Vol. 44 No.

11

SCIENCE IN CHINA (Series D)

November 2001

PGE geochemistry of Jiding ophiolite in Tibet and its constraint on mantle processes
XIA Bin ([ )1,2, CHEN Genwen (/6!)1, MEI Houjun ( X)1, GUO Lingzhi ( a)3, XIAO Xuchang ( )4, YU Hengxiang ( QI Liang (< )2, WANG Guoqiang ( )1 & ZHONG Zhihong (
1. Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China; 2. Open Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550002, China; 3. Department of Geosciences, Nanjing University, Nanjing 210093, China; 4. Institute of Geology, Chinese Academy of Geological Sciences, Beijing 100037, China Correspondence should be addressed to Xia Bin (email: xiabing@public.guangzhou.gd.cn) Received March 29, 2001

)1, )1

Abstract The total PGE amount (PGE) of mantle peridotite in the Jiding ophiolite is slightly higher than that of the primitive mantle, but the PGE contents of basalt are higher than those of the mid-ocean ridge basalt (MORB), with obviously lower Pd/Ir ratios. The accumulates, dyke swarm and basalts show remarkable negative Pt and positive Rh anomalies, resulting in the special N-type PGE patterns. Mantle peridotite and crustal rocks have similar distribution patterns. It is proposed that the PGE distribution patterns in the Jiding ophiolite are closely related with a higher degree of partial melting of the mantle in this region. Magmatic crystallization-differentiation led to PGE fractionation, thus making the contents of PGE in the accumulates decrease in the ascending direction. The higher content of Au in the Jiding ophiolite is the result of metasomatic alteration at later stages. Pt-Pd fractionation indicates that both the PGEs are controlled by their alloy and sulfide phases. Positive Rh anomalies seem to be related with higher oxygen fugacity in the melts.
Keywords: platinum group element (PGE), geochemistry, ophiolite, upper mantle, Jiding of Tibet.

The platinum group elements (PGE) are distributed largely in basic and ultrabasic rocks in nature, and 99% of the PGE occurs in magmatic sulfide deposits throughout the world[1]. As the PGE and Au have similar properties, they are always used together to study the evolution of mantle materials, core/mantle differentiation, the distribution of Earths materials in the early periods of time, mantle processes, meteorite impact events, the origin of basalts and the genesis of PGE-bearing magmatic sulfide deposits and chromite deposits[26]. In recent years we have made detailed investigations on the PGEs in ophiolites developed in the Yarlung Zangbo River suture zone[7]. This paper focuses on the PGE geochemistry of the Jiding ophiolite and its relations with the mantle processes. 1 Samples and analytical methods The Yarlung Zangbo River ophiolite zone is considered to represent the early tectonic background of the oceanic basin[813]. The Jiding ophiolite is located in the middle segment of the Yar-

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Yarlung Zangbo River suture zone and is one of the well developed ophiolite zones in China (fig.1). It was formed during the Early Cretaceous. In the Jiding ophiolite mantle peridotite, accumulate, dyke swarm, pillow basalt and radiolarian chert are developed. The mantle peridotite is composed mainly of harzburgite. In going downwards the rock grades to lherzolite; in going upwards, dunite. The rocks have been ophiolitized. The accumulate zone has been obviously differentiated with its lower part consisting of diallage peridotite, olivine diallagite and diallage gabbro and in going upwards the rock facies grades to stratiform gabbro and isotropic gabbro. Wang et al.[9,10] classified the accumulate zone into: (1) the critical zone or transitional zone at the bottom; (2) the layered complex zone; and (3) the isotropic gabbro zone. The dyke swarm is composed of gabbro diabase and diabase. Dolerite and pillow basalt are recognized at the top. The studied samples in this work include harsburgite and dunite in the mantle peridotite, diallage gabbro and gabbro in the accumulates, diabase in the dyke swarm in the lower part, and basalt in the upper part. The samples were taken almost from every part of the ophiolite section. Sample analyses were made by Qi Liang at the Open Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences. The samples were fused and decomposed with Na2O2, coprecipitated with Te, and analyzed by using isotope dilution-ICP-MS techniques. Twice coprecipitation with Te was conducted to purify HCl and SnCl2 in the chemical reagents used for analysis. The analytical instrument Finnigan MAT ELEMENT Model high resolution ICP-MS was employed in this study. The technical detection limit (109) was Ir 0.02, Ru 0.045, Rh 0.024, Pt 0.23, Pd 0.11, and Au 0.32. The detailed analytical procedure was described in ref. [14]. Ni, Cu and Cr were determined using ICP-MS techniques.

