In recent decades, the problem of precious-metal (gold,PGE) potential of carbonaceous terrigenous-sedimentary units(black shales) has been hotly discussed by geologists. Theserocks seem to be the most probable unconventional naturalsources of gold and PGE in the future. Data on the contentsof precious metals in them are contradictory, and the metalspecies and mineralization nature have been poorly studied,which significantly hampers estimation of the ore potential ofcarbonaceous shales and development of their processingtechnology.
In this paper, the term carbonaceous shales is used inreference to terrigenous-sedimentary rocks formed in differentsedimentary environments (shallow-water seas of platforms,passive continental margins, deep-water trenches and seas ofactive continental margins, transform boundaries of continen-
tal and oceanic plates, etc.) and enriched in solid carbonaceoussubstance imparting them a black color. These rocks, as a rule,underwent regional metamorphism of greenschist and epidote–amphibolite (up to lower amphibolite) facies, which explainsthe presence of different forms of carbon in them—fromstructureless finely dispersed material to graphite.
Carbonaceous terrigenous complexes with high contents ofPGE, Au, and Ag are known in different parts of the world.Exploration of some deposits revealed precious metals asby-products. These are U deposits in North Australia, Ni–Modeposits in South China, Cu deposits in Poland, Au depositsin Russia, Kazakhstan, Uzbekistan, and Brazil, Fe deposits inRussia and Brazil, etc. (Buryak et al., 1988; Chernyshev, 1999;Manikyamba et al., 2008; Mirzekhanov and Mirzekhanova,1991; Obolensky et al., 2011; Parada, 2004; Pieczonka et al.,2008; Razvozzhaeva et al., 2008; Sener et al., 2002; Sharapovet al., 2012; Vinokurov and Omel’yanenko, 1990). Neverthe-less, the nature of precious-metal mineralization in carbona-ceous strata is still unclear. Though deposits and occurrencesof precious metals are often localized in such strata, not allof the latter have commercial or even elevated contents of
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3,
these elements. Most of the known mineralization in blackshales is related to the formation of quartz-sulfide veins. Forexample, in the large Natalka deposit, northeastern Russia, Ptand Pd occur in sulfides (Plyusnina et al., 2003). The SukhoiLog and Olimpiada deposits in Russia, Muruntau deposit inUzbekistan, and Kumtor deposit in Kirghizia, localized infoliated carbon-rich siltstones and mudstones, are of the samegold–sulfide type. However, high contents of precious metalsare often found in carbonaceous shales without quartz-sulfidemineralization (Gurskaya, 2000). This suggests the presenceof precious-metal mineralization of special type (Khanchuk etal., 2009a).
Elevated contents of precious metals in terrigenous rocksare the result of the following geologic processes: sedimenta-tion, diagenesis, metamorphism and metasomatic alterationsof rocks with formation of orebodies. All these geologicprocesses are indicated by certain mineralogical, geochemical,and petrochemical properties of the ores and host rocks(Mitrofanov et al., 2005). Thus, the host rock strata and oredeposits and occurrences with the same metallogenic speciali-zation must show similar characteristics. Studies of suchcharacteristics pointing to the possible precious-metal potentialof carbonaceous complexes seems highly promising. They willpromote a more effective detection of precious-metal miner-alization during geological mapping and prospecting.
We attempted to determine such characteristics by studyingsome world deposits and the carbonaceous rocks of the Sutyr’and Kimkan strata in the eastern Bureya massif, where highAu and PGE contents were found (Khanchuk et al., 2009b).We calculated petrochemical modules, performed a faciesidentification of the studied rock units, established the generalage characteristics of the enclosing Earth’s crust, reconstructedgeodynamic settings during the formation of the rocks,revealed a difference between the rock provenances, anddetermined the geochemical precious-metal specialization ofthe strata.
