, 1954) and given adequate sub-surface drainage iron may be removed from the system and is deposited as concretions at lower levels or removed to greater distances. By analogy with these known conditions in modern tropical soils it is possible to make suggestions concerning the environment under which the Tonsteins were formed. That the medium was acid is indicated by the predominance o f fungal attack and that it was conducive to metabolic activity is demonstrated by the continued attack upon groundmass organic material; thus the medium provided the minimal requirements o f atmospheric or dissolved oxygen, and essential quantities o f calcium, magnesium and potassium for metabolic activity were also present as shown by analyses of these rocks. The pH was therefore above 4-5 and ranged nearer pH 5.5-7 with high humidity and presumably high temperatures. Rainfall, possibly of a monsoon type, with a fluctuating water table was adequate for leaching--but since the SiO2 : AlzO3 ratio and kaolinite content decreases with increasing rainfall (Mohr & Van Baren, 1954) this would not be excessive. For Hawaian soils developed from the same parent rock material at 500 and 1000 mm rainfall, respectively, the optimum SiO2 and A1203 percentages in the composite colloid were 43.92% SiO2, 31.33~o A1203 and 40.25~o SiO2, 33.04% A1203. These observations make it possible to integrate the various biological and physico-chemical requirements which were conducive to the formation of the mixed inorganic-organic colloidal complex, constituting the original gel-like material of the Tonstein. They illustrate also the bio= chemical and biophysical nature of the environment, in which the Kaolinite macrocrystals 343 macrocrystals of kaolin developed and provide a basis for the consideration of crystal development described subsequently. D E V E L O P M E N T OF K A O L I N I T E M A C R O C R Y S T A L S The smallest recognizable crystalline areas with a vitreous appearance are ovoid in plan, lens shaped, and range between 2 and 10 t~. Larger examples simulate the 'boule' or Gruppen habit and either include coccoid cells, filaments and fragments of organic material, or this material is in part present on the surface. The organic material may be irregularly distributed, partly radially arranged, or distributed in a concentric manner. The inorganic matter is similarly arranged and optically is only partially crystalline, consisting of isolated or separated crystallites. These crystalloid or semi-crystalline mineral aggregates and their associated organic matter have already been illustrated (Moore, 1963) for the Erda Tonstein. Other Tonsteins exhibit these characteristics to a more marked degree, and the organism Anthracomyces cannellensis (Renault, 1900) is included within the 'boule' from the Hermance Tonstein (Fig. 2a). Tabular crystals of kaolinite in thin plate-like forms are common; they do not exhibit a preferred orientation and are frequently seen in juxtaposition over a considerable size range. Their in situ development results from the reorganization of the constituents of the mixed inorganic and organic colloidal groundmass and takes place in what are considered to be developmental stages in the formation of the macrocrystal. Initially over the rectangular area of a developing crystal the groundmass appears lighter in colour and the poorly defined borders merge into the groundmass without suggestion of crystal growth pressure at this stage. The organic content of this area consisting of bacteria-like cells, fungal hyphae and small carbonaceous fragments, is either extruded to the surface of the developing crystal or is included within it but shows a minimum of orientation. At a later stage the inorganic matter, though still of only a partially ordered nature, forms lamellae approximately at right angles to the long axis of the crystal. The organic material is disposed in prominent planar fashion on the surface of the crystal and between the lamellae in the position of cleavage planes of the macrocrystal (Figs. la and lb). With increasing organization of the kaolinite and consequently with developing crystal pressure at the margins, the macrocrystal assumes a definite crystal outline. The outline may then be marked by a rim of organic material, either extruded from the developing crystal margin, or resulting from compression of the groundmass parallel to the crystal margin. The planar distribution of organic matter may be uniform and regular throughout the macrocrystal, but is more commonly impersistent. Further reorganization of the cry- 344 L. R. Moore stalline material takes place from local centres within the macrocrystal boundary, with the development of lens-shaped crystalline areas o f uniform optical properties. The consequent displacement of surrounding organic matter by crystal pressure results in discrete patterns of organic and inorganic material. The reorganization is frequently less regular and a spherical crystalline mass with radially arranged optical properties resembling the 'boule' habit may occur within the tabular macrocrystal. The included organic matter of the macrocrystal is then compressed and displaced in sweeping curves around the developing crystalline mass (Moore, 1963). Very few completely formed tabular crystals without organic content are seen, but such as are observable have less developed cleavage and more uniform optical properties. The vermicular macrocrystals vary considerably in size and occur as simple curved crystals, or as forms with amazing complexity. Their development follows