Fig. 1. Sketch map showing distribution of the Jiding ophiolite (from ref. [9]). 1, Cretaceous; 2, basalt; 3, diabase; 4, sheeted sill; 5, cumulate; 6, gabbro; 7, harzburgite and dunite; 8, fault; 9, sampling section.

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2 The contents of PGE and Au and their distribution 2.1 The contents of PGE and Au mantle peridotite The contents of PGE and Au in the mantle peridotite in the Jiding ophiolite of Tibet vary over a narrow range (table 1), but the contents of PPGE (Pt and Pd) vary a little more greatly than those of IPGE (Ir and Ru). The total amount of PGE is 1.4 2.3 times that of the primitive mantle (20.6 109)[15,16]. The Pd/Ir ratios range from 0.67 to 2.49. The total amount of PGE in harzburgite and pyroxene-bearing dunite is (27.6930.1) 109 and 46.25 109, respectively, being 1.4 and 2.3 times that of the primitive mantle peridotite. As compared with the harzburgite, the pyroxene-bearing dunite is obviously enriched in Pd, Pt and Au.
Table 1 PGE and Au contents of the Jiding ophiolitea) Ir JD-42 Harzburgite JD-43 Harzburgite JD-44 Pyroxene-bearing dunite JD-50 Orthopyroxene peridotite JD-51 Gabbro troctolite JD-52 Gabbro troctolite JD-57 Dark-colored pyroxenite JD-59 Diallage gabbro JD-63 Diallage gabbro JD-66 Diallage gabbro JD-72 Diallage gabbro JD-80 Diabase JD-81 Diabase JD-83 Diabase JD-84 Diabase JD-85 Diabase JD-111 Basalt JD-112 Basalt JD-116 Basalt JD-119 Basalt JD-122 Basalt JD-123 Basalt JD-125 Basalt Primitive mantle 6.49 7.60 7.01 4. 41 0.83 7.33 0.88 0.52 0.70 0.68 0.59 0.67 0.98 0.64 0.57 0.82 0.75 1.18 0.86 0.78 0.54 0.73 0.63 3.6 Ru 7.98 9.81 8.70 10.99 2.11 1.96 1.02 1.40 0.85 2.30 1.22 1.75 1.26 1.80 1.29 0.60 1.78 0.83 3.19 1.63 1.33 1.70 0.54 4.3 Rh 0.98 0.95 1.02 5.94 4.96 0.99 0.76 1.45 1.53 0.54 1.22 9.62 0.82 3.30 1.77 1.04 1.01 0.54 2.97 0.63 0.48 1.35 0.81 1.7 Pt 6.90 4.55 12.10 9.29 2.90 11.21 1.98 1.22 2.53 0.51 0.00 2.85 0.17 0.75 0.06 0.45 0.44 0.50 2.80 0.25 0.76 0.61 0.16 7 Pd 7.75 4.77 17.42 6.63 6.04 5.94 1.32 1.98 1.63 1.39 1.18 3.31 3.31 4.99 2.88 3.71 2.52 1.22 6.26 1.25 0.90 1.17 1.37 4 Au 22.39 22.52 38.15 7.01 4.95 10.83 15.58 5.18 3.17 7.43 4.99 3.75 4.25 3.88 3.56 2.46 2.90 2.81 2.42 2.42 4.08 3.51 2.86 1 PGE 30.10 27.69 46.25 37.26 16.84 27.43 5.96 6.52 7.24 5.42 4.21 18.20 6.54 11.48 6.54 6.62 6.50 4.27 16.08 4.55 4.01 5.56 3.51 20.6 Cu 7.58 9.35 7.43 13.89 146.57 145.53 60.94 51.60 81.51 71.25 111.82 9.99 6.60 57.28 52.89 56.06 16.75 14.17 38.48 30.05 56.25 34.09 29.63 28 Ni 1842.81 2133.85 1778.13 1804.82 336.57 32277 106.47 131.31 108.47 136.23 134.80 7.20 14.85 66.08 50.11 47.19 9.95 9.55 41.89 8.84 45.82 21.87 24.96 2110

