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VOI.

42

NO.

SCIENCE IN CHINA (Series D)

December 1999

Organic carbon isotopes of the Sinian and Early Cambrian black shales on Yangtze Platform, China *
LI Renwei

(%iiE#)',

LU Jialan

(p%$!)2,
2. Guangzhou Institute of Geochemistry,

ZHANG Shukun

(% ?&!* LEI Jiajin (S$U ))' ) 3 and @


, China;

(1 . Institute of Geology, Chinese Academy of Sciences, Beijing 100029

Chinese Academy of Sciences, Guangzhou 510640, China; 3. Institute of Geomechanics, Chinese Academy of Geological Sciences, Beijing 100081, China) Received July 9 , 1998; revised February 19, 1999 Abstract Organic matter of the Sinian and early Cambrian black shales on the Yangtze Platform belongs to the light carhon group of isotopes with the 6 I3cvalues from - 27% to - 35 % , which are lower than those of the contempomneously deposited carbonates and phosphorites. A carbon isotope-stratified paleooceanographic model caused by upwelling is proposed, which can be used not only to interpret the characteristics of organic carbon isotopic compositions of the black shales, but also to interpret the paleogeographic difference in the organic carbon isotope compositions of various types of sedimentary rocks. Keywords : black shales, stable carbon isotopes, paleooceanography , the Sinian, the E r y Cambrian. al

The Sinian and Early Cambrian black shales are extensively distributed on Yangtze Platform. As an important reservoir of carbon owing to the huge quantity of organic matter, they have an influence on the global biochemical cycle and the evolution of the biospherer']. Many major phosphorites, Mn and Ba ore deposits that occur in the Sinian and Early Cambrian strata in China are intimately related . to the black shales in originL2] In addition, the abundant noble and rare metals in the Early Cambrian black shales, such as V , Mo , Ni , Co , Cr , Se , U and AU[~-'] , have important economic valuesL6]. Geologists have already studied the black shales, but still lack sufficient knowledge about their stable isotope geochemistry. This paper reports on the organic carbon isotope compositions and reconstructs the paleooceanographic conditions for the formation of the black shales.

1 Geological setting
The black shales dealt with in this paper include those from the Early Sinian Datangpo, the Late Sinian Doushantuo and Dengying, and the Early Cambrian, which are distributed in such areas as Minle, Yuanling, Taojian-Yiyang and Dongkou counties in Hunan Province, Zunyi and Qingzhen counties in Guizhou Province, and Xiushan County in Sichuan Province (fig. 1) The Early Sinian black shales outcrop mainly in Hunan , Guizhou and Sichuan provinces. However, the thickness var-

* Project supported by the National Natural Science Foundation of China (Grant No. 49472114) and the Open Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences. 1) Wu Chaodong, Upper Sinian-Lower Cambrian black shale series and the related ore mineralization, Ph. D. Dissert&wn, 1997, Institute of Geology, Chinese Academy of Sciences.

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ies from greater than 20 m in Minle to only a few meters in Xiushan. Many important Mn carbonate ores, e . g. the Minle and Xiangtan ores in Hunan Province, the Datangpo ore in Guizhou Province and the Xiushan ore in Sichuan Province, occur in the Early Sinian black shale series. The heavy sulfur iso) tope ( 3 4 ~ abounds in pyrite from the Mn carbonate ~ ores and black shales, with 8 3 4 value high , up to + 60% . Possibly, they formed in isolated, closed basins far from the open ocean on a geological setting of the late Proterozoic supercontinent[7981 There are Fig. 1. Studied area in this paper. 1 , Xiushan; 2 , two sets of black shales in the sinian Doushantuo Yuanling; 3 , Yiyang-Taojian ; 4 , Dongkou ; 5 , Minle; 6 , Formation. The thickness of the early Doushantuo Qingzhen ; 7 , Zunyi . black shales are less than one meter in the Xiushan area, and a few meters in Yuanling area ( e . g. at Sanjiaoping Village). The late Doushantuo black shales are relatively thick, even greater than 10 m in the Zunyi area ( e .g the Son& Village) and Yuanling area ( e . g. the Sanjiaoping Village) The Doushantuo is a major P-accumulated timeCg1, and many phosphorites are closely related to the Doushantuo black shales in origin. In the Yuanling area, a few meters of phosphorites are continuously superimposed on the early Doushantuo black shales. Phosphorites of low grade are intercalated in the late Doushantuo black shales in the Zunyi area. The black siliceous rocks intercalating black shales were deposited later during the Dengying stage of the Late Sinian. Some Chinese geologists call it Liuchapo Formation. Owing to enrichment of organic matter, the siliceous rocks are considered for the study of stable carbon isotopes in this paper, as well. The Early Cambrian black shales are extensively distributed in southeastern China including the Yangtze Platform, with an area of at least 500 000 km2. Its thickness is over one hundred meters in the Qingzhen, Taojing and Dongkou areas. The early Cambrian is another P-accumulated time in the geological history of chinaLg1 and the deposited phosphorites are closely related to the contempo, raneous black shales in origin of as well. The Late Sinian and Early Cambrian black shales were mainly deposited in outer shelf-slope basin . So far, we lack precise date on the geological age of the Sinian and Early Cambrian black shales. The Rb-Sr isochron age of the Mn carbonates ores taken from Minle area is (728 28) ~ a ' " ] , which would approach the age of the Early Sinian black shales. The Sm-Nd isochron age of the phosphorites taken from the upper part of Doushantuo Formation is (645.5 23.6) ~ a [ " ], which would approach the age of the black shales of the late Doushantuo.

