Pore water geochemistry of shallow surface sediments in the southern South China Sea and its implications for methane seepage activities
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摘要:
海底沉积物孔隙水地球化学特征能快速响应甲烷渗漏活动及其生物地球化学过程，从而记录甲烷渗漏活动特征。对采自南海南部北康盆地的3个重力沉积柱状沉积物孔隙水样品（BH-H75、BH-H13Y和BH-H61）进行了甲烷浓度、溶解无机碳（DIC）和碳同位素（δ13CDIC）、阴离子（SO42−、Cl−）以及主微量元素（Ca2+、Mg2+、Sr2+、Ba2+）等地球化学分析。（△DIC+△Ca2++△Mg2+）/△SO42−比率图解与δ13CDIC深度剖面特征揭示了有机质硫酸盐还原反应（OSR）和硫酸盐驱动-甲烷厌氧氧化反应（SD-AOM）在不同沉积柱中所占比例的不同，其中BH-H13Y沉积柱中OSR和SD-AOM共同存在；BH-H75沉积柱中OSR占主导；在BH-H61沉积柱中SD-AOM占主导，且其底部可能存在微生物产甲烷作用。硫酸盐浓度线性拟合关系指示BH-H13Y的硫酸盐-甲烷过渡带（SMTZ）的深度约为700 cmbsf。结合SO42−浓度、DIC浓度最大值和δ13CDIC最小值推测BH-H61的SMTZ深度约为480 cmbsf。BH-H61和BH-H13Y沉积柱中，较浅的SMTZ深度、上升的DIC浓度以及强烈负偏的δ13CDIC值指示研究区存在甲烷渗漏活动。此外，在BH-H61和BH-H13Y站位，硫酸盐浓度随深度降低的变化梯度在沉积柱下部较上部陡，指示向上迁移的甲烷通量在时间上逐渐增强。孔隙水中Ca2+、Mg2+、Sr2+浓度以及Mg/Ca、Sr/Ca比值变化特征指示研究区沉积物中可能有自生高镁方解石矿物生成；而BH-H61站位SMTZ界面以下，孔隙水中Ba2+浓度升高，指示了硫酸钡的溶解作用。
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关键词:
- 孔隙水 /
- 硫酸盐驱动甲烷厌氧氧化(SD-AOM) /
- 硫酸盐-甲烷过渡带 (SMTZ) /
- 甲烷渗漏 /
- 北康盆地
Abstract:The geochemical characteristics of pore water in seabed sediments may quickly respond to the changes in the methane seepage and related biogeochemical processes. In this paper, methane, DIC and its carbon isotope value (δ13CDIC), anions (SO42−, Cl−), major and trace elements (Ca2+, Mg2+, Sr2+, Ba2+) are analyzed for the pore water samples (BH-H75, BH-H13Y and BH-H61) collected from the Beikang Basin in the southern SCS. The (△DIC+△Ca2++△Mg2+)/△SO42− ratios and δ13CDIC show that organoclastic sulfate reduction (OSR) and sulfate-driven anaerobic oxidation of methane (SD-AOM) vary from different columns. For the column of BH-H13Y, OSR and SD-AOM occur together. However, OSR is dominant in column BH-H75, while SD-AOM dominates the BH-H61 column. There may be microbial methanogenesis at the deeper layer in the BH-H61 column. Based on the linear fitting sulfate concentrations, the sulfate-methane transition zone (SMTZ) of BH-H13Y is estimated to be about 700 cmbsf. According to SO42− concentrations, the maximum DIC concentration and the minimum δ13CDIC value, the SMTZ depth of BH-H61 is estimated at about 480 cmbsf. Sallower SMTZ depths, increasing DIC concentrations and highly negative δ13CDIC values recorded in BH-H61 and BH-H13Y columns suggest a remarkable methane seepage in the study aera. The gradients for sulfate concentrations of lower part of BH-H61 and BH-H13Y columns are steeper than that of the upper part, indicating that the methane flux upward migration increases with time. Features of Ca2+, Mg2+ and Sr2+ concentrations and Mg/Ca and Sr/Ca ratios in pore water indicate the possibility of the formation of high-Mg calcite. Below the SMTZ interface at BH-H61 column, Ba2+ concentrations increase with depth, indicating the barium sulfate dissolution occurs.
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图 3 研究区BH-H75、BH-H13Y和BH-H61沉积物孔隙水中部分碱土金属元素浓度（Ca2+、Mg2+、Sr2+、Ba2+）、Sr/Ca与Mg/Ca比值深度剖面图
Figure 3.