the trends described above for tabular crystals, but the form is vermicular even at the earliest stages and the groundmass is reorganized in this form. Thus the small vermicular crystals do not show marked planar distribution of organic matter, but the larger vermicular crystals exhibit marked planar distribution of the bacterialike cells, filaments, and fragments of organic matter in the cleavage directions (Figs. lb and le). This direction is at right angles to the long axis of the crystal at a given point. Where large wood fragments are incorporated into the crystal f r o m the groundmass, reorientation is often not affected and the fragments (Fig. lb) lie at angles across the cleavage. Similar features concerning local centres of reorganization within the macrocrystal and the formation of a definite crystal outline are noticeable: alignment of the groundmass parallel to the margins o f the vermicular crystal (Fig. lc) is a common feature. Fie. 1. (a) Constance Tonstein x 500. Tabular kaolinite macrocrystal showing planar orientation of organic matter in direction of cleavage planes, between inorganic larnellae. (b) Hermance Tonstein x 500. Tabular kaolinite macrocrystals joined at right angles. Note general alignment of organic matter, and position of non-aligned larger wood fragment. (c) Hermance Tonstein x250. Vermiform kaolinite macrocrystals. Note (i) alignment of groundmass parallel to borders of macrocrystal at lower margin of figure; (ii) planar distribution of orgalaic material within main macrocrystal, and incipient development of rounded 'boule' on its lower border; (iii) dark zone of organic material in groundrnass with little (or longitudinal) orientation of contents, also wedge-shaped area indicating flow and compression ofgrourzdmass between crystals; (iv) small amount of orientation in the upper crystal and smaller amount of included organic material. Kaolinite maerocrystals 345 346 L. R. Moore There are many other irregular forms which masses of macrocrystalline kaolinite may assume and which appear to be various combinations o f the three previously described habits. These occur more commonly in restricted or irregularly shaped areas of groundmass and in those rocks with a greater amount of organic matter present as large entities. A common form depicted in Fig. 2b has an irregular rounded but crenulate margin suggestive of plastic flow conditions. The margins o f such crystalline areas are well defined and the adjacent groundmass shows compressional features. Optically there is a lack of uniformity and incipient crystallization with patchy extinction indicates a radial direction of the crystallites developing from several individual centres. The included organic matter is similarly oriented in a very general radial direction and intersects the margins at right angles--a direction at considerable variance to that of similar organic matter in the surrounding groundmass. Fig. 2c illustrates the complexity of other kaolin macrocrystalline masses, and shows the very considerable changes in the direction of alignment o f the organic matter over a small area. It is clear that this alignment is in part due to the development of the separate kaolin macrocrystals and that there is no preferred orientation resulting from external causes during macrocrystal formation. Some degree o f directional control appears to have been exercised upon the form of the resulting macrocrystal by the nature or manner of distribution of the organic content :included within the groundmass. Thus in Fig. 2c the wood fragments along the upper margin controlled the direction of the developing crystal at this point and the organization of the degraded material and hyphae associated with it suggests a form typical of the degradation of tracheid material. This is strikingly so in the lower part o f the figure where the fungal remains represent a 'Phellomyces' pseudomorph after tracheid structure (Moore, 1963). The curved remains have led to the development of a vermicular crystal, with a breadth that FIo. 2. (a) Hermance Tonstein x 650. 'Boule'-like form of kaolinite containing colonies of Anthracomyces cannellensis arranged in partly radial manner; these may have contributed to the aggregation and form of the kaolinite mass. (b) Constance Tonstein x 250. An irregular form of kaolinite. Represents part of a continuous succession of such forms, suggestive of plastic flow. Note radial and lateral orientation of included organic matter, sharp contact with, and compression of, groundmass. (c) Hermance Tonstein x 800. Note (i) control of upper margin of crystal by wood fragment, and its displacement by later rounded 'boule'; (ii) 'Phellomyces' pseudomorph after tracheid structure and control on size of central vermicular crystal; (iii) large mass of wood fragments and hyphae (left centre), and poorly oriented and indecisive form of crystalline material. Kaolinite maeroerystals 347 348 L. R. Moore of the distance between the wood elements. The larger mass of wood fragments and associated fungal hyphae to the left centre of the figure are only partially oriented and this mass may have controlled the indecisive form of the crystalline material thereabout. The size and form of macrocrystals are frequently controlled by large resistant masses of carbonaceous material or wood cells in the adjacent groundmass. Where these objects are less resistant they are often plastically displaced by the developing crystalline area particularly by the rounded 'boule' habit (Fig. 2c) and by vermicular crystals. Macrocrystals may occur in