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THE DEVELOPMENT OF Re-Os ISOTOPE GEOCHEMISTRY IN CHINA

 

ZHI Xiachen,  XIA Qiongxia,  MENG Qing,  JIN Yongbin and ZHENG Lei

School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China

 

The Re-Os isotope system, based on its unusual qualities, has been widely used on the dating and tracing in the geoscience and geochemistry. As a reflection of the international development of the Re-Os isotope geochemistry, Chinese geoscientists have also done a large quantity of work in this research field. In China from 1993 to 1996, the main work was focus on the determination of Re-Os isotope model age of molybdenite from ore deposits by isotope dilution and inductively coupled plasma mass spectrometry (ID-ICPMS), then from 1997 to 2002 mainly on the determination of Re-Os isotope system by negative thermal ion mass spectrometry (N-TIMS) and the applications to the Re-Os isotope geochemistry of mantle peridotite xenoliths, also on the precise and accurate dating of molybdenite from ore deposits by ID-N-TIMS and with 186Os-188Os double spikes and by Os-Os technique. In this paper we mainly describe the development of Re-Os isotope geochemistry in China based on the Chinese publications issued at home. These include: 1) the methods of analysis and determination of Re-Os isotopic systematics in geological samples; 2) the geochronology and technique of Re-Os isotope system for metal ore deposits; 3) the dating and tracing of sub-continental lithospheric mantle (SCLM) by Re-Os isotope system; 4) miscellaneous fields; 5) the introduction and review of international development of Re-Os isotope geochemistry; 6) the references of Re-Os isotope geochemistry published by Chinese scientists, mainly in Chinese at home and a few in English abroad.

 

I.  The METHODS OF analysis and determination of Re-Os isotopic systematics in geological samples

In early 1990's ID-ICPMS was first used to the Re-Os isotope model age of molybdenite from metal ore deposits by researchers at Institute of Rock and Mineral Analysis, Chinese Academy of Geological Sciences in China (Du et al., 1993, 1994; He et al., 1993, 1994). They presented their technique of Re-Os isotope geochronology of molybdenite as follows: Samples were dissolved and equilibrated with 185Re- and 190Os-enriched spikes by alkaline fusion. Separation of rhenium from matrix elements was effected by solvent extraction and cation exchange chromatography while osmium was distilled as OsO4 from H2SO4-Ce (SO4) 2 solution. All rhenium and osmium isotopic measurements were made on a VG plasma Quad facility. Total chemical recoveries for both elements were greater than 90% and total procedural blanks were 0.07ng and 0.01ng for Re and 187Os respectively.

In the determination of Re-Os isotopes for molybdenites by ICP-MS, for different solution and different condition of distillation, the chemical behavior of Os is different. The measured count rate of Os() is 50 times as great as that of Os(,) when introducing the sample solution with a Meinhard concentric nebulizer (He et al., 1993, 1994).

Then N-TIMS was used to the low-level, low-blank and high-precise Re-Os isotope system of geological samples, which was first done by the researchers at the department of Earth and Space Sciences, University of Science and Technology of China in China (Sun et al., 1997a, b). The ID-N-TIMS technique was used to measure the osmium composition in mantle peridotite xenoliths (Sun et al., 1997c). This technique was also used to the Re-Os isotope geochronology of molybdenite together with the Carius tube digestion of samples (Du et al., 1998, 2001; Zhao et al., 1998), also to obtain high-precise results for both PGEs concentrations and the Os isotope compositions combing with a new sample digestion (HPA-S), a modified chemical separation method with solvent extraction and anion-exchange resins (Yang et al., 2001).

In addition, the Os-Os technique (Gao et al., 1999; Gao & Li, 2001) was used in Re-Os dating of molybdenites. In the technique 186Os and 188Os can be obtained by decay of 186Re and 188Re respectively, which come from the nuclear reaction 185Re(n, ) 186Re and 187Re(n, ) 188Re. The yields of 186Os and 188Os depend on the neutron flow in the reactor and the Re contents of the sample being irradiated. So the Os-Os age can be obtained from Os isotope ratios.

