Diagenetic effect of mantle-derived CO2 charge to clay minerals in the Baiyun-Liwan deepwater area of the Pearl River Mouth Basin in South China Sea
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摘要: 珠江口盆地白云-荔湾深水区油气勘探中钻遇大量高含量CO2气层，使得如何规避高CO2风险成为当前面临的挑战。通过工区充注CO2的储层砂岩黏土矿物X射线衍射（XRD）、流体包裹体显微测温和稀有气体同位素组成等分析，明确了幔源无机CO2的成因，并运用黏土矿物特征讨论高温幔源无机CO2充注的黏土矿物成岩响应：有序带倒转和大量自生高岭石的生成。依据CO2气井的XRD全定量分析数据剖面图将幔源无机CO2气层段的黏土矿物组合分为3类：Ⅰ类为I/S混层黏土矿物中S体积分数介于10%~25%之间，有序度处于R2~R3带，高岭石体积分数高；Ⅱ类为I/S混层黏土矿物中S体积分数介于10%~15%，有序度为R2~R3带，自生高岭石体积分数低；Ⅲ类为I/S混层黏土矿物中S体积分数介于50%~60%，有序度为R0带，高岭石体积分数低。总结出幔源CO2在珠江组和珠海组中存在2种运聚模式：一是幔源CO2通过与基性岩浆连通的深大断裂垂直向上运聚；二是垂直向上运移后通过连通砂体侧向长距离运聚。研究结果对珠江口盆地白云-荔湾深水区下一步油气勘探规避高含量CO2风险具有指导作用。Abstract: During petroleum exploration in the Baiyun-Liwan deep-water area of the Pearl River Mouth Basin (PRMB), South China Sea, a huge number of CO2 gas reservoirs has been met. Therefore, how to avoid the high CO2 risk has become a big challenge now. In this paper, the X-Ray diffraction (XRD) of clay minerals in the sandstone filled with CO2, microthermometry of fluid inclusions and isotopes of noble gas were used for analysis. The results show that the origin of inorganic CO2 is magmatic. The effects of mantle-derived CO2 on clay minerals are the inversion of clay mineral order degree and the formation of a largeamount of authigenic kaolinite. Moreover, the clay mineral assemblage was divided into three types based on the of XRD analysis data in CO2 wells. Finally, two patterns of CO2 migration and accumulation in the Zhujiang and Zhuhai Formations were summarized: (1) the mantle-derived CO2 migrates vertically upward through the deep faults which connected with the mafic igneous rocks, and (2) lateral long-distance migration through connecting sand bodies after vertical upward migration. These results have certain guiding significance for avoiding the risk of high CO2 in the future exploration in the deep-water area of PRMB, South China Sea.
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图 1 珠江口盆地白云-荔湾深水区构造区划图及采样井分布
Figure 1. Map of structural units division and distribution of samples in Baiyun-Liwan deepwater area, PRMB
图 2 珠江口盆地白云-荔湾深水区天然气中3He/4He-δ13CCO2-PDB关系图(底图据文献[25])
Figure 2. Plot of 3He/4He-δ13CCO2-PDB of the natural gas samples in Baiyun-Liwan deepwater area, PRMB