2 Analytical methods and results


Inorganic minerals, such as carbonates and silicates, were removed from rocks using HCVHF by heating before the organic carbon isotopes of the rocks were analyzed. Due to the very low soluble organic matter that can be identified from the Rock-Eval pyrolytic measurements: the So and S1 values
are near zero[51and the high contents of organic carbon of the black shales (table I ) , the organic matter obtained from the above method is similar to kerogen of the rocks in composition. The stable

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isotope analyses of organic carbon were completed by the Laboratory Center of Institute of Petroleum Exploration and Development, Beijing , using PDB standard.
Table 1 Data on stable carbon isotopic and organic geochemical analyses of the Sinian and Early Cambrian sedimentary rocks Area Strata Sample
Lithology

TOC
(wt%)

H/C (atomic)

6 "c,, (460)

6 '3C,d.

(460)

Gdn
%d Yuanling
-I

%1

%d

YiyangTaojian Dongkou Qingzhen


Zunyi

-t

-I
-,
*I

%dn

%dn
%d
Minle
2 1

~84 BSH ~55 P-BSH ~52 BSH ~ 4 7 ~ ~ 4 0 L ~31 BSH ~73 D B50 BSH B49 BSH x47 BSH B41 SR B39 SR B34 BSH B23 P B9 BSH 87 M D B3 D Y6 BSH T37 P-BSH D9 BSH Dl BSH 4567 BSH TB47 BSH TB45 BSH TB42 P- BSH TB39 D SD22 D SD20 D SDll BSH SD4 P-BSH M45 D M36 BSH M26 M n M22 M n M15 Mn-BSH MI0 MD M 6 SL M 5 D

6.28 11 -58 10.96 0.03-0.20 2.66 0.66 9.86 10.16 10.47 1.13 1.21 7.25 0.98 2.30 1.14 0.06 10.00 21.40 9.65 5.80 1.74 4.75 5 -08 14.83 0.31 3.35 3.25 0.05 2.4 2.20 2.85 2.58 0.74 1.18 0.12

- 31.4
0.29

- 31.2
- 34.4
-8.e-8.5 -34.1

0.30

- 33.2
0.31 33.3 -33.7 32.7 - 30.8 -33.7 - 24.2 35.0 32.5

-5.2

28.9

0.33 0.38

-4.8 0.19 0.15 0.17 0.13 0.36 0.32 0.33

27.7

- 32.9 - 31.9
-27.1

- 28.2 - 32.9
-33.3 - 34.4

- 31.9
+ 1.5
-27.7

+ 2.0 + 0.7
-3.9

29.7

- 30.5
0.41

- 31.9
29.3 -33.2 - 34.4 34.7 - 34.9 - 30.0 - 32.0

-5.2

26.8

Stable carbon isotope analyses of carbonate rocks of the Sinian and Early Cambrian age on Yangtze Platform were needed for comparison with the organic carbon isotopes of the black shale. Samples reacted with anhydrous H3PO4 at 250C for 24 h for limestone, and for 72 h for dolostone. The results are represented by PDB standard. Elemental analysis of the isolated organic matter of the black shale samples was made in the Open Laboratory of the Guangzhou Institute of Geochemistry, Chinese Academy of Sciences. The data