And 186Os-188Os double spikes combining with ID-ICPMS (Qu et al., 2001a; Qu et al., 2001b) are also used to the Re-Os isotope geochronology of molybdenite. The advantage of this method is that 186Os and 188Os double spikes can effectively compensate for the mass discrimination effects of ICP-MS, therefore the common correction practice for mass bias in the isotope dilution method with a single spike is unnecessary. In addition, the method enables one to reduce the determination error arising from instrumental instability.

 

II.  The GEOchronology and techniques of Re-Os isotope system of metal ore deposits

Based on the ID-ICPMS technique of Re-Os determination, the first and important application of the Re-Os isotope system is the metallochronology of metal ore deposits in China.

Huang et al. (1994) reported the geochronology of molybdenites from the East Qinling Mo ore belt, which lies on the southern margin of the North China Craton. (1) For 5 samples of molybdenites from Huanglongpu carbonatite type Mo-Pb ore deposits, Shanxi Province, the Re and Os contents are 284-633 ppm and 670-1430 ppb respectively, subsequently Re-Os model age is 220-230 Ma; (2) For 3 samples of molybdenites from Jinduicheng porphyry Mo ore deposits, Shanxi Province, the Re and Os contents are 13-20 ppm and 8-12 ppb respectively, therefore Re-Os model age is 29-139 Ma; (3) For 1 samples of molybdenites from Shijiawan porphyry Mo ore deposits, the Re and Os contents are 100 ppm and 14 ppb respectively, then Re-Os model age is 138 Ma; (4) For 5 samples of molybdenites from Nannihu-Sandaozhuang porphyry-skarn type Mo-W ore deposits, Henan Province, the Re and Os contents are 13-54 ppm and 20-81 ppb respectively, consequently the Re-Os model age is 146-156 Ma. All molybdenites mentioned above are 2H or 2H3R type in polymorph, and the error of the Re-Os model age is 3%4%. The authors suggested that the formation of the carbonatite type Mo-Pb ore deposits were associated with the minerogenic materials derived from the upper mantle.

Chen and Li (1994, 1998) reported the geochronology of molybdenites from the Tongkuangyu porphyry Cu ore deporsits in the Zhongtiao mountain, of which the Re and Os contents of 6 samples of fine vein disseminatedCdisseminated type molybdenites are 6-650 ppm and 0.2-20 ppb respectively, then the model age is 2883-3065 Ma, and the Re-Os isochron age is 194728 Ma. And the Re and Os contents of another 6 samples of fine vein type molybdenites from the same locality are 7-152200 ppm and 0.2-3332 ppb, then the model age is 2076-2140 Ma, and the Re-Os isochron age 210832 Ma. In terms of different isochronic ages the authors suggested that the formation of the Tongkuangyu porphyry copper deposit underwent a multistage and complex ore-forming processes.

Liu et al. (1996) reported the geochronology of molybdenites from the NO.8 group (H8) of the eastern orebody of Bayan Obo REE ore deposits, the Re and Os contents are 49 ppm and 224 ppb respectively, subsequently the Re-Os model age is 4398 Ma. This result proves previous conclusion that there existed an ore-forming process in Caledonian period in the area.

 

Li et al. (1996) reported the Re-Os isotope geochronology of 6 samples of molybdenites which is 2H1 type in polymorph from the Shizhuyuan W-Sn-Mo-Bi-Be polymetallic ore deposits, the Re and Os concentrations are around 1 ppm and 4-19 ppb (but one is 165 ppb) respectively, the 187Re /186Os ratio is 24670-287, the 187Os /186Os ratio is 64.6-2.9, consequently the Re-Os isochron age is 151.03.5 Maand the initial ratio of 187Os /186Os is 2.170.08.