a) PGE and Au in 109; Cu and Ni in 106. Pt of the primitive mantle are from ref. [15]. The other PGE and Au data of the primitive mantle are from ref. [16], and Cu and Ni data from ref. [17].

The total amount of PGE is (4.2137.26) 109, showing a wide range of variations. As compared with accumulates in ophiolites of Bay of Island district[18], orthopyroxenite in the accumulates is extremely high in PGE contents while clinopyroxenite shows a great variation in PGE contents, which is considered as an outstanding feature of ophiolites in the orogenic belt. In the Troodos ophiolite suite the contents of PGE in the upper portion of gabbro are within the range

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of (11 22.5) 109 and those in the lower portion may reach 100 109[19]. The total amount of PGE in gabbro in the KKdi ophiolite of West Kunlun is estimated at (2.420.59) 109 and that of pyroxenite ( 2.3723.98 ) 109[20]. The situation is similar to that in the region studied. There have been recognized two PGE-high horizons in the lower part of the accumulate at Jiding. This case has been also encountered in the Troodos complex, but its PGEs are concentrated mainly in the chromite and sulfide-high horizons in the lower part. However, in the region studied no chromite horizon has yet been found, and microscopic observations have not revealed any sulfide. The contents of PGE, especially Ir, Pd, Pt and Ru, in the section show a tendency of decreasing from the bottom to the top. This indicates that in the course of formation of the accumulate the crystallization-differentiation would have constrained, to some extent, the fractionation of PGE. The Pd/Ir ratios are within the range of 0.817.27 and Pd/Pt ratios, 0.532.73 (excluding sample DJ-72). The Pd/Ir and Pd/Pt ratios in the most majority of the samples are higher than those of chondrites and primitive mantle. The contents of Au in ophiolite are abnormally high and show little variation, i.e. the contents of Au in the different rocks show little variation. The contents of PGE are highly variable from one rock type to another in the Jiding ophiolite, which tend to decrease in the order of mantle peridotite accumulate diabase and basalt.

2.2 PGE distribution patterns The chondrite-normalized PGEs were plotted in the order of their melting points (fig.2). The PGE distribution patterns in the mantle peridotite are of irregular U-shape, different from the smooth PGE distribution patterns in the primitive mantle peridotite. The IPGE values of peridotite samples are very close to each other and they are relatively concentrated in the normalized pattern diagrams. Comparatively, the PPGE values of the samples show a significant difference. Dunite is obviously richer in PPGE than harzburgite, with (Pd/Ir)N ratios being 0.562.24 and (Pd/Pt)N, 1.83 2.52. Negative Pt anomalies [21] are dominant, with (Pt/Pt*=PtN/SQRT (RhNPdN)) ranging from 0.79 to1.07. Some similarity has been observed in PGE distribution patterns between gabbro and diabase, i.e. the PGE distribution patterns are of N-type. In other areas such PGE distribution patterns can be observed in chromite, and sulfides and komatiites in a part of the ophiolite suite, the marginal belt and main belt of the Bushveld Complex and the chromite bed at the bottom of the Stillwater stratiform intrusive rock[22]. Similar PGE distribution patterns have also been observed in the sulfide-bearing gabbro in the Troodos ophiolite suite[19]. (Pd/Ir)N values of the gabbro are within the range of 0.736.59. With the exception of one sample, the ratios in all the rest samples are larger than unity, reflecting that the pattern curves are of the positive slope type. The Pt/Pt* ratios vary from 0.19 to 2.37. Except one sample, all the rest samples show negative anomalies. The ratios of several specific PGEs in the diabase are similar to those of gabbro, but the diabase shows more remarkable Pt anomalies than gabbro, as indicated by much lower Pt/Pt* ratios, ranging from 0.01 to 0.18. These rocks are all possessed of similar PGE distribution patterns. In comparison to the mantle peridotite the other types of rocks show a PGE distribution pat-