The tectonic position and brief geologic andpetrological characteristics
According to modern concepts of the tectonic structure ofsouthern Far East Russia, the Bureya massif (terrane), togetherwith the Jiamusi massif, is part of the Early Paleozoic orogenicbelt (Khanchuk, 2000, 2006; Parfenov et al., 2003) (Fig. 1).The massif is composed mainly of metamorphic rocks ofgreenschist-amphibolite facies. The weakly altered rocks havepreserved the Early Cambrian fauna. The highly metamor-phosed rocks of the massif were earlier considered Archeanand Lower Proterozoic (Turbin et al., 1994). But detailedisotope studies showed that the age of their protolith is within1.2–0.5 Ga and the time of amphibolite-facies metamorphismis ~490 Ma (Kotov et al., 2009; Sorokin et al., 2010, 2011).Thus, the crystalline rocks of the Bureya massif are not abasement for the less metamorphosed deposits. Together withthe latter, these rocks make a single fragment of continentallithosphere formed in the Early Ordovician.
The Bureya massif is formed by turbidite rocks, cherts,jaspers, phtanites, ferromanganese rocks, and limestones. Thepredominant deposits of sedimentary paleo-oceanic genesisoccur among terrigenous sand–shale complexes at differentstratigraphic levels, forming isolated bodies a few meters to afew kilometers in size (Krasnyi, 1966). A similar rockassociation is typical of the well-studied Mesozoic andCenozoic accretionary prisms in subduction zones of theSikhote-Alin area, Japan, and other regions (Khanchuk, 2006).Thus, the available geological and geochronological dataindicate that the Bureya massif is mainly an accretionary prismmetamorphosed in the Early–Middle Ordovician.
The Sutyr’ and Kimkan rock units are weakly metamor-phosed deposits of the Bureya massif.
The Sutyr’ rock unit (Early Proterozoic) composes a long(75 km) narrow (<5 km) tectonic block in the Khingan Faultzone, where the valley of the Sutyr’ River is located. The unitis formed mainly by micaceous shales, often with carbona-ceous material, and subordinate highly carbonaceous phyllitesand metasiltstones, marbles, quartzites, and sheet-like andlenticular bodies of graphite-bearing1 shales 4 to 150 m thick
Fig. 1. Terranes and orogenic belts in East Asia. 1, cratons: a, North Asian;b, Sino-Korean; 2, terranes: AR, Argun; BJ, Bureya–Jiamusi; SR, Sergeevka;YT, Yenisei–Transbaikalian; KhN, Khanka; WD, Wundurmiao (fragments ofEarly Paleozoic orogenic belts); VZ, Voznesensk (fragment of the passivemargin of craton); 3, orogenic belts: SL, Solonker (Permian); SM, South Mon-golian (Late Paleozoic); MO, Mongol-Okhotsk (Early Cretaceous); HS, Honsu–Sikhote-Alin (Middle Cretaceous); SH, Sakhalin–Hokkaido (Eocene); 4, areasof study: Sut, Sutyr’; Kim, Kimkan.
1The term graphite and its derivates are used conventially, because data onthe analytical identification of graphite in the studied rocks are insufficient.It is not ruled out that much of their carbonaceous substance is lower-temperature modifications of graphite. Therefore, we use predominantly theterm carbonaceous.
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and up to 900 m long with 10–80% carbonaceous material.At some sites, the rocks were subjected to the contactmetamorphism of Paleozoic intrusions and thus are of gneis-soid habit, often containing garnet, sillimanite, and andalusite.The total thickness of the unit is estimated at 1500 m. In theSutyr’ basin, there is the gold-promising Sutyr’ occurrence,where the rocks are sulfidized to different degrees and locallycontain a network of thin quartz veinlets and 1–20 cm (up to50 cm in rare cases) thick veins. Semiquantitative spectro-graphic analysis for gold showed its average content of0.01 ppm in the common carbonaceous rocks and up to0.1 ppm in the samples with quartz veinlets.
The Kimkan rock unit (Lower Cambrian) composes alarge block in the granite roof relics. The rocks metamor-phosed to the greenschist and epidote–amphibolite faciescompose the upper section of the Vendian–Lower CambrianKhingan Group. They rest upon the deposits of the LondokoFormation including marbleized limestones, carbonaceous-clayey and siliceous-clayey shales, sandstones, and siltstones.The Kimkan unit is dominated by foliated sandstones, silt-stones, and carbonaceous clayey shales, locally transformed
into graphitic phyllites. Mica–quartz schists, marbles, andquartzites include members of highly carbonaceous (Corg ≤25.7%) shales up to 100 m thick and up to 2500 m long. Nearthe Ordovician granite intrusions, the foliated rocks weresubjected to contact metamorphism to form hornfelses of theamphibole– and muscovite–hornfelse facies.