Huang et al. (1996) also reported that the Re-Os isotope ages of molybdenites from the northern margin of Yanliao Mo ore belt in the North China Craton. (1) the Re and Os contents of 4 samples of molybdenites and 1 concentrated molybdenite from Lanjiagou porphyry Mo ore deposits are 5-82 ppm and 9-11 6ppb respectively, then the model age is 185-192 Ma, and the isochron age is 186.50.7 Ma; (2) the Re and Os contents of 4 samples of molybdenites from Yangjiazhangzik and Xiaojiayingzi skarn type Mo ore deposits are 34-120 ppm and 65-217 ppb respectively, therefore the model age is 177-191 Ma; (3) the Re and Os contents of 1 sample of molybdenite each from Xiaosigou and Shouwangfen porphyry-skarn Cu-Mo ore deposits are 11 and 37 ppm, 16 and 51 ppb, and the model age are 134 and 148Ma respectively; (4) the range of Re content of 1 sample of molybdenite and 4 samples of molybdenites from Dawang porphyry-skarn type Mo ore deposits and Dazhuanke explosive breccia type Mo ore deposits is 11-20 ppm, the range of Os content is 17-30 ppb, and the model age is 144-147 Ma respectively; (5) the Re and Os contents of 2 molybdenites from Bizigou sedimentary metamorphic Cu-Mo ore deposits are 31-579 ppm and 646-11600 ppb respectively, then the model age is 1919-1980 Ma.

Wang et al. (1997) reported that the Re-Os isotope ages of molybdenites from the Anjishan Cu ore deposits and Tongshan Cu-Mo ore deposits in the Nanjing-Zhenjiang mountain, of which the Re and Os contents of the Anjishan molybdenites are 326 ppm and 361 ppb respectively, therefore the Re-Os model age is 108 Maand the Tongshan molybdenites which is 2H1 type in polymorphy, the Re and Os contents are 144 ppb and 90 ppb respectively, consequently the Re-Os model age is 106 Ma.

Zhao et al. (1997) reported that the Re-Os isotope age of molybdenite from Duobaoshan and Tongshan porphyry Cu-Mo ore deposits. The Re and Os contents of 5 samples of molybdenites are 303-822 ppm and 208-4288 ppb respectively, then the Re-Os model age is 476-521 Ma, but this age is quite different from the lithogenetic and metallogenetic ages of the deposits. In addition, also reported another molybdenite from Wunuketushan Cu-Mo ore deposits, the Re and Os contents are 50.9 ppm and 81 ppband the Re-Os model age is 155 Ma.

Wu and Zou (1997) reported that the Re-Os isotope age of molybdenites from Chenmenshan Cu ore deposits, Jiangxi Province. The Re and Os contents are 3.6-11.9 ppm and 5.3-22.3 ppb respectively, and the 187Os C187Re isochron age is 1402Ma.

Mao et al. (1999) reported 5 samples of molybdenites from the Xiaoliugou W-Mo ore deposits in the northern Qilian mountains, the Re and Os contents are 0.8-8.4 ppm and 3.9-42.8 ppb respectively, then the Re-Os model age is 436-496 Maand the 187Os C187Reisochron age is 46213 Ma.

Mao and Du (2001) reported the Re-Os ore-forming age of the ores from Dapoling, Xiaopoling and Qingmingshan in Baotan, Guangxi Province. Of which the Re and Os content of 8 ore samples are 2-657 ppb and 3.8-125 ppb respectively, the 187Re /188Os ratio is 1.51-53.2, the 187Os /188Os ratio is 0.127-0.986. Subsequently the Re-Os isochron age of Cu-Ni sulfide ore deposits is 98221Ma, and the initial ratio of 187Os /188Os is 0.1020.010.

 

III.  The dating and tracing of sub-continental lithospheric mantle (SCLM) by Re-Os isotope system

The application of Re-Os isotope system to the tracing and dating of sub-continental lithospheric mantle (SCLM) is another important research field of Re-Os isotope geochemistry developing in China in addition to the dating of molybdenite.