表 1 南海南部北康盆地海域采集的3个沉积柱信息
Table 1. Information of three sedimentary columns collected from the Beikang Basin in the southern SCS
站位 北纬 东经 水深/m 岩心长度/cm 海底温度/℃ 校准地温梯度/(K/km) BH-H75 6.8482° 112.8052° 1 663 397 2.826 88.9 BH-H13Y 6.7107° 111.4839° 1 867 400 2.61 87.2 BH-H61 6.4809° 111.7519° 1 938 518 2.585 36.1 
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表 2 BH-H75、BH-H13Y和BH-H61站位沉积物孔隙水中甲烷浓度、阴离子（SO42−、Cl−）、主微量元素（Na+、K+、Ca2+、Mg2+、Sr2+、Ba2+）、DIC和δ13CDIC、Sr/Ca与Mg/Ca比值特征
Table 2. Features of methane concentration, anions （SO42−、Cl−）, major trace elements （Na+、K+、Ca2+、Mg2+、Sr2+、Ba2+）, DIC and δ13CDIC, Sr/Ca and Mg/Ca ratios of sediment pore water in BH-H75, BH-H13Y and BH-H61 sites
站位 取样深度/
cmbsfCH4/
mMSO42−/
mMCl−/
mMNa+/
mMK+/
mMMg2+/
mMCa2+/
mMSr2+/
μMBa2+/
μMDIC/
mMδ13CDIC/
‰Mg/Ca Sr/Ca BH-H75 20 0.176 26.99 540.4 443.3 12.42 48.54 9.09 110.02 0.763 2.347 −7.23 3.238 0.0265 40 0.200 26.80 531.5 442.75 12.47 48.41 9.17 112.07 0.517 2.217 −6.26 3.202 0.0267 60 0.179 25.87 529.6 444.57 12.69 48.49 9.28 107.03 0.527 2.282 −6.65 3.167 0.0252 80 0.161 25.94 534.5 444.81 12.85 48.38 9.24 109.98 0.476 2.455 −7.96 3.174 0.0260 100 0.172 26.22 541.9 445.53 12.89 48.36 8.89 108.24 0.473 2.593 −6.73 3.299 0.0266 120 0.162 25.19 536.1 442.19 11.69 48.08 9.03 140.37 0.604 3.449 −10.64 3.228 0.0340 140 0.170 24.81 532.3 443.87 12.17 48.13 9.18 111.29 0.467 3.309 −9.44 3.181 0.0265 160 0.248 24.78 541.5 444.44 12.3 48.24 9.01 107.27 0.453 3.657 −10.32 3.248 0.0260 180 0.182 25.10 554.8 441.66 12.04 47.81 9.05 105.17 0.477 3.780 −10.52 3.203 0.0254 200 0.204 24.21 541.9 446.06 12.28 48.3 9.16 107.66 0.462 4.059 −10.90 3.199 0.0257 220 0.203 23.83 543.1 442.09 12.01 47.74 8.71 105.59 0.554 4.267 −10.58 3.325 0.0265 240 0.194 23.06 533.2 443.16 12.18 47.6 9.24 104.66 0.522 4.072 −10.75 3.125 0.0248 260 0.251 22.75 536.6 443.3 12.06 47.59 8.53 105.72 0.519 4.355 −11.65 3.383 0.0271 280 0.200 22.01 531.7 436.13 12.07 46.52 8.57 102.99 0.634 4.786 −10.85 3.292 0.0263 300 0.231 21.81 539.2 441.42 12.04 46.9 8.42 105.08 0.572 5.251 −12.30 3.379 0.0273 320 0.241 21.09 541.7 437.66 11.85 46.2 7.98 102.24 0.559 5.678 −12.77 3.510 0.0280 340 0.230 20.21 539.2 446.32 12.19 46.86 8.11 102.58 0.591 5.856 −12.63 3.502 0.0276 360 0.259 19.18 537.5 443.86 12.08 46.49 9.69 102.43 0.592 6.364 −13.60 2.911 0.0231 380 0.227 18.50 540.9 448.83 12.29 46.61 7.9 101.95 0.631 7.210 −13.78 3.578 0.0282 400 0.255 17.49 535.6 444.61 12.05 45.94 7.56 98.68 0.769 7.132 −14.29 3.685 0.0285 BH-H13Y 20 0.182 27.09 543.43 457.45 12.67 49.8 9.52 110.95 0.695 2.524 −10.90 3.171 0.0255 40 0.223 26.65 541.46 457.73 12.76 49.63 9.58 114.23 0.630 2.461 −8.37 3.143 0.0261 60 0.249 26.47 550.53 454.46 12.55 49.23 9.46 109.03 0.543 2.892 −10.27 3.156 0.0252 80 0.213 25.77 544.72 447.61 12.26 48.67 9.13 108.59 0.520 1.942 −11.84 3.231 0.0260 96 0.223 25.52 544.89 456.75 12.6 49.59 9.29 108.43 0.491 3.082 −13.23 3.237 0.0255 120 0.148 25.21 547.51 455.22 12.96 49.45 9.11 108.59 0.473 2.766 −14.23 3.293 0.0261 140 0.152 24.63 543.91 451.65 12.56 48.83 8.84 106.81 0.446 3.428 −15.44 3.350 0.0264 160 0.158 24.47 547.45 451.41 12.48 48.94 9.02 106.87 0.436 3.769 −16.12 3.289 0.0259 180 0.182 24.03 545.01 457.18 12.44 49.17 