图 3 珠江口盆地白云-荔湾深水区天然气CO2/3He-δ13CCO2-PDB关系图(底图据文献[25])
Figure 3. Plot of CO2/3He-δ13CCO2-PDB of the natural gas samples in Baiyun-Liwan deepwater area, PRMB
图 4 珠江口盆地深水区P5井砂岩岩屑样品(穿石英颗粒裂纹中)检测到含CO2盐水包裹体及其伴生的气液两相盐水包裹体
Figure 4. Roman spectrogram of CO2 inclusions and photomicrographs of CO2 inclusions and their coeval aqueous inclusions, plane polarized light in the PRMB
图 5 珠江口盆地深水区流体包裹体均一温度频率直方图
Figure 5. Histogram of homogenization temperatures of fluid inclusions in deepwater area of the PRMB
图 6 高含CO2井区单井XRD分析黏土矿物质量分数-深度剖面图
a.P5井，2 836.2~2 912 m为含CO2层段，φ(CO2)为14.00%~16.10%；b.P6、P7、P8井，2 733~2 903.5 m为含CO2层段，φ(CO2)为8.47%~9.00%；c.P11井，3 612~3 820 m为含CO2层段，φ(CO2)为7.67%~58.50%；d.W14井，3 184.9~3 189 m、3 321.2~3 370.1 m为含CO2层段，φ(CO2)分别为59.36%~62.16%、85.75%~92.41%
Figure 6. Cross plots of clay mineral contents-depth for the single well XRD in deepwater area
图 7 白云-荔湾深水区CO2气层砂岩样品SEM照片
a.长石发生溶蚀作用；b.孔隙间充填假六方板状自生高岭石；c.孔隙间生成自生石英
Figure 7. SEM photograph of sandstone samples of CO2 gas reservoir in Baiyun-Liwan deepwater area
图 8 含CO2的岩屑长石砂岩中自生碳钠铝石矿物岩石学照片
a.W14井，3 156.4 m，正交偏光，碳钠铝石交代有孔虫体腔壁；b.W14井，3 156.4 m，正交偏光，碳钠铝石沿有孔虫体腔壁向体腔中心发育；c.W14井，3 239.1 m，扫描电镜(SEM)，粒间孔隙生长的纤维状碳钠铝石；d.P9井，2 516.72 m，正交偏光，粒间孔隙中的碳钠铝石
Figure 8. Petrological photographs of dawsonites developed in the bearing CO2 debris-arkosic sandstones
图 9 深水区砂岩粒间孔隙充填方解石、白云石和Fe-白云石胶结物的透射光、阴极光照片
a, b.P13井，3 372.6~3 372.75 m，粗砂岩，粒间孔隙充填大量发桔红色阴极光的含铁方解石胶结物；c, d.L2井，2 196.0~2 196.15 m，极细粉砂岩，充填暗棕色阴极光的铁方解石脉；e, f.L18井，3 440.59 m，细砂岩，粒间孔隙充填发桔黄色阴极光的含铁方解石胶结物和发桔黄色阴极光的粒状白云石，白云石多为菱形自形，可见环带结构；g, h.L11井，2 878 m，砂岩，粒间孔隙充填发暗棕色阴极光的粒状白云石，白云石多为菱形自形，可见环带结构
Figure 9. Transmission and cathodic photographs of intergranular pores of sandstone filled with calcite, dolomite and Fe-dolomite cement in deepwater area
图 10 白云-荔湾深水区温度-方解石胶结物δ18O关系图(底图据文献[7])
Figure 10. Scatter diagram between homogenization temperature and δ18O of aqueous inclusion in in the carbonte cements of Zhuhai and Zhujiang Formations in deepwater area
图 11 珠江口盆地白云-荔湾深水区幔源CO2运移聚集模式图
Figure 11. Geological cross sections of the deepwater area of PRMB illustrating the migration and accumulation of mantle-derived CO2 gas
表 1 珠江口盆地白云-荔湾深水区CO2及稀有气体同位素和体积分数分析结果
Table 1. Concentrations and isotopic of CO2 and rare gases in Baiyun-Liwan deepwater area, PRMB