Zhi et al. (1996) first reported the osmium isotope compositions of Cenozoic basalts and their peridotite xenoliths from Anhui and Jiangsu Provinces determinated by ID-ICPMS techniques (Du et al., 1995).

Sun et al. (1997c) and Zhi et al. (1999, 2001a) reported the Re-Os isotope geochemistry of mantle-derived peridotite xenoliths, which was included in the Cenozoic basalts along the boundary between Jiangsu and Anhui Provinces by N-TIMS. The osmium isotope composition of whole rock, 187Os/188Os is 0.119-0.129, which indicates that most of the mantle-derived peridotite is depleted in Os isotope compositions. This is deduced from the linear correlation between 187Os/188Os ratio and the major element compositions such as Al2O3, the formation age of SCLM in this region is Proterozoic.

Zhi et al. (2001b, c, 2002) reported the Re-Os isotopic systematics of more than 40 samples of peridotite xenoliths from Anhui and Jiangsu Provinces collaborated with French scientists, which were analyzed in the laboratory of CRPG/CNRS in France. The range of Re and Os contents and 187Os/188Os ratio are 0.018-0.375 ppb, 0.921-3.35 ppb and 0.115-0.134 respectively. Based on the correlation between osmium compositions and the index of melt depletion degree, such as Al2O3, Yb and Lu etc., the formation of SCLM in this region is middle Proterozoic. The spinel phase lherzolites in upper mantle may be the residual parts of the middle Proterozoic SCLM survived the delamination after formation.

Gao et al. (2002) reported the Re-Os data for Chinese peridotite xenoliths determined in the Carnegie Institution of Washington, USA, collaborated with American scientists. Their sample set includes 3 samples of peridotite xenoliths contained in the Ordovician kimberlites from Fuxian and Mengyin in the eastern North China Craton, 10 samples of peridotite xenoliths in the Qixia Cenozoic basalts, Shandong province, and 11samples of peridotite xenoliths in the Hannuoba Cenozoic basalts from Trans-North China Craton Orogen. The range of Re and Os concentrations of these samples are 0.008-0.293 ppb and 0.54-9.2 ppb respectively, and the ratio of 187Os/188Os and 187Re/188Os are 0.119-0.130 and 0.016-0.480 respectively. 7 of 10 samples from Hannuoba show a 187Os/188Os-187Re/188Os isochron, and the age is 1910220 Ma. The model age TRD of 2 samples from Fuxian is 2.5-2.8 Ga, 1 sample from Mengyin is 1.46 Ga, and 10 samples from Qixia is 0.13-1.33 Ga. The authors concluded that the peridotite xenoliths from Fuxian and Mengyin are the presence of ancient lithosphere beneath the Eastern Block of North China Craton until Ordovician, the peridotite xenoliths from Hannuoba represent the residual fraction of the Proterozoic mantle replacing the Archean SCLM, and the peridotite xenoliths from Qixia represent the formation of Phanerozoic new lithosphere after the removal of older lithospheric mantle, and the SCLM replacement is associated with the Mesozoic collision-subduction between Yangtze and North China Cratons.

Wu et al. (2002, in press,) reported the Re-Os data for Chinese mantle-derived peridotite xenoliths determined in the University of Maryland, USA, collaborated with American scientists. The sample set includes 18 samples of mantle-derived peridotites in the Cenozoic basalts from Shuangliao and Wangqing volcanic fields, Xing'an-Mongolian Orogenic Belt (XMOB), and 11 samples of mantle-derived peridotites in the Cenozoic basalts from Longgang volcanic fields in North China Craton. The range of Re and Os concentrations are 0.01-0.49 ppb and 0.1-5.1 ppb respectively, and the ratio of 187Os/188Os and 187Re/188Os are 0.117-0.127 and 0.024-0.926 respectively. The authors suggested that the most refractory xenoliths (Al2O3 < 1.2 wt. %) from both tectonic blocks yield Os model ages (TRD) between 1.2 and 0.4 Ga. For the XMOB, this indicates that some portions of the underlying SCLM are approximately the same age as the overlying continental crust. This is typical of the age relations between SCLM and the overlying crust for most cratons in the world. The refractory xenoliths with minimally depleted 187Os/188Os, however, suggest the addition of much younger, Phanerozoic lithospheric mantle. The lack of any xenoliths with Archean model ages in the SCLM underlying the NCC, sampled by this study, suggests that the original SCLM underlying the NCC block has been largely removed. This may have occurred during the Proterozoic, the Phanerozoic, or during both periods. These results highlight the complex age structure in the current SCLM beneath northeastern China.