The Kimkan rock unit bears Fe- and Fe–Mn-ore depositsas well as occurrences of graphite, Be, REE, U, magnesiumore, and placer gold. There are also sites where carbonaceousbeds are enriched in Pt (up to 10 ppm) and Pd (up to 0.6 ppm)(Gurskaya, 2000).
Geochemistry
The studied shales are conventially divided into two groupsaccording to carbon content (Table 1): highly carbonaceousand phyllite-like in the Sutyr’ unit and highly carbonaceousand carbonaceous in the Kimkan unit.
The chemical compositions of typical carbonaceous shalesof both units are presented in Tables 2 and 3.
Table 1. Average content of Corg in shales of the Sutyr’ and Kimkan rock units
Rock unit Shales Number of samples Corg, %
Sutyr’ Highly carbonaceous 13 4.42
Phyllite-like 3 1.27
Kimkan Highly carbonaceous 3 1.71
Carbonaceous 9 0.54
Note. Analyses were carried out at the Far East Geological Institute, Vladivostok (analysts M.G. Blokhin and M.N. Bezrodnova).
Table 2. Chemical composition of carbonaceous shales of the Sutyr’ and Kimkan rock units (wt.%)
Rock unit Shales Sample no. SiO2 TiO2 Al2O3 Fe2O3 tot MnO MgO CaO Na2O K2O P2O5 Total
Note. Total contents are given with ignorance of LOI and trace elements. Analyses were carried out by XRF: samples 552, 562-t, 608, 610, 613, 631–637, andKI-9—Institute of Tectonics and Geophysics, Khabarovsk (analyst L.M. Il’in); samples 572 and 574—Northeastern Complex Research Institute, Magadan(analyst V.I. Manuilova); and samples 511–515—National Geophysical Research Institute, Hyderabad, India (analyst V. Balaram).
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Facies typification
On the ASC diagram (Gorbachev and Sozinov, 1985)(Fig. 2), the shales of the Sutyr’ rock unit fall into the fieldsof terrigenous-carbonaceous and siliceous-carbonaceous for-mation, and the shales of the Kimkan rock unit, into the fieldof terrigenous-carbonaceous formation. The compositions ofhighly carbonaceous shales from both units are shifted towardthe fields of siliceous formations, and those of carbonaceousshales, toward the fields of carbonate formations. No signifi-cant correlations between parameters A, S, and C at the 0.95confidence level have been revealed for the units, whichobviously confirms the nonclastogene (biogenic) nature ofmost SiO2 in the shales. Analysis of the relations between theoxides of rock-forming elements showed their negative orminor positive correlation with SiO2.
We have established a significant positive correlationbetween Al2O3 and K2O. Highly carbonaceous shales of theSutyr’ rock unit contain mainly <3 wt.% K2O and <15 wt.%Al2O3, and phyllite-like shales are more potassic and alumi-nous (Fig. 3). Highly carbonaceous shales of the Kimkan rockunit contain mainly >4 wt.% K2O and >13 wt.% Al2O3,whereas carbonaceous shales have <4 wt.% K2O and the sameAl2O3 contents.
According to Condie (1993), the Cr and Ni contents in theupper horizons of continental crust regularly decrease fromancient to younger rocks. On the diagram (Fig. 4), thefigurative points of rocks of the studied units are localized atthe intersection of the fields of Neoarchean and post-Archeanrocks, which agrees with geological data. The carbonaceousshales of both rock units lie in the close vicinity of thecomposition point of Proterozoic shales (Condie, 1993),whereas the more carbon-saturated varieties are richer in Crand poorer in Ni, significantly shifting toward the average-composition trend.
Table 3. Trace-element composition of carbonaceous shales of the Sutyr’ and Kimkan rock units (ppm)
Note. Analyses were carried out by ICP MS in the Group of Geochemical Studies (head V. Balaram, National Geophysical Research Institute, Hyderabad,India). Samples were prepared by fusion of shales with NiS.
