Abstract (English):
An extensive review describes the unique properties of apatite, which, due to the peculiarities of its structure, allows for diverse isomorphic substitutions both in its cationic part (Mn, Sr, Ba, REE, U, etc.) and in the anionic part (CO 2, SO3, SiO 2, OH, F, Cl, etc.). Since these substitutions occur under well-defined conditions in both endogenous thermal and exogenous low-temperature processes, the composition of apatite turns out to be an indicator of these processes. At the same time, the conditions of formation of most igneous and metamorphic rocks can be judged by the composition of accessory apatite, and the genesis of phosphorus ores, both endogenous (Khibiny, Kiruna type, etc.) and exogenous (phosphorites), is judged by the composition of ore-forming apatite. The review is based on the recent "Irish" review 2020, covering 147 literary sources and compiled by 4 co-authors from Dublin and one from Stockholm [130]. Since the compilers of the "Irish" review practically did not use literature in Russian, it became necessary to seriously supplement it with the data given in the domestic literature, as well with a number of foreign works that are not covered by the "Irish" review. The resulting text should make it much easier for the geologist reader to use apatite in practice as a remarkable mineral-an indicator of various geological processes

Keywords:
apatite, carbonate-apatite (francolite), halogens, sulfate, trace elements, REE, manganese, strontium, neodymium, uranium

1.1. Hydroxyl Crystallization of Ca phosphate from very weakly supersaturated solutions occurs by the so-called "classical" mechanism, when ionic monomers are slowly deposited on the active growth surface. If the solution is supersaturated, then the "classical" growth mechanism gives way to the "non-classical" one, when whole ion clusters quickly settle on the active surface. In particular, the height of the steps on the surface of active growth (0.8 nm) exceeds the width of the molecular unit of 0.24 nm for the phosphate ion PO43–, and the kinetic coefficient of attachment of the growth unit to the steps (i.e., the kinetic coefficient of the step) under physiological conditions (pH 7.4) is 100 times less than for similar ionic minerals. This can be seen as the reason that in natural conditions biogenic hydroxyapatite Ca10(PO4)6(OH)2 is not formed immediately, but is preceded by biophosphate-1 – or octacalcium phosphate Ca8(HPO4)2(PO4)4.5H2O, or brushite CaHPO4.2H2O, and with particularly strong supersaturation – amorphous Ca-phosphate CaxHy(PO4)znHO (n = 3–4.5). Hydroxyapatite turns out to be biophosphate-2, it is formed only by the substrate of biophosphate-1, most often – octacalcium phosphate. Studying urolites, Syktyvkar mineralogist Valentina Katkova proved that phosphate spherulites and spherocrystals of monomineral composition in urolites are pseudomorphoses of carbonate hydroxyapatite by octacalcium phosphate. In agreement with foreign predecessors [88; 133], she admits that the transformation process was the result of hydrolysis with loss of three water molecules by octocalcium phosphate at elevated pH: 5Са8Н2(РО4)6 5Н2О  4 Са10Н2(РО4)6 (ОН)2 + 6 Н3РО4 At the same time, it is noted [29, p. 12]: "in phosphate urolites, as a rule, the main mineral components are struvite, carbonate-containing hydroxylapatite and newberyite." It has recently been shown that based on the study of the morphology of crystals of the so-called nanohydroxyapatite (NGAP), it is possible to judge which polysaccharides were present in the environment at the origin of NGAP crystals. The fact is that natural polysaccharides play an important role in the formation of NGAP crystals in biological systems. Chinese researchers [101] synthesized NGAP crystals in the presence of four polysaccharides: pectin, carrageenan, chitosan and amylose, designated as PeHa, CaHa, CsHa and AmHa, respectively. The shape of the obtained crystals is needle-shaped/rod-shaped in all cases, and their size increases in the order of PeHa  CaHa  CsHa  AmHa. The presence of polysaccharides induces heterogeneous nucleation of NGAP and further modulates crystal growth. However, a high concentration of polysaccharides and a short reaction time are unfavorable for the growth of NGAP crystals, especially for polysaccharides with carboxyl groups. As a result, the results obtained can give an idea of the effect of polysaccharides with various chemical functional groups (–COOH, –OSO3H, –NH2, –OH) on the formation of NGAP crystals. One of the natural ways of bioapatite formation (which allows for the "repair" of damaged bones) is to obtain it by metasomatic phosphatization of porous calcium carbonate structurally compatible with phosphate. It has long been known that hydroxyapatite can be obtained by treating corals with a phosphate solution, and recently a successful experiment was conducted on phosphatization of the lamellar region of the cuttlefish bone (Sepia