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used to check the primary memory of the organic carbon isotope compositions will be discussed later. The data on the stable carbon isotopes of the black shales and some carbonate rocks of the Sinian and Early Cambrian on Yangtze Platform are listed in table 1 . The distribution of the samples in stratigraphic profile is shown in fig. 2 . 6 values of organic carbon ( 6 l3 c,,. ) of the Early Sinian black shales and the Mn carbonate ores related to the black shales (M15-M36 in table 1 ) in Minle
Yuanling Xiushan Zunyi

I.. ..I

I_._[4

SDl 1 SD4

Fig. 2 . Profiles of the late Sinian and Early Cambrian strata on Yangtze Platform. Lithology: 1 , Limestones; 2 , dolostones; 3 , siltstones; 4 , silty shales; 5 , siliceous rocks; 6 , black shales; 7 , phospboms nodulebearing black shales ; 8 , phosphorite beds. Strata: 43, , the Lower Cambrian; dn, Dengying Formation ; 1 , 1,iuchapo Formation ; d , Doushantuo Formation.

area are similar, with a range from - 33 -280 to - 34.9% The 6 l3cO,. value of the early Sinian organic-rich rock (M6) in age is - 32.0%0. The Late Sinian Doushantuo black shales (Y31, B9, B34, SD11 and SD4 in table 1 ) have 6 ' 3 ~ 0 r g . values with a range from - 30.5% to - 35.0% , and the organic-rich siliceous rocks of the Late Sinian Liuchapo (B1 and B39 in table 1 ) have 6 13c,,,. values with a range from - 30.8%0 to - 32.7%. Tang has obtained similar data on organic carbon isotopes of the contemporaneous siliceous rocks, with a range of 6 l3 COT.values from - 29.3% to
- 35.3%')

. The

l3

C,,.

values of the Early Cambrian black shales are from

- 27.

l%o to

- 34.4%0. Compared to black shales the carbonate rocks and phosphorites are clearly enriched with
heavy carbon ( l 3 c ) . For example, the Dengying dolostone from Zunyi area (SD22) and the Early Cambrian limestone from Xiushan area have 6 l3cOrg. values - 27.7960 and - 26.2%, respectively. The 6 ' 3 ~ , , , , value of the Doushantuo phosphorites from Yuanling area is - 24.2%0.
1 ) Tang Shimng, Sedimentology and sedimentary geochemistry of the Cambrian and Sinian siliceous rocks in Hunan and Sichuan

provinces, Ph . D . Dissertation , 1995 , Institute of Geology, Chinese Academy of Sciences.

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3 Discussion
3.1 Checking the preservation of stable carbon isotopic memory Before discussing its characteristics and significance, we should check the perservation of primary memory of the stable carbon isotope compositions of the Sinian and Early Cambrian black shales on Yangtze Platform. Did the black shales really record the primary information on the stable organic carbon isotope compositions? There have been several criteria that can be used for judging the diagenetic alteration of stable carbon isotope compositions of carbonate rocks, for example, the petrographic , characteristics, the compositions of trace elements (especially the Sr/Mn rati~)['~-'~' and the oxygen isotope compositions['s1. The primary memory of the stable carbon isotope compositions of carbonates listed in table 1 has been checked by the above criteria. The diagenetic alteration of organic carbon isotope compositions of sedimentary rocks can be determined by the H/C atomic ratios of kerogenC169171 change of 6 13cvalues of kerogen could not exceed 5% for those rocks that have H/ . The C atomic ratios greater than 0 . 2 . Therefore, the 6 l3 C values of the black shales from Xiushan , Yuanling, and Zunyi-Qingzhen area should be close to the primary organic carbon isotope compositions as their W C atomic ratios of organic matter are all greater than 0 . 2 (table 1) . H/C atomic ratios of organic matter for the black shales in Yiyang-Taojian and Dongkou area are a little less than 0.2. Therefore, the primary 6 13cvalues of organic carbon in sedimentation should be more negative than those in table 1 . The differences of 6 values between carbonate carbon and organic carbon, defined as A , in such rocks as SD22 and Y87, or in the rocks (including black shales) that are adjacent in strata and have experienced similar depositionary and diagenetic history, e . g. M5 and M6, M36 and M45 , B3 and B7, Y3 1 and Y73 , are relatively consistent, from 27 to 30. They are close to the average of late Proterozoic sedimentary rocks, additionally indicating that the data on the stable carbon isotope compositions in table 1 preserve the primary information. 3 . 2 Characteristics of the organic carbon isotope compositions of the Sinian and Early Cambrian black shales Based on a systematic study of stable carbon isotope compositions, two groups of amorphous kerogens from Phanerozoic sedimentary rocks are divided by Lewan (1986). They are the l-amorphous kerogens that are light carbon ("(2)-rich in stable carbon isotopes and the h-amorphous kerogens that are heavy carbon (13c)-rich in stable carbon isotopesr181. 6 13cvalues of the former are within a range of - 35% to - 26%, and 6 13cvalues of the later are within a range of - 24% to - 20%0. The organic matter, similar to kerogen, in all black shales of the Sinian and Early Cambrian ages on the Yangtze Platform, have lower 6 13cvalues in the stable carbon isotope compositions, under - 26%, belonging to the 1-amorphous kerogen group according to the division by Lewan ( 1986) In the data reported by Lewan (1986), only a small amount of kerogens have 6 values lower than - 30%. However, a majority of the Sinian and Early Cambrian black shales have 6 values lower than - 30% (table 1 ) , therefore they are more 12c-rich in stable carbon isotope compositions even in the 1-amorphous kerogen group. Though the 6 1 3 ~ , , g , values of the carbonate rocks, e . g. SD22 and Y87 in table 1 are quite negative, they are greater than those of the contemporaneous black shales. Organic carbon of the Late Sinian phosphorite (B23) has 6 13C value of 24.2%, which is markedly greater than those values of the underlying and overlying black shales. This difference in carbon iso-