Fig. 2. ASC petrochemical diagram (Gorbachev and Sozinov, 1985). Composi-tion fields of sedimentary formations: I, carbonate-carbonaceous; II, terri-genous-carbonaceous; III, siliceous-carbonaceous (volcanogenic-siliceous-car-bonaceous). Hereafter: 1, highly carbonaceous and 2, phyllite-like shales of theSutyr’ rock unit; 3, highly carbonaceous and 4, carbonaceous shales of theKimkan rock unit. A = Al2O3/(CaO +K2O + Na2O), S = SiO2/(Al2O3 + Fe2O3 +CaO + MgO), C = CaO + MgO.
Fig. 3. K2O–Al2O3 diagram for carbonaceous rocks of the Sutyr’ and Kimkanrock units.
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Geodynamic settings of formation
Analysis of Th, La, Sc, and Zr contents (Bhatia and Crook,1986) showed that both rock units were sourced from volcanicarcs (Fig. 5). Their figurative points are localized in the fieldsof island-arc complexes formed on continental basement.
In accordance with the lg(K2O/Na2O)–SiO2 discriminationdiagram proposed by Roser and Korsch (1986), the depositsof the Sutyr’ and Kimkan rock units formed under theinfluence of active continental margin (Fig. 6).
Taking into account that such geochemical diagrams arenot highly reliable (the degree of reliability for Miocene–Qua-ternary deposits in particular geodynamic settings (Armstrong-Altrin and Verma, 2005) is no higher than 62%), zones ofsubduction-related volcanism that takes place on the continen-tal basement seem to have formed the provenances of theSutyr’ and Kimkan units. These zones include both continentalarcs and active continental margins, which are suggested asthe sedimentary environments of the rocks studied in Figs. 5and 6.
Figure 7 presents a discrimination diagram proposed byMurray (1994) in the review of siliceous deposits. It includes
Fig. 4. Condie (1993) diagram for the average contents of Cr and Ni in shales ofthe Sutyr’ and Kimkan rock units. 1, 2, upper horizons of Archean (1) andpost-Archean (2) continental crust, after Rudnick and Gao (2004) and Taylorand McLennan (1985); 3, 4 – average compositions of Archean (3) and Protero-zoic (4) shales, after Condie (1993).
Fig. 5. La–Th–Sc (a) and Th–Sc–Zr/10 (b) discrimination diagrams, after Bhatia and Crook (1986). A, oceanic and B, continental island arcs; C, active and D, passivecontinental margins.
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data on the Sutyr’ and Kimkan rock units as well as theevolutionary trend of Cretaceous–Cenozoic sediments fromDSDP borehole 1149 drilled on the oceanic slope of theIzu–Bonin trench (Plank et al., 2007). Among them, rock unitsIII and IV are Valanginian–Albian cherts, siliceous clays, andchalk; rock unit II is upper Cretaceous red pelagic clays; androck unit I is volcanic ashes and Cenozoic siliceous-clayeysediments. The compositions of these deposits can be used asreference ones, indicating a change in the sediment geochem-istry at the point moving together with the underlying platefrom the central part of the ocean to a volcanic arc. Thestudied Sutyr’ and Kimkan units are similar to the volcano-genic deposits of the upper core of the Izu–Bonin trench, thuspointing to the sedimentation near the boundary between thecontinental margin or arc and the ocean. As seen from thediagram, hydrothermal-sedimentary enrichment with metals,similar to that in mid-ocean spreading zones, was hardlypossible during the accumulation of the studied ancient strata.
The compositional trend of the studied rocks shows aserious change in Al/Fe and a minor change in La/Ce, whichpoorly agrees with the model for the sedimentation evolutionfrom pelagic to continental-margin. The Fe depletion andalumina enrichment might be due to postsedimentary (oreformation?) processes.
The provenances
The nature of sources of the studied rocks was establishedfrom the discrimination diagrams proposed by Roser andKorsch (1988). As seen from Fig. 8, the petrochemicalcomposition of the parental rocks of the Sutyr’ unit isdetermined by felsic igneous and quartz-rich sedimentaryrocks. The significant contribution of biogenic silica, indicatedby the siliceous-carbonaceous composition of some deposits,cannot be ruled out either. The Kimkan rock unit formed fromrocks of basic and intermediate compositions and, to a lesserextent, from redeposited sediments.