井号 深度/m φ(CO2)/% δ13CCO2-PDB/‰ 3He/4He CO2/3He 幔源He贡献率/% L11 1 502.0 0.56 -2.4 2.17 3.36×107 26.94 L13 1 763.6 0.96 -5.7 2.22 5.41×107 27.57 L18 2 511.5 4.46 -3.2 1.14 6.48×108 14.04 W14 1 907.3 3.98 -4.1 2.18 3.72×108 27.07 W14 2 249.0 9.00 -4.2 2.18 1.18×109 27.07 W11 3 192.0 3.89 -4.6 1.21 7.42×108 14.91 P4 2 711~2 766 3.81 -3.3 1.70 3.27×108 21.05 P5 2 743~2 758 3.38 -3.2 1.76 2.45×108 21.80 P5 3 249.0 11.84 -3.8 1.30 3.08×109 16.04 P11 2 111.0 97.92 -4.8 5.90 1.88×109 73.65 P11 2 111.0 98.27 -6.5 6.59 7.10×109 82.31 P14 3 189.4 60.11 -5.0 6.92 3.57×108 86.42 P14 3 321.2 85.75 -3.9 6.51 2.46×108 81.30 L11 3 370.1 90.09 -1.2 6.86 6.70×108 85.76 注：取国际公认值空气标准：Ra=(1.40±0.03)×10-6；w(4He)=5.24×10-6；幔源He贡献率(%)=(R测-R壳)/(R幔-R壳)，式中，R壳为壳源中3He/4He(R壳=0.02Ra)；R测为测试样品中3He/4He值(R测=(8±1)Ra)，Ra为大气中3He/4He值 
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表 2 白云-荔湾深水区流体包裹体均一温度及现今地层温度
Table 2. Homogenization temperature of fluid inclusions and current formation temperature in Baiyun-Liwan deepwater area
井号 深度/m 层位 CO2包裹体
均一温度
ThCO2/℃伴生盐水
包裹体均一
温度Th/℃现今地
层温度
T/℃L1 2 169~2 172 N1z 29.3 136.1 100.0 L11 2 883 N1z 27.7 112.9 103.6 L13 2 722 N1z 33.8 140.4 107.4 L18 3 791 E3z 32.5 170.3 162.4 L18 3 804.98 E3z 27.9 189.9 163.1 W14 3 385 E3z 31.4 194.7 165.8 W14 3 397 E3z 29.7 197.8 166.4 W11 3 270 E3z 29.3 210.4 192.3 P4 3 005 N1z 29.3 160.8 121.1 P5 2 838 N1z 30.7 130.3 104.9 P5 2 859 N1z 29.4 130.5 105.7 P11 3 367 N1z 29.5 167.2 134.4 P14 3 776.5 N1z 32.5 174.2 149.5 P14 3 765 N1z 29.8 187.0 149.1 P14 3 765 N1z 28.8 176.7 149.1 注：N1z.珠海组；E3z.珠江组
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表 3 珠江口盆地白云-荔湾深水区自生高岭石含量、黏土矿物有序带及CO2稳定同位素统计表
Table 3. Data of authigenic kaolinite contents, S% and the orders in I/S mixed clay minerals, and natural gas components contents and stable carbon isotopic ratios of CO2
井号 深度/m 层位 岩性 高岭石
wB/%I/S中S
wB/%有序带 黏土矿物
组合类型CH4 CO2 N2 δ13C1-PDB/
‰δ13C2-PDB/
‰δ13C3-PDB/
‰δ13CnC4-PDB/
‰δ13CnC5-PDB/
‰δ13CCO2-PDB/
‰φB/% L4 2 725~2 748 N1z2 砂岩 76.80 10 R3 Ⅰ 88.660 3.570 0.33 -36.70 -26.85 -25.61 -25.01 -7.89 L16 2 372~2 374.5 N1z2 砂岩 23.70 25 R2 Ⅰ 89.44 2.52 0.98 -38.20 -28.40 -27.30 -27.00 -25.40 -8.40 L16 2 471~2 513.5 N1z2 砂岩 42.40 25 R2 Ⅰ 90.33 3.29 0.84 -37.10 -29.20 -26.40 -26.00 -24.90 -9.50 L20 2 976.5~2 990.28 N1z2 砂岩 43.30 25 R2 Ⅰ 87.50 3.98 0.48 -39.10 -29.10 -28.30 -27.60 -25.90 -9.10 L20 3 006.8~3 008.2 N1z2 砂岩 53.70 25 R2 Ⅰ 88.48 