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terns with a much larger slope and much bigger variations.

Fig. 2. The PGE distribution patterns in the Jiding ophiolite (the numbers are the same as in table 1).

3 3.1

Discussion

The influence of partial melting of the upper mantle on PGE fractionation The contents of CaO in three mantel peridotite samples from the Jiding ophiolite are 0.1%, 0.01% and 0.5%, and their Al2O3 contents are 0.14%, 0.09% and 1.63%, respectively, indicating a strongly depleted residual mantle left behind a higher degree of partial melting. In combination with the REE contents of mantle peridotite and basalt in the Jiding ophiolite, both the rocks show LREE depletion and their (La/Yb)N ratios are 0.47 and 0.39, respectively. The La contents of peridotite are within the range of (0.02 0.10) 106 and its REE (excluding Y) values are (0.571.03) 106; the La contents of basalt are within the range of (2.49 3.10) 106 and its REE (excluding Y) values are (35.40 61.26) 106, also indicating that the mantle in this region has undergone a high degree of partial melting. The mantle peridotite in the Jiding ophiolite is depleted in Rh while the crustal rocks are enriched in Rh, more or less indicating that the PGE is related with partial melting of the upper mantle. The PGE distribution patterns in the mantle peridotite of the Jiding ophiolite have a slightly positive slope. If Rh is not taken into consideration, the PGE distribution patterns in the accumulate, dyke swarm and lava in the upper part would be similar to those of the mantle peridotite in

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the lower part (fig. 2). It is shown that the intrusive rocks as a whole have inherited the PGE composition of the mantle peridotite and the PGE distribution patterns are closely related with partial melting of the upper mantle. The lavas have the positive slope-type distribution patterns marked by higher PGE and lower Pd/Ir, inconsistent with the significantly sleep slope-type distribution patterns of MORB but similar to those of komatiites[23]. The PGE distribution patterns of komatiites are considered to be the result of a high degree of partial melting of the upper mantle. Many studies have shown that most of the PGE in the mantle is present in the form of sulfides . However, no sulfide has been found in the peridotite and accumulate samples taken from the region studied, indicating that sulfur in the lava did not reach the saturation state. Some lines of indirect evidence suggest that sulfides do have constraints on the distribution of PGE. For instance, in the lower accumulate there is a horizon where the sulfophile element copper is high, and also a horizon where the PGEs are concentrated. Samples JD-50 and JD-52 can be taken for example in this respect. As can be seen from the Ni/Pd-Cu/Ir plot (fig. 3), distribution of PGE is controlled by some major geological facFig. 3. The plot of Ni/Pd vs. Cu/Ir for the tors. The figure shows that the samples are precisely disJiding ophiolite. The arrow points to the directributed along the direction of sulfide differentiation, intion of differentiation of different minerals[12]. dicating that in the course of magmatic differentiation the In the plot the triangles stand for peridotite samples, and the others are accumulate, diadistribution of PGE is substantially controlled by sulbase and basalt samples. fides. At the present time, such a viewpoint is commonly accepted that the PPGE is present mainly in the form of low-temperature sulfides while the IPGE occurs chiefly as Os-Ir-Ru alloy or high-temperature sulfides in coexistence with spinel[24]. So, in the case of a low degree of partial melting, the PPGE will find a way, together with some Cu-bearing sulfides, into melts, but the IPGE will be left behind as residues. In this way the PPGE is separated from the IPGE. As a result, in the residual mantle peridotite there appear the PGE distribution patterns marked by a negative slope while in the basalt are produced the positively steep-inclined PGE distribution patterns characterized by low PGE contents. These distribution patterns are significantly different from
[3,20,22]