Judging from the isotope characteristics of carbon (Ta-ble 4), the shales of both rock units are enriched in biogenicorganics.
Precious-metal specialization
Table 5 presents some petrochemical modules (Yudovichet al., 1998) calculated from data on the chemical compositionof rocks from some gold and PGE deposits and occurrenceshosted by carbonaceous strata in Australia, China, Brazil,Uzbekistan, India, and Russia, as well as the modules for therocks of the Kimkan and Sutyr’ rock units. The precious-metalspecialization of these complexes is best indicated by the TAMand AM modules (Fig. 9). Ore-bearing rocks with elevatedPGE contents show high K2O/Na2O values (3.6–40), thoughthe K2O + Na2O content is low (0.1–3.1 wt.%). Gold oresshow, on the contrary, low K2O/Na2O values (0.5–6.3) buthigh K2O + Na2O content (4.3–7.8 wt.%). According to thetotal content of alkalies and K2O/Na2O ratio, the shales andFe-ores of the Kimkan rock unit are obviously the Pt-bearingprospects. The alkaline properties of the Sutyr’ unit rocks aresimilar to those of black shales bearing gold deposits.
Figure 9 shows the fields of rock groups with similaralkalinity modules. These are mainly complexes with the sameore specialization and geologic characteristics of mineraliza-tion. The average values of petrochemical modules for thesegroups are given in Table 6.
The average AM value of rocks with high (commercial)PGE contents (field I) is more than six times higher than thatof rocks in other fields (groups), with the minimum valuehigher than 4. The total K2O + Na2O content in them does
Fig. 6. log(K2O/Na2O)–SiO2 discrimination diagram for sandstone–mudstones,after Roser and Korsch (1986). PCM, passive and ACM, active continentalmargins; IA, island arcs.
Fig. 7. (La/Ce)n–Al2O3/(Al2O3 + Fe2O3 tot) discrimination diagram for siliceousdeposits, after Murray (1994), with the evolution trend of sediments from DSDPborehole 1149 drilled on the oceanic slope of the Izu-Bonin trench (Plank et al.,2007). Roman numerals mark the rock unit numbers. The contents of La and Ceare normalized to the NASC shale standard (Gromet et al., 1984).
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not exceed 3 wt.%, with the average being <2 wt.%. Theaverage IM value in the rocks with high PGE contents isalmost twice higher than that in other rocks. The hydrolysationmodule shows the widest variations in each group. Its averagevalue is the highest in the PGE-rich rocks, but the differencein its values between the groups is within the statistical error,and its indicatory role for altered rocks with precious-metalmineralization must be refined.
The difference between the Sutyr’ and Kimkan carbona-ceous units with different precious-metal specialization is alsoexpressed in the frequency of occurrence of microinclusionsenriched in Pt and Au. In the Kimkan shales, 32.8% ofmicroinclusions are enriched in Pt, while it is only 12.8% inthe Sutyr’ rocks. In contrast, Au-containing inclusions showan opposite tendency—8.6 and 10.3%, respectively.
Discussion
Carbonaceous shales of the Kimkan and Sutyr’ rock unitsbelong to terrigenous-carbonaceous and siliceous-carbona-ceous formations. They accumulated in deep-water environ-ments near the source of volcanoterrigenous clastics, e.g., inthe trench above subduction zone, and the active continentalmargin was probably the main feeding province. Note that thepresent-day zones of deep-water trenches are as wide as400 km and more, i.e., they are large sedimentary basins.Associations of different sedimentary rocks, such as siliceous-clayey shales, jaspers, limestones, and dolomites of pelagicand hemipelagic nature, on the one hand, and typical ter-rigenous siltstones and sandstones, on the other, might be theresult of their synsedimentary mixing in subduction zone.