 

IV.  MISCELLANEOUS FIELDS

Sun et al. (2001) reported the Re-Os isotope geochemistry of Dongling CD iron meteorite determined by N-TIMS. The concentration of  Re, Os and the ratio of 187Re/188Os, 187Os/188Os are 185 ppb, 176030 ppb and 0.4950.009, 0.136340.00002 respectively. The result was compared with that of the other irons and chondrites. The Re and Os concentrations of the Dongling iron meteorite were plotted on the trends of the group A and A irons. The Pt-Os relation of the Dongling iron meteorite is similar to that of the group A irons. That suggests a higher fractionation for the Dongling iron meteorite.

Yao et al. (2002) reported the PGE and Re-Os isotope compositions and their significances of Co-rich ferromanganese nodules from the Middle and Western Pacific Ocean, which were determined with ICP-MS. The concentration of Re, Os and the ratio of 187Re/188Os, 187Os/188Os are 0.084-0.272 ppb, 0.723-3.258 ppb and 0.134, 0.757, respectively. In the diagram of 187Re/188Os-187Os/188Os, the Re-Os isotope composition is obviously different from the rocks of the continental crust, but close to the meteorite, which indicates that extra-terrestrial PGE components maybe exist in the Co-rich ferromanganese nodules.

 

V.  introduction and review on the progress of Re-Os isotope geochemistry in the world

Since early 1990s, Chinese geoscientists have published many papers to introduce and review the progress of Re-Os isotope geochemistry in the world. They are rather useful to the development of Re-Os isotope geochemistry in China.

Xiong and Zhai (1994a,b,c,d, 1995) introduced the principles of Re-Os isotope geochronology of molybdenite; the application of Re-Os isotope system in the basic-ultrabasic rocks; the application of Re-Os isotope system to the origin of ore-forming materials of magmatic ore deposits; and the principles and application of coupled Re-Os and Pt-Os isotope systems respectively. Li (1996) and Xie and  Chen (1998) introduced the application of Re-Os isotope system to the origin of metal ore deposits. Li (1997) introduced the method of determination of natural abundance of Osmium by ICP-MS. Sun et al. (1997d) introduced the method of Os-Os isochronology. Guo and Fan (1997) and Wu and Sun (1999) introduced the principles and the application of Re-Os isotope system in general. Xie (1998) introduced the geological significance of Os isotope composition in the platinum group minerals (PGM). Guo (1998) and Lan (1999) introduced the application of Os isotope to the oceanic palaeo-environment. Wang and Du (1999) introduced the method of determination of rhenium and osmium in sulfide by ICP-MS with sample digestion by reverse aqua regia. Zhi (1999) introduced the Re-Os isotope system and the dating of sub-continental lithosphere mantle (SCLM). Yang et al. (2001) introduced the application of the Re-Os isotope system to meteorites. Liu et al. (2001) introduced the techniques of microdistillation to separate, enrich and purify osmium to meet the requirement of N-TIMS and the techniques on the determination of osmium isotope by N-TIMS. Zhang et al. (2002) introduced the progress in geological sample digestion and chemical separation and purification for Re and Os isotope analyses.

Acknowledgements   We acknowledge support by the National Natural Science Foundation of China, grant No. 40173009 and the Research Fund from the Doctoral Program of High Education of China No. 1999035816 to. Zhi Xiachen.

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