3.42 0.16 -39.00 -28.40 -27.70 -27.20 -26.00 -8.20 W14 3 184.9~3 189.4 N1z 砂岩 37.00 10 R3 Ⅰ 35.04 62.16 1.73 -51.10 -34.00 -30.10 -28.40 -4.80 W14 3 321.0~3 321.2 N1z 砂岩 34.00 10 R3 Ⅰ 12.29 87.61 0.00 -53.20 -34.90 -30.20 -27.70 -2.90 W14 3 354.3~3 370.1 E3z 砂岩 64.00 10 R3 Ⅰ 5.74 91.77 2.27 -52.90 -35.10 -30.40 -28.60 -3.20 P5 2 904~2 912 泥质细砂岩 77.00 10 R3 Ⅰ 5.29 2.69 91.70 -34.40 -28.50 -29.90 -7.20 P7 1 727~1 728.7 N1z1 中粗砂岩 67.50 25 R2 Ⅰ 87.70 1.57 4.33 -35.80 -25.40 -26.40 -8.40 P7 2 903~2 903.5 细砂岩 78.50 15 R2 Ⅰ 85.20 3.79 3.44 -36.70 -29.70 -28.90 -5.10 P6 1 907.3~1 917.0 粉-细砂岩 48.00 20 R2 Ⅰ 89.91 4.41 0 -38.10 -29.20 -27.90 -27.60 -27.40 -6.30 P6 2 249 N1h 粉-细砂岩 53.00 25 R2 Ⅰ 85.60 8.47 0 -36.80 -29.30 -28.20 -27.50 -27.60 -6.20 P9 2 711~2 726 N1z2 砂岩 52.70 15 R2 Ⅰ 88.58 4.10 0.57 -35.50 -28.80 -27.20 -26.70 -26.50 -4.50 P9 2 743~2 758 N1z2 砂岩 76.88 15 R2 Ⅰ 89.13 3.94 0.46 -36.90 -28.80 -27.70 -27.50 -27.30 -5.40 P13 3 281 N1z2 灰质细砂岩 24.00 20 R2 Ⅰ 84.37 7.41 0.50 -37.66 -28.96 -26.85 -26.16 0 -3.25 P13 3 313.5 N1z2 粉砂岩 38.00 20 R2 Ⅰ 88.03 4.63 0.07 -37.61 -29.10 -27.44 -26.64 0 -5.12 P13 3 329 N1z2 细砂岩 30.00 20 R2 Ⅰ 90.28 3.45 4.24 -37.24 -29.15 -27.09 -26.33 0 -4.82 P16 3 230~3 238.5 N1z2 细砂岩 73.75 15 R2 Ⅰ 78.09 14.56 0.11 -36.38 -28.07 -26.26 -26.65 -25.59 -4.22 P20 4 055.6~4 056.3 N1z2 粉砂岩 10.00 15 R2 Ⅰ 75.78 18.50 0.09 -35.60 -28.50 -26.90 -25.80 0 -2.50 P11 3 612~3 632.8 N1z2 细砂岩 0.00 15 R2 Ⅱ 80.00 13.80 0.43 -34.60 -27.70 -27.00 0 0 -2.50 P11 3 650~3 660 N1z2 细砂岩 1.00 15 R2 Ⅱ 78.80 13.80 0.61 -36.80 -28.60 -27.40 0 0 -4.70 P15 3 242~3 249 N1z 细砂岩 3.00 15 R2 Ⅱ 82.19 11.91 0.03 -35.90 -29.10 -27.80 -27.10 -26.60 -5.00 W10 2 111.5~2 116.5 E3z 砂岩 3.00 50~60 R0 Ⅲ 2.16 93.95 3.89 -35.71 -26.87 -23.77 0 0 -6.47 注：N1h为韩江组
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表 4 W14井岩屑长石砂岩XRD分析结果[26]
Table 4. XRD measurement of debris-arkosic sandstones in Well W14
深度/m 层位 矿物wB/% 石英 钾长石 方解石 白云石 菱铁矿 黄铁矿 碳钠铝石 3 109~3 112 珠江组 29.0 1.4 1.4 27.8 5.7 - - 3 277~3 280 珠江组 41.2 1.9 - 5.3 0.9 3.0 0.3 3 331~3 334 珠江组 63.7 4.2 - 3.1 3.3 1.0 - 3 379~3 382 珠海组 73.9 1.9 - 1.2 3.7 1.5 - 3 475~3 478 珠海组 67.4 - - 0.8 3.1 0.9 0.8 3 646~3 649 恩平组 41.5 - 1.0 3.3 3.2 2.9 - 3 916~3 919 文昌组 44.6 2.7 13.9 3.8 - 0.4 - 注：“-”代表含量微少；样品测试在吉林大学测试科学实验中心完成
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