juxtaposition or even interfere one with another, and groups of tabular crystals may have the plastic groundmass packed against them or appearing to have flowed over them often with the formation of later vermicular crystals. It is possible to suggest the relative order of formation of macrocrystals under these conditions. The evidence described above indicates that the kaolinite macrocrystals were formed #1 situ by processes involving macrocrystallization from an aluminium silicate gel; the latter was either formed or contained within the groundmass and intimately associated with the humic products of microbiological decay in the form of a mixed colloid. The development of macrocrystals from a colloidal groundmass is an unusual feature and the processes described differ significantly from those normally associated with the formation of crystals from solutions or melts. Baver (1956) has stated that in most soil colloids there is a mutual interaction of the organic and inorganic colloidal fractions on the physico-chemical properties of the mixture. By polar adsorption the organic colloid particles are closely packed on the surface of the orienting substance and the mineral particles joined together in this process. The platy structure and physico-chemical properties of the kaolin particle leads especially to such alignment. These observations appear to be of particular significance to the present work. POSSIBLE CAUSES OF MACROCRYSTAL FORMATION There is a very close analogy on microbiological, physical, chemical and mineralogical grounds, between Tonsteins and some of the characteristics of certain soil types. In seeking a possible explanation of the presence of macrocrystals of kaolinite and of their wide range of form, and also in considering the processes involved in their formation it is pertinent to bear in mind the evidence of soil science. The occurence of mixed colloids containing an inorganic constituent of kaolinite, and an organic constituent of humic degradation products which carries microbiological organisms is well known. The interrelationship of these two constituents is however of considerable interest; Kaolinite macrocrystals 349 it is known that there is a mutual interrelationship between the two fractions and that this controls the physico-chemical properties of the mixture. Since micro-organisms are an essential part of the organicmatter content, and are intimately concerned in macrocrystal formation their relationship to the original kaolinite particle is of interest. Thus, are the micro-organisms directly concerned, in a vitalistic physicochemical sense, with the actual production of the kaolinite particle as a result of their metabolic processes, or by means of enzymatic degradation products? There does not appear to be an answer to this question. The micro-organisms do, however, produce the necessary environment, in terms of requisite pH control and humic degradation products, for the genesis of the kaolin particle and its association in the mixed colloid, and in this sense the environment is biochemical. Concerning the broader aspects of the interrelationship of the organic and inorganic fractions of the colloid, there is evidence of the physical relationships. Thus Sideri (1936) observed organic molecules to be adsorbed and oriented on the surface of clay particles by reason (Myers, 1937) of the attraction of the slightly ionized polar humic compounds by the electronegative inorganic colloid particles; the resulting polar adsorption leads to close packing of organic colloids on the surface whilst the inorganic particles are joined together beneath. Dehydration of the adsorbed organic matter effects a close union between the inorganic and organic material and the tenacious cementation which follows is responsible for the formation of aggregates. In this manner the organic fraction brings about an orientation of the inorganic matter which could lead to the processes of inorganic linkage and incipient crystallization. The formation of stable aggregates in colloids provides a means of organization of particles; in soils this is due (Baver, 1956) to the presence of cementing agents amongst which organic matter, colloidal clay and dehydrated colloidal oxides of iron and alumina are the most important. Organic colloids (Bayer, I956) cause a high degree of aggregation of the clay particles, produce large aggregates and are most effective in aggregating the finer clay fractions. Many authors have referred to the effects of microbiological activity in aggregate formation. Martin & Waksman (1940) have reported that the growth of micro-organisms leads to aggregation of soil particles, the degree of this being dependent upon the nature of the organism, and amount of its growth, and the nature of the substrate. They also claim that fungi cause both mechanical binding by mycelial growth and aggregation resulting from the synthesis of organic compounds; these conclusions have been substantiated by Martin (1945) and McCaUa (1942). Peele & Beale (1940) innoculated clay loam with various organisms and discovered that aggregation varied with different species 350 L. R. Moore o f organism; fungal species representative of Penicillium and Fusarium were much more effective than bacteria. Geoghegan (1950) believes the metabolic products of micro-organisms to be much more effective in aggregate formation than the cells of the organisms, and McCalla (1942) has noted that some of the metabolic products render the aggregates impermeable to water. It is likely that some effects of aggregation by organic matter