officinalis). The main thing in this experiment is to first obtain an intermediate compound - amorphous carbonate. As a result, an amorphous calcium hydrophosphate dihydrate, CaHPO4 2H2O, was obtained in a short time (up to several hours) [96]. Not so long ago, it was experimentally shown that in urolithiasis (nephrolithiasis), the formation of calcium oxalate monohydrate of whewellite CaC2O4 H2O is closely related to the earlier formation of hydroxyapatite. Model experiments were carried out that showed the full reality of the substitution of carbonate hydroxyapatite with wevellite [125]. The fact is that the so-called Randall plaques, known to urologists for a long time, forming lighter organo-mineral spots directly in the renal tissue, in their mineral part consist just of carbonate hydroxyapatite Ca5(PO4)3OH. Under the influence of a pathogenic decrease in the pH of urine up to pH = 4.5, Randall plaques partially dissolve, releasing Ca2+ into the liquid phase, and thereby induce the deposition of whewellite on them. Indeed, doctors have long known that many oxalate stones "sit" directly on Randall's plaques. Sometimes nitrogen admixture is found in samples of obviously biogenic hydroxyapatite according to EPR spectra, which, generally speaking, should not be here. As N. O. Dudchenko experimentally showed [22], nitrogen-containing radicals (NO42-) are formed in samples during heat treatment of biogenic hydroxyapatite under conditions of lack of oxygen. During the heat treatment of the mineral in conditions of excess oxygen, such radicals are not formed. At the same time, the maximum intensity of the EPR spectrum of nitrogen-containing radicals or their maximum amount is observed during annealing in the temperature range of 800-850 ° C. The Ukrainian author came to the conclusion that this nitrogen-containing center is included in the structure of biogenic hydroxyapatite due to the isomorphic substitution of phosphorus with nitrogen (P←N). Thus, the admixture of nitrogen in natural biogenic apatite indicates that it has undergone thermal effects. Moreover, natural heating of obviously biogenic apatites can form such rare minerals as berlinite Al[PO4] and hydroxyl-ellestadite Ca5[(Si, P, S)O4]3(OH, F, Cl), found in the Romanian Cyclovina cave. Since they were formed from cave guano, and it is impossible to imagine any external heating of guano, the authors of this amazing find suggested that high temperatures somehow arose in the guano itself [116]. Some materials on the topic were given in our 2011 book [80, p. 284]. The references made there to the literature are replaced here with angle brackets – <...>. In particular, it was reported that phosphate nodules in the Kuonam formation of the Cambrian on the Molodo River differ greatly in composition from the host (practically carbonless) black siliceous-clay mudstones. According to Siberian geologists, this indicates the biochemical (bacterial) nature of phosphate <...>. The source of phosphorus in phosphorites among cyanobacterial mats on Polynesian atolls is clearly biogenic <...>. Among the fused cluster-like clusters of juvenile pelicypods in Naragansett Bay (Merceparia merceparia) and Boca Kiega Bay in Florida (Agropecten irradians), microconcretions, up to 250 microns in size, of amorphous Ca-phosphate (sometimes with an admixture of Al-phosphates) with a concentric-zonal structure are described. Most likely, these formations are biogenic – coprolites <...>. 1.2. Halogens As it was shown during the study of the Magnitogorsk ore-magmatic complex of the Southern Urals, the ratio of halogens in apatite is an excellent indicator of the fluid regime in petro- and ore genesis [10]. The fact is that there are two trends of magmatic differentiation: (1) tholeiitic – the evolution of the melt towards the accumulation of iron and the formation of ferruginous gabbroids, with which the titanium-magnetite ores of the Kuibass massif are associated, and (2) calcareous-alkaline – the evolution of the melt towards an increase in its silicicity and alkalinity, which reflects the change in the ferruginous magmatites of the subvolcanic and hypabyssal facies of the gabbro-granite Magnitogorsk intrusion, which is associated with skarn-magnetite mineralization. According to experimental data, the occurrence of tholeiitic and calcareous-alkaline trends in the differentiation of melts is due to the liquation orthopyroxene barrier, the overcoming of which depends on the degree of saturation of the melt with water. These trends are well documented by the content of chlorine and fluorine in apatites. As can be seen on the "chlorine - fluorine" graph compiled by the authors [10, Fig. 2, p. 31], clear fields are distinguished here by the magnitude of the Cl/F ratio: a) in rocks of gabbro-granite intrusion Cl/F = 0.0-0.35; (b) in oreless gabbro Cl/F = 0.35-0.90; (c) in ore-bearing (titanium-magnetite) gabbro Cl/F = 0.90-3.40. As it moves upward from "dry" reduced magmas