those of peridotite, as well as of dyke swarm and lava in the upper part in the region studied (fig. 2) because in this region, there is one sample whose PGE distribution patterns are marked by a negative slope, the other two mantle peridotite samples are characterized by a positive slope. Although the PGE distribution patterns of lavas are marked by a positive slope, their Pd/Ir ratios are far smaller than those of lavas in some typical ophiolites. For example, in the Troodos ophiolite suite the pillow lavas have a Pd/Ir range of 90160[21]. In the case of a high degree of partial melting and partial melting proceeding rapidly, the refractory Os-Ir-Ru alloy or high temperature sulfides will melt together with low temperature sulfides, making both compatible and incompatible elements enter into the melts. As a result, the PGE contents of crustal rocks will be enhanced

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and the steep-inclined PGE distribution patterns like those observed in the MORB will not be produced. At the same time, both peridotite and crustal rocks will possess similar PGE distribution patterns, as is further evidenced by Cu and Ni contents of the ophiolites in the region studied. As Ni shows the characteristics of a compatible element during the mantle processes while Cu is an incompatible element, so, in common cases, with increasing degree of partial melting of the mantle, Cu will find its way into melt and the contents of sulfides in the mantle residues tend to become lower and lower. Therefore, the mantle is depleted in S and Cu and enriched in Ni. But the case is not true in the region studied. Peridotites in this region show depletion in Ni and Cu, with the contents of Cu ranging from 7.43 106 to 9.35 106, only equivalent to 1/41/3 of the total in the primitive mantle (28 106). The contents of Ni are also relatively low ((1778.132133.85) 106, averaging 1918.26 106). Cu is positively correlated with Ni, implying that in the process of partial melting Cu and Ni were exported together and also indicating that both elements were controlled by the same geological process in the geological history. This phenomenon can be well explained by the fact that when the mantle underwent a higher degree of partial melting, Ni began to be incorporated into melt, thus making the mantle rocks become depleted in Ni, though the degree of Ni depletion was lower than that of Cu. The influence of magmatic differentiation on PGE fractionation As compared with diabase dykes, the accumulates in this region have relatively high PGE contents, which shows a tendency of decreasing from the lower part upwards. Clinopyroxenite and gabbro-troctolite in the lower accumulates tend to become remarkably enriched in PGE, reflecting that during the crystallization-differentiation of gabbro there occurred PGE fractionation. Such phenomenon has been also observed in accumulates of the Troodos ophiolite suite[18]. The PGE fractionation may be attributed to the differentiation of sulfide and spinel. For example, the two horizons (one is relatively high in spinel and the other is high in copper) in the lower part of accumulates have higher contents of PGE. More PGE is observed in accumulates in the Troodos ophiolite suite. In the horizons where chromite occurs the PGEs are generally high[19]. 3.3 Au enrichment and Rh, Pt depletion As for its distribution in the Jiding ophiotite, Rh features negative depletion in the peridotite 3.2

but shows a positive anomaly in the accumulate, dyke swarm and basalt. It is deduced that Rh fractionation is attributed to extraction which took place in the process of partial melting of the mantle. The chemical properties of Rh lie between those of the PPGE and IPGE. According to the classification proposed by Barnes et al.[22], Rh belongs to the PPGE. In the study of the solubility of Rh in silicates, Amosse et al.[24] and Gueddari et al.[25] reconfirmed its double character, i.e. at 1430 and fO2< 102 Pa Rh possesses the properties of PPGE; in the case of fO2> 102 Pa, Rh will become trivalent. Under this circumstance, Rh is easy to find its way into the lattice of spinel. This is in consistence with the conclusion of Capobianco et al.[26] In the experiments Capobianco et al.