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tope compositions signals a sedimentary environmental change of paleoocean in the phosphorites deposition. 3 . 3 Paleooceanographic depositionary environments and origin of the Sinian and Early Cambrian black shales So far, the origin of the Sinian and Early Cambrian black shales has been a question without a satisfactory answer. It is discussed here through the data of stable carbon isotopes. Sinian and Early Cambrian sedimentary organic matter was derived from the photosynthetic aquatic phytoplankton. The carbon isotope compositions were determined both by the forms and compositions of the available carbon dioxide in the ocean and by the mechanism of photosynthesis[1~18~-201. discussing the causes In for the anomalous carbon isotope compositions of the 1-amorphous kerogen and the organic matter of Jurassic Toarcian black shales, several suggestions have been proposed, such as ( i) special plankton species, (ii) a change in atmospheric C 0 2 , (iii) bacterial reworking of organic matter, and (iv) special paleooceanographic environments. However, only the fourth suggestion could provide a reasonable explanation[18320-221 . Generally, the 6 13C values of dissolved inorganic carbon in oceans equilibrated with atmospheric C02 are close to 0-1%. In anaerobic basins, such as the Jurassic studied by KUSpert (1982), organic matter is degraded by sulphate-reducing bacteria, and the oxidized organic carbon is much more enriched in 12cthan normal oceanic inorganic carbon and has the 6 13cvalue of ca . - 25560. Due to restriction of sea water, light carbon accumulates in the deeper water. Once it escapes to the photic zone by convection and diffusion and is in turn taken up by planktons, the produced organic matter is 12c-rich in stable carbon isotopesLm1 In the restricted epicontinental basins of . shallow water with depth less than 200 m , C02 produced by the microbial degradation of organic matter can be the source for phytoplanktons. Applying this oceanographic model, Lewan (1986) has explained the origin of the I-amorphous organic matter[lE1 The occurrence of the Late Sinian and Early . Cambrian black shales on Yangtze Platform is closely related with siliceous rocks and phosphorites in the spatial and temporal distributions[91. Furthermore, Ba is enriched in the black shales and barite ores occur in the black shale strata1) . According to the characteristic sedimentary association of C-SiP and c - s ~ - B ~ [ ~ ~ ]reasonable to suggest that the Late Sinian and Early Cambrian black shales , it is " ) formed in an upwelling setting of high organic productivity. The ocean could become stratified in the stable carbon isotopes during long lasting periods in such an upwelling setting (fig. 3). In the oxygen minimum zone (OMZ) , as shown in fig. 3, the C02 derived from the bacterial degradation of large amounts of organic matter (CH20) under reducing conditions, having a low 6 13cvalue to

- 25%o,

was a 12C-rich inorganic carbon reservoir, compared with that of the surficial ocean. Applying this oceanographic model to the Yangtze Platform, the characteristics of stable carbon isotope compositions for the Late Sinian and Early Cambrian sedimentary rocks, including the black shales, can be understood. Generally, the photosynthesis in oceans occurs above a depth of ca. 200 m. In the platform setting where carbonates deposited, such as A shown in fig. 3 , photosynthesis of surficial ocean could not be influenced by the oxygen minimum zone (OMZ) However, in the outer shelf and the slope

1 ) Wang Zhongcheng, Sedimentation of Early Cambrian stratiform barite and witherite in South China bioorganism and palmmarine environment, Ph . D . Dissertation , 1997, Institute of Geology, Chinese Academy of Sciences.