The abundance of organic carbon in the rocks of both units,especially containing biogenic(?) silica and carbonates, is bestexplained by the intense vital activity of microorganisms(mainly phytoplankton) in zones of the ascent of deep-seatednutrient-rich waters near continental or island-arc slopes onthe ocean margins, such as those in the Peru–Chile Trench.Favorable conditions for the progression of microorganismsand bottom algae might also have existed in the well-ventilatedand heated shelves of marginal seas, where their remnants,together with terrigenous material, must have been washed offinto neighboring deep-water basins.
It was shown earlier that carbonaceous terrigenous-sedi-mentary strata and precious-metal ores formed in them haveparticular petrochemical characteristics, different for com-plexes with predominantly PGE and gold mineralization.These properties are equally expressed on different continentsand do not depend on the rock age and ore-bearing structures.According to these characteristics, the studied shales andFe-ores of the Kimkan rock unit are obviously PGE-rich oreprospects, and the Sutyr’ unit rocks are similar to black shalesbearing gold deposits.
Table 4. Isotope characteristics of carbon in shales of the Sutyr’ and Kimkanrock units
Rock unit Shales Sample no. Corg, % δ13CVPDB, ‰
Sutyr’ Highlycarbonaceous
565 4.77 –23.1
653 5.07 –20.9
6411 2.64 –23.1
561 3.6 –22.7
570 7.2 –21.0
567 7.9 –23.7
Phyllite-like 563 0.5 –20.7
Kimkan Highlycarbonaceous
514 2.0 –23.3
681 2.01 –18.9
KI–9 4.28 –16.9
Carbonaceous 695 0.4 –17.6
543 0.3 –19.1
Note. Analyses were carried out in the Laboratory of Stable Isotopes at theFar Eastern Geological Institute, Vladivostok (analyst T.A. Velivetskaya).
Fig. 8. Discrimination diagrams for the sources of sandstone–mudstones strata,after Roser and Korsch (1998), using: a, concentrations of major rock-formingelements; b, their ratios.
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Table 5. Petrochemical modules calculated from the chemical composition of ores and the host rocks of large gold and PGE deposits
Note. Modules were calculated after Yudovich et al. (1998): AM = (Al2O3 + TiO2 + Fe2O3 + FeO + MnO)/SiO2, IM = (Fe2O3 + FeO + MnO)/(Al2O3 + TiO2),AM = K2O/Na2O, TAM = K2O + Na2O.
Table 6. Average petrochemical modules for groups of ore-bearing objects
Field (Fig. 9) Ore specialization of group objects Number of objects in group AM IM TAM AM
I With high contents of PGE in deposits of different types 11 0.46 0.91 1.84 12.37
II With elevated contents of PGE in gold deposits 7 0.37 0.49 4.77 2.55
III 8 0.32 0.35 6.06 1.39
IV Epithermal gold deposits 2 0.39 0.33 7.46 2.11
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The nature of precious-metal mineralization in carbona-ceous terrigenous complexes is still unclear, but based on ourstudy of such complexes in southern Far East Russia (Berd-nikov et al., 2010; Khanchuk et al., 2007, 2009a,b, 2010a,b),we assume that PGE mineralization is genetically related tothe formation and transformation of carbonaceous rocks.Elevated background contents of platinum in the dispersed (atthe atomic-molecular level) form were revealed in shales(Khanchuk et al., 2010b), where it is present as a widespectrum of microinclusions, from Pt-poor (few at.%) amor-phous ones to Pt-rich (tens of at.%) microcrystals, plates, andfilaments (Berdnikov, 2010). This platinum often shows aparagenetic relation with graphite or other forms of carbon.Most of gold in the carbonaceous shales is native and showsno relation with carbon; it is present in mineral assemblagesresulted from superimposed sulfidization and silicification.The established petrochemical characteristics seem to reflecta different character of the processes resulting in predomi-nantly PGE or gold mineralization in carbonaceous terrigenousrocks. Therefore, carbonaceous complexes with high Fecontents, low total contents of alkalies, and high K/Na ratiosare promising for PGE-rich mineralization. Gold complexesare usually localized in black-shale strata with high totalcontents of alkalies and low K/Na ratios.
This work was supported by grants 10-05-98004-r_sibir’_aand DVO RAN 11-III-D-08-047 from the Russian Foundationfor Basic Research.
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