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found strong evidence suggesting that Rh has a good geochemical affinity for spinel and its partitioning coefficient between spinel and fluid is 90. Orthopyroxene peridotite and gabbro troctolite in the lower accumulates in the region studied contain 5.94109 and 4.96109 Rh, respectively. The contents of Rh are obviously higher than those in the gabbro in the upper part. All this provides further evidence for the conclusion of Capibianco et al. However, this could not effectively explain the positive Rh anomalies in the whole accumulate, dyke swarm and basalt. In the study of the PGE distribution patterns in the Bushveld complex, Mairer et al.[27] obtained a series of PGE distribution patterns of accumulates by controlling the composition of starting material, the proportion of monosulfide, the contents of sulfides and other factors. It was found that when the proportion of monosulfide solid solutions exceeded 80%, both silicolite and chromitite would show positive Rh anomaly and negative Pt anomaly. Their PGE distribution patterns are similar to those of accumulates in the region studied. This indirectly evidenced the influence of fO2 on the formation of Rh. Based on the limited knowledge of Rh at the present time, it is considered that the positive Rh anomalies in lavas are the result of Rh and Pd enrichments in the various types of rocks when they were both incorporated into low-temperature sulfides and then exported by melting under the conditions of fast resorption to a higher degree and relatively high fO2. In the lavas Rh negatively correlates with Ir whereas Rh positively correlates with Pd (fig. 4), also indicating that both Rh and Pd have similar geochemical properties.

Fig. 4. Correlations between Rh and Pd and Ir in crustal rocks of the Jiding ophiolite.

In the Jiding ophiolite, either mantle peridotite or oceanic crustal rock possesses remarkable Au anomalies. There is no significant difference in Au contents for the various types of rocks and Au shows a poor correlation with other PGEs, indicating that Au has an independent source. This implies that Au would have resulted from metasomatism of the rocks by extraneous Au-bearing fluids. Such metasomatism seems to have originated from later metasomatic alteration. Field observations disclosed that the rocks have been serpentinized . Although this study did not deal with the influence of serpentinization on the migration of PGE, the fact that the contents of PGE in some strongly serpentinized rock samples are relatively constant suggested that the PGE maintained

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constant in the process of serpentinization. Previous studies [4,18,22] indicate that metasomatic alteration would not lead to PGE migration, though it could make Au remobilize and migrate. Negative Pt anomalies in the mantle peridotite are closely related with the unique properties of Pt itself. Studies have shown that the partition coefficient of Pt between alloy and sulfide melt is 1000 times that of Pd[2]. In the case of alloy-sulfide coexistence, Pt shows a strong tendency of entering into the alloy phase. Sulfides separated from melts are rich in Pd. Partial melting of the mantle led to the separation of Pt from Pd in the crustal rocks and ubiquitous depletion in Pt. 4 Conclusions

From the above analysis we can come into the following conclusions: (1) The total PGE amount of mantle peridotite in the Jiding ophiolite is slightly higher than that of the primitive mantle and the PGE contents of basalt are higher than those of MORB, with distinctively lower Pd/Ir ratios. The contents of Au in the ophiolite are commonly high. As observed in the accumulate, dyke swarm and basalt are negative Pt and positive Rh anomalies. The mantle peridotite and crustal rock have similar PGE distribution patterns. (2) The PGE distribution of the Jiding ophiolite is related with the higher degree of partial melting of the mantle in the region studied. (3) The high contents of Au in the Jiding ophiolite are attributed to later metasomatic alteration. Pt-Pd fractionation indicated that they were both controlled by alloy phase and sulfide phase, respectively. Positive Rh anomaly may be related with relatively high fO2 in the melt. (4) Crystallization-differentiation of the accumulates led to PGE fractionation and caused PGE in the accumulates to decrease in the ascending direction.
Acknowledgements Thanks are due to Prof. Xu Yigang for his valuable comments. This work was financially supported jointly by the National Natural Science Foundation of China (Grant No. 49772109), the National Climbing Program of China (Grant No. 95-Yu-25-03), and the National Key Basic Research Program of China (Grant No. 1999043204).

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