to more aqueous and oxidized ones, the fluid becomes more chlorinated. Thus, the quantitative content of chlorine and fluorine in apatites of rocks and ores is a qualitative characteristic of the fluid regime during their formation. Researchers of three North Chilean iron-phosphorus deposits (Kiruna type) of Cretaceous age in the Andes also indicate that the ratio of halogens in apatites is an important indicator of the fluid regime during their formation [118]. Despite the inconsistency of the proposed models, the authors are inclined to a new flotation model in which microliths of magmatic magnetite crystallize from a silicate melt, and then rise, carried away by bubbles of liquids dissolved in magma. As these suspensions of magmatic magnetite rise, they merge, and the magnetite content increases due to the deposition of hydrothermal magnetite in the form of rims on the primary magnetite and filling the intermediate space up to the level of neutral buoyancy, which reflects a continuous process – from magmatic to hydrothermal. In 8 stratified trap intrusions of the Siberian Platform, the geochemistry of chlorine and fluorine in accessory apatites, as well as in rock-forming micas and amphiboles was studied according to over 1000 analyses [54]. In the overwhelming mass of apatites F > Cl. The maximum halogen contents have chlorapatite (Cl = 6.97 wt.%) and fluorapatite (F = 6.04 wt.%). The total ferruginous content (f = Fe/(Fe + Mg), at.%) of femic minerals varies: in micas from 2 to 98 at.%, in amphiboles from 22 to 95 at.%. The graphs of the dependence of Cl - f and F - f in minerals show an increase in the content of Cl with an increase in f, and an increase in F with a decrease in f. Thus, chlorine exhibits pronounced ferrophilicity, and fluorine exhibits magnesiophilicity. In rock-forming minerals, the richest halogens are: fluorophlogopite (F = 7.06 wt.%, f = 7 at.%), chlorannite (Cl = 6.30 wt.%, f = 89 at.%), chlorferrigastingsite (Cl = 5.22 wt.%, f = 90 at.%). It is assumed that the crystallization of halogen-containing minerals occurred under conditions of increased fluid pressure of halocarbon fluids at the levels of MW-, IW- and QIF buffers. An indicator of the reducing conditions of the magmatic process are the finds in the rocks of graphite and native metals/ Of particular interest is the thorough study of phosphate minerals from the Ural, Ozernoye and Chelyabinsk chondrites carried out in 2014, samples of which are on display at the Ural Geological Museum at the Ural State Mining University (Yekaterinburg) [24]. In all cases, chlorapatite and merrillite were found in the chondrites. Merrilite Ca9Na(Fe, Mg)[PO4]7 is an anhydrous terminal element of a series of 14 solid solutions, and the hydrolyzed terminal element is whitlockite Ca9 (Fe, Mg) [HPO4][PO4]6. However, contrary to earlier (less thorough) studies, vitlokit was not found in the studied chondrite samples, The study of other meteorites has shown that merrillite is the predominant primary Ca-phosphate mineral in Martian meteorites and, consequently, on Mars. The mineral is the main phase in the study of differences in geological processes between Earth and Mars. It is assumed [82] that merrilite even has astrobiological significance – it could serve as a source of phosphorus for life on Mars! As for the Ural meteorites, the content of Cl in 4 grains of chlorapatite from the Ural chondrite was 4.28-4.70%, in the grain of apatite "Lake" Cl = 4.09%, and in 4 grains of chlorapatite from the Chelyabinsk chondrite Cl = 3.04–4.07%. At the same time, two varieties of chlorapatite have been identified in the Chelyabinsk chondrite – extremely chlorinated and with a high content of the hydroxyl group. Unfortunately, as our geologists note [24], the study of samples of the Ozernoye meteorite turned out to be associated with a very unsightly history. This meteorite was found in 1983 by a shepherd N. L. Hismatullin 4 km north of the Ozerny site of the Trans-Ural state farm of the Almenevsky district of the Kurgan region (about 100 km southwest of Kurgan). In 1985, the same person discovered a second piece of identical chondrite near the village of Ozernoye in the same area, so that the total mass of both fragments was about 3.66 kg. Both of them were transferred to the Ural Meteorite Commission for study, and in 2014 a small fragment from the first piece was already stored in the Ural Geological Museum (its authors studied it). However, simultaneously with the second piece of Ozernoye chondrite, a larger fragment of a meteorite weighing 22.4 kg was discovered (in the same place – near the village of Ozernoye), but it was deliberately not handed over to specialists for study. And in 2007, this fragment was already in Kurgan and was soon sold by the owner to the famous meteorite collector S. P. Vasiliev (living in Prague) – and with the permission of the Ministry of Culture of the Russian Federation (!) was taken to the Czech Republic… Our