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near it ( B , C , D in fig. 3) , photosynthesis occurred not only directly in the upper OMZ , but also in the surficial ocean influenced by the OMZ, where the inorganic carbon reservoir had markedly less 6 13cvalue than that in the platform due to the upward convection and diffusion of the 12c-rich C% from the OMZ . As shown in table 1, the Sinian and Early Cambrian sedimentary rocks have similar A values ( = 6 l3cCmb. 6 13Co,. ) . We suggest that the carbon isotope fractionation in photosynthesis in the ocean was not changed greatly. Then, the synthesized organic matter in the outer shelf and adjacent slope would have markedly negative 6 13C values, compared with those in the platform setting. This sedimentary record has been kept in the Late Sinian and Early Cambrian rocks. For example, the 6 13c,,. value of SD22 in the Zunyi area is ca. - 28%, but the 6 13c,,. values of the black shales in Xiushan, Yuanling and Taojian area located in the outer shelf and adjacent slope are as low as - 34%.
Sea level

I \ Upwelling
Fig. 3 .
Paleooceanographic environments for the formation of the Late Sinian and Early Cambrian black shales.

The change of the stable carbon isotope compositions of carbonates deposited on Yangtze Platform during the Late Sinian and Early Cambrian supports the paleooceanographic model shown in fig. 3. The 6 l3cCarb. of Y47-Y40 deposited in the outer shelf are around - 8% (table 1 ) . But in values the platform setting, where the surficial ocean was not influenced by the OMZ and had high organic productivity due to the rich nutrients carried by upwelling, the 6 13C values of the inorganic carbon reservoir of the surficial ocean increased as the light carbon (12c) was selectively taken up from sea water by the flourishing phytoplankton through photosynthesis. This sedimentary record has indeed been kept in the Late Sinian carbonate rocks. For example, the 6 13~,,,a value of SD22 from Zunyi area is + 2.0% (table 1) , and it ranges from + 4% to + 7% in the Yangtze Gorge area'"] . We have no evidence to use the upwelling model described above for explaining the origin of the Early Sinian and even the Late Sinian Doushantuo black shales. However, the mechanism proposed The Early Sinian black by Kuspert (1982) and Lewan et al. (1986) is worthy to be shales and related Mn carbonate ores formed in isolated, closed basins far from open ocean. Organic matter was degraded by sulphate reducing bacteria under anaerobic conditions leading to the formation of black shales. Although the formation of Mn carbonate ores was not under the same anaerobic condi-

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tion, it depended upon the degradation of organic matter by Mn reducing bacteria: CHzO + Mn O2 = Mn2+ + C02 + H ~ o [ ~ The 12c-rich C02 derived in these two cases could be the carbon sources for ]. photosynthesis of organic matter, and then light carbon isotope was enriched in the organic matter of the Early Sinian black shales and related Mn carbonate ores.

4 Conclusion
This paper studies the organic carbon isotopes of the Sinian and Early Cambrian black shales on values of the Yangtze Platform. The organic carbon of these rocks is rich in light carbon (12c) . 6 13c Early Sinian black shales and related Mn carbonate ores are from - 33%0 to - 35%0, the Late Sinian Doushantuo black shales from - 31% to - 35%0, the Late Sinian Dengying black siliceous rocks from 31% to - 33%o, and the Early Cambrian black shales h m - 27% to - 34%. Possibly, the Late Sinian and Early Cambrian black shales on Yangtze Platform formed in an upwelling setting of high organic productivity, and the paleoocean was stratified in the stable carbon isotopes. The light carbon isotope was markedly enriched in the inorganic carbon reservoir of the oxygen minimum zone, and the difference of organic carbon isotope compositions in the rocks deposited in various sedimentary environments could be interpreted as the extent of influence of the oxygen minimum zone upon the photic zone. Compared with the carbonate rocks deposited in platform setting, the black shales formed in the outer shelf and adjacent slope basins had markedly lower 6 13c,,. values. The difference of stable carbon isotope compositions in carbonates deposited in various sedimentary environments supports this conclusion. The 6 l3cCarb. values of carbonates deposited in outer shelf basin are negative. However, they are positive for the carbonates deposited in the platform setting. The Early Sinian black shales and related Mn carbonate ores formed in the restricted basins where the carbon isotopes were stratified, as well.

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