8.82 108.91 0.447 3.884 −17.32 3.380 0.0270 195 0.192 24.25 556.92 452.68 12.31 48.78 8.62 107.75 0.543 3.998 −17.94 3.431 0.0273 220 0.179 22.71 543.81 452.49 12.32 48.37 8.67 104.89 0.490 4.095 −18.02 3.384 0.0265 240 0.184 22.29 540.84 451.25 12.22 48.06 8.94 104.56 0.461 4.686 −19.49 3.259 0.0256 260 0.244 21.95 546.77 448.87 12.03 47.7 8.51 103.90 0.483 4.713 −20.54 3.401 0.0267 280 0.230 21.15 543.46 449.36 12.01 47.18 8.39 103.50 0.508 4.991 −21.72 3.409 0.0270 BH-H13Y 300 0.215 20.11 537.08 447.42 12 46.51 8.32 102.63 0.539 5.861 −22.49 3.391 0.0270 320 0.212 19.46 546.95 453.52 12 47.19 8.29 103.31 0.604 5.592 −22.87 3.453 0.0272 340 0.283 18.10 541.56 449.22 11.85 46.31 8 103.42 0.645 6.344 −25.37 3.509 0.0282 360 0.235 16.78 535.98 449.7 11.8 45.87 7.99 102.00 0.693 7.263 −26.09 3.484 0.0279 380 0.276 15.59 533.93 444.82 12.66 45.19 7.55 97.01 0.754 7.374 −26.96 3.628 0.0281 400 0.267 14.82 547.52 449.07 11.56 45.21 7.92 99.01 0.813 8.463 −28.40 3.462 0.0273 BH-H61 20 0.247 25.84 538.4 454.1 13.09 49.28 8.96 104.35 0.558 2.422 −13.08 3.335 0.0255 40 0.262 25.64 551.9 451.77 13.14 48.42 10.6 101.93 0.523 2.766 −15.33 2.769 0.0210 60 0.316 24.42 542.6 453.09 13.01 48.48 8.01 106.13 0.543 3.096 −17.09 3.672 0.0290 80 0.273 23.65 542.6 451.84 12.81 48.16 8.34 105.04 0.527 3.491 −19.05 3.500 0.0275 100 0.254 23.18 541.5 450.5 12.87 47.64 7.59 102.04 0.552 3.332 −19.52 3.808 0.0294 120 0.247 22.35 536.0 450.57 12.13 48.43 7.97 102.09 0.537 4.478 −21.95 3.685 0.0280 140 0.292 21.72 536.4 453.87 12.28 48.42 8.05 103.68 0.568 5.051 −22.73 3.647 0.0282 160 0.257 21.32 540.5 454.5 12.3 48.27 7.91 106.74 0.655 4.880 −22.50 3.702 0.0295 180 0.275 20.74 539.3 456.83 12.47 48.13 7.72 102.96 0.587 5.396 −25.10 3.783 0.0292 200 0.262 20.02 535.9 454.22 12.64 47.43 7.3 103.11 0.626 4.905 −25.78 3.941 0.0309 220 0.300 19.41 543.2 447.65 12.12 46.83 7.44 97.33 0.655 5.036 −24.80 3.815 0.0286 240 0.288 18.55 534.6 452.94 12.16 47.36 7.25 98.69 0.732 5.899 −25.41 3.960 0.0298 260 0.279 18.16 537.2 449.73 12.12 46.77 7.42 101.83 0.817 6.140 −25.81 3.824 0.0300 280 0.248 17.09 534.3 451.92 11.96 46.44 7.24 93.98 0.860 6.779 −27.81 3.888 0.0284 300 0.276 16.54 531.5 453.23 12.05 46.11 6.82 100.82 1.023 7.145 −27.27 4.099 0.0323 320 0.218 15.53 538.8 453.64 11.96 45.61 6.62 100.99 1.249 7.571 −28.66 4.175 0.0333 340 0.368 14.45 540.2 446.22 12.12 44.36 6.42 95.29 1.367 8.152 −29.02 4.192 0.0325 360 0.215 13.36 540.2 448.78 11.88 44.39 6.2 96.56 1.657 8.880 −30.16 4.338 0.0340 380 0.254 12.03 533.6 441.29 11.74 43.31 5.93 93.73 1.981 9.809 −31.44 4.431 0.0346 400 0.282 11.03 535.4 445.44 11.8 43.45 5.99 91.60 2.217 9.353 −31.32 4.400 0.0334 420 0.238 9.69 545.9 449.54 11.72 43.1 5.41 89.43 2.600 11.214 −32.33 4.833 0.0362 440 0.253 8.06 548.1 444.96 11.8 42.15 5.06 90.38 3.317 11.688 −31.80 5.047 0.0390 460 0.235 5.67 539.8 446.84 11.87 41.69 4.92 87.55 4.437 12.656 −33.81 5.134 0.0389 480 0.261 2.90 541.1 443.6 11.76 40.55 3.95 86.94 6.049 12.674 −35.07 6.221 0.0481 500 0.284 1.13 538.3 440.84 11.69 40.24 3.24 86.91 8.980 13.449 −25.59 7.542 0.0587 520 0.277 1.28 530.7 436.26 12.05 39.84 3.64 83.04 9.311 11.883 −23.87 6.647 0.0499
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