patriotic geologists [24] indignantly remind the reader of the complete illegality of this commerce, because according to Russian laws, "extraterrestrial bodies that have fallen on the territory of the Russian Federation are the cultural heritage and property of Russia." So, within the framework of our topic, chlorapatite, and especially merrilite, may turn out to be indicators of the extraterrestrial (meteoritic) genesis of the rock containing them. 1.3. Sulfate and silica Since one of the components included in the anionic part of apatite may be sulfate, some apatites contain sulfur. Interest in the entry of sulfur into apatite has increased markedly after the recent eruptions of volcanoes El Chicon (in Mexico) and Pinatubo (in the Philippines), whose lavas contained anhydrite, and large masses of sulfur were released into the atmosphere. Previously, anhydrite was not noted in effusions, since it was quickly dissolved by meteoric waters or disappeared even earlier - during post-magmatic hydrothermal processes. Therefore, a more stable early apatite is much more suitable for studying the magmatic geochemistry of sulfur. In 2004, Hannoverian geochemists [119] made special experiments at 200 MPa and 800–1.100 oC with glass imitating the composition of rhyolite (SiO2 = 77.34, Na2O = 4.24, K2O = 4.85%), but without apatite components. 4 weight % apatite was added to the melt of this glass. (CaO = 55.80, P2O5 = 42.10, Cl = 0.04, F = 3.22 %). Subsequent addition of up to 0.5% S to the system under oxidizing conditions increased the solubility of apatite in the melt, since part of the Ca was bound to sulfur. If in the experiment the sulfur content in the melt was reduced, then with a decrease in temperature, the sulfur content in apatite also decreased. The molar coefficient of sulfur distribution between apatite and the melt Kds increased from 4.5 to 14.2 with a decrease in temperature under conditions of anhydrite undersaturation. However, in the supersaturated anhydrite melt, at 800 oC, the Kds was lower – about 8. Thus, the Kds value depends not only on the temperature, but also on the sulfur content in the melt. As a result, these first experiments showed that, according to the sulfur content in apatite, it is possible to judge the evolution of sulfur contents in magmatic systems under oxidizing conditions. In 2011, Italian volcanologists studied 14 samples from the lavas of two historical eruptions of Vesuvius – 1631 and 1872. It was possible to identify 5 varieties of apatite, each of which not only differs in association with other minerals, but also has clear differences in color, structure and composition [123]. For example, apatites of type-1 (yellow) and type-4 (green) are associated with large-crystalline clinopyroxene and phlogopite, and apatites of type 2 (transparent and colorless) – with microcrystalline minerals of the cancrinite group, feldspar and opaque ore. On Si–S–P/100 triangles, these types form almost non-overlapping fields. For example, the poorest in silicon and the most sulfurous are apatites of type 3 (transparent and colorless), and the most siliceous are apatites of type 5 (aquamarine color). So, quite noticeable admixtures of silicon and sulfur, replacing phosphorus, allow us to distinguish well between different types of apatites from volcanic eruptions. In 2013, Yekaterinburg geologists [1] described the Middle Devonian epidote-containing porphyries of trachyandesite-trachydacite composition forming a dike field in the zone of the active continental margin of the Middle Ural segment of the Ural folded belt. A remarkable feature of these rocks is the presence of sulfur-containing apatite and igneous anhydrite. Apatite has an oscillatory type of zoning for sulfur and progressive for fluorine. The SO3 content varies from 0.5 to 1.5 wt. % in cores and from 0.05 to 0.2 wt. % in the borders of apatite phenocrysts. It is believed that the crystallization of sulfur-rich apatite occurred at 850–800 °C and 10–8 kbar. Poor in S apatite in paragenesis with anhydrite was formed at 725–700° and 7.5–6 kbar. The initial magma was very rich in water, sulfate-saturated and oxidized with oxygen fugacity = 0.5–1.5 log units above the NNO buffer. The source of sulfur could be both sulfide-enriched rocks of the lower crust and emanations of mantle fluids separating from mafic magmas. In the work of Ural geologists [73] it was noted that the rocks of the Late Paleozoic Khudolazov complex, specialized for Cu-Ni mineralization, are characterized by apatites with the highest contents of sulphate sulfur (up to 0.65 wt.%), isomorphic with phosphorus in the composition of the anionic complex (PO4)3–. These apatites have a reduced fluorine content (< 2 wt.%) with a noticeable chlorine content (up to 1.50 wt.