are to be seen in the form of macrocrystals in the Tonsteins. Thus, the close association of colonies o f fungal hyphae and bacterial-like cells with the form of some of the irregular crystalline areas and rounded aggregates may reflect the binding effects of the organism (Fig. 2). The pattern of microbiologically degraded cellular structure controls the form of the crystals in cases such as Fig. 2c. It is difficult to demonstrate any effects of metabolic processes. A considerable degree of reorganization due to incipient crystallite formation has taken place but this does not appear to be inevitable (e.g. Fig. lb and Fig. 2a). These controls within the macrocrystalline mass are additional to those exercised by large objects in the groundmass described above. The occurence of tabular or vermicular macrocrystals may follow from the initial form o f the kaolinite colloidal particles. These are hexagonal, compact and plate-like with colloidal properties determined only by external surfaces; the unsatisfied valencies on the edges o f the particle are responsible for ionic reactions, and such particles can be readily aligned. The processes by which alignment is achieved may follow from the polar adsorption of organic matter referred to above but it is also likely that viscosity or plasticity plays a part. Plate-like particles of small dimension constitute the most plastic colloidal materials. Upon the application of pressure the particles are orientated and slide over one another; with the release of pressure the particles are held in the new position by water tension and there is no return to the original position. The orientation pressure might be external and of a geological nature, but the in situ development from a gel-like medium, lack of pre-orientation and juxtaposition of the crystals, renders outside pressure unlikely and certainly not severe. Internal pressure of a localized character and of variable degrees o f intensity from place to place would follow from the strain and stress relationship which occurs during alternative wetting and drying. According to Peterson (1944) this could be expected to produce plate-like aggregates in a soil colloid. Alternate wetting and drying causes aggregation, and cementation follows drying when the colloidal content is high; reversibility of the process may be slow. Such a method provides a means by which regular orientation of particles is effected, and following which crystaUization may commence. There is still the problem of what defines Kaolinite macrocrystals 351 the form and the boundaries of a tabular crystal which has developed from the groundmass and is unhindered by any obstacles within it. Vermicular macrocrystals probably owe their origin to pressure conditions coincident with wetting and a higher state of plasticity which leads to plastic flow and which has created a basic orientation of particles upon which crystallization develops. It is singularly difificult to explain on other grounds the complex arrangements of crystalline masses such as that Fig. 2c. Examples such as Fig. 2b are reminiscent of plastic flow, their form, the orientation o f inclusions and the incipient crystallization directions resemble features associated with glacier ice. The presence o f roots, or burrows would also produce the local pressure conditions resulting in reorganization of particles in a manner likely to produce vermicular or irregular crystalline areas. Plasticity is to a large extent governed by moisture content, but many other factors have considerable effects upon it. Thus (Baver, 1956) it is directly related to particle size, and dependent upon the amount o f colloidal matter, and the nature of the inorganic content; it also varies with the organic content, the plastic limits tending to be higher with the presence of organic matter. The exchangeable cations present in a colloid, and the temporary presence of electrolytes have an effect on plasticity. These factors may not be significant in governing the various effects seen in any one Tonstein but they may be of importance in assessing the differences seen in the kaolin macrocrystals from different Tonsteins. It may be concluded, therefore, that the macrocrystallization of kaolinite has taken place, or was initiated within a still plastic medium, represented by a gel, paste or aggregate. Loss of water either intermittently by wetting and drying, or by a slow process of drying and attendant dehydration appears to have been an important factor in providing the final diagenetic features. Other factors enumerated above would play some part but their actual contribution is difficult or impossible to define. REFERENCES BAVERL.D. (1956) Soil Physics, 3rd edn. Chapman & Hall, London. GEOGHEGANM.J. (1950) Trans. 4th int. Congr. Soil Sci. 1, 198. GRIMR.E. (1953) Clay Mineralogy. McGraw-Hill, New York. HOEHNEK. (1951) Decheniana 105-106, 33. HOEHNEK. (1954) Chem, d. s 17, 6. JOFrE J.S. (1949) Pedology, 2nd edn. Pedology Publications, New Brunswick. KELLERW.D. (1956) Bull. Amer. Ass. Petrol. GeoL 40, 2689. MARTINJ.P. (1945) Soll Sci. 59, 163. MARTINJ.P. & WAKSMANS.A. (1940) Soil Sci. 50, 29. MASONB. (1960) Principles o f Geochemistry, 2nd edn. Wiley, London. MCCALLAT.M. (1942) Proc. SoilSci. Soc. Amer. 7, 209. 352 L. R. Moore VAN DER MERWE C.R. (1949) Tech. Commun. Bur. SoilSci. Harpenden46, 8 and 128. MOHR E.C.J. & VAN BARENF.A. (1954) Tropical Soils. Interscience, New York. MOORE L.R. (1963) Proc. Yorks. geol. Soc. (In press). MYERS H.E. (1937)SoilSci. 44, 331. 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