%). Such a character of the ratio of halogens and sulfur in apatites can be recommended as one of the most effective indicator signs of specialization of Late Paleozoic accretion-collisional gabbrodolerites of the Western Magnitogorsk zone of the Southern Urals for Cu-Ni mineralization. An additional criterion for such specialization is the presence of sulfide minerals rich in Cu, Ni and Co in rocks. According to the review of Novosibirsk chemists [75], the substitution of the phosphate group with the SiO44– silicate group gives the surface of hydroxyapatite (HAP) new properties, therefore, such Si-HAP is widely used in medicine for coating implants, synthesis of biocompatible ceramics, production of medicines and cosmetics, etc. [75, p. 478]: "The high surface activity of Si-HAP <...> is associated with the formation of silanol groups -SiOH <...> on the surface of the material. Due to differences in the sizes of terahedral anions (distances Si–O = 0.166 nm, P–O = 0.155 nm), the substitution of phosphate ion for silicate is accompanied by microstresses in the structure of apatite. As a result, silicate ions are segregated on the surface of the particle". During the mechanochemical synthesis of Si-HAP in a planetary mill, where monetite СаНРО4, CaO and amorphous silica gel of the composition SiO2 nH2O (n = 0.59–0.71) were mixed, followed by annealing at 1000 oC in a chamber electric furnace, a product with the formula was obtained: Ca10(PO4)6–x (SiO4)x OH2–x where x was set equal to 0.1, 0.2, 0.4 and 0.8. For example, GAP-08 was obtained mechanochemically according to the equation: 5.2 СаНРО4 + 4.8 СаО + 0.8 SiO2 0.71 H2O = Ca10 (PO4)5.2(SiO4)0.8 (OH)1.2 + 2.568 H2O 1.4. Carbonate Carbonate radicals CO32– can form already in bioapatite (hydroxyapatite), where they can replace both OH– and PO43– in the lattice. Carbonate reduces the crystallinity of apatite and makes it more amorphous and brittle. Carbonate apatites are particularly characteristic of bone tissue. In tooth tissues, they are formed in the immediate vicinity of the enamel-dentine border due to the production of anions by HCO–3 pulp cells (odontoblasts). The formation of HCO–3 is possible as a result of the metabolism of the aerobic microflora of plaque. The accumulation of carbonatapatite over 3-4% of the total mass of hydroxyapatite contributes to the development of caries. With age, the amount of carbonatapatites in the teeth increases. During the formation of most phosphorites, carbonate-apatite (francolite) is formed in diagenesis, as the sediment is buried and removed from the "bottom water/sediment" boundary. In this process, as shown by V. S. Savenko and his daughter A.V. Savenko [56], there is an increase in the carbonate alkalinity of pore waters, as a result of which the initially formed precipitate of calcium phosphate begins to dissolve and return the phosphate group PO43– to the pore waters (and then to the bottom water – "phosphorus respiration of the sediment"), which is replaced by the carbonate group CO32– . .In turn, if phosphorites formed in diagenesis sink into the catagenesis zone, then as our most prominent experts Yu. N. Zanin [25] and V. Z. Bliskovsky [9] have shown, a strong decrease in carbonate content occurs in the composition of francolites, with a corresponding removal of strontium. So, in the aspect of our topic (apatite as an indicator), the content of the CO32–group in apatite can serve as an indicator: (a) the mineral belongs to bioapatites; (b) mineral formation in diagenesis; (c) mineral changes in catagenesis. In addition to the well-known phosphorite deposits, where the phosphate mineral is represented by diagenetic francolite, it is necessary to emphasize the enormous resources of francolite in the weathering crust of carbonatites of the unique Russian Tomtor deposit – with complex niobium-rare earth-scandium ores. The deposit is located in the north of Yakutia and is associated with one of the world's largest carbonatite complexes (Ş=300 km2) with the most significant carbonatite manifestation (12 km2). The massif has a rounded shape in plan and a concentric zonal structure – carbonatites form its central core, and alkaline and nepheline syenites, occupying most of the area of the massif, make up the marginal zone; carbonated iyolites, significantly inferior in area to syenites, are present in the form of a crescent-shaped body separating the syenite marginal zone from the carbonatite core of the massif. Within the Tomtor massif, an indigenous iron ore deposit with resources of more than 1 billion tons has been preliminarily estimated. Francolite ores with P2O5 resources of about 500 million tons have been identified in the weathering crusts of carbonatites with average phosphorus pentoxide contents of about 17%. However, the main wealth of Tomtor is its unique complex rare-metal ores, which contain more than two and a half dozen components in the ore complex and which significantly exceed in their parameters the ores of the richest developed foreign rare-metal deposits of the weathering crust of Arasha and Mount Weld carbonatites.

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