CROSS-SECTION DISTRIBUTION AND MORPHOLOGY OF AUTHIGENIC PYRITE AND THEIR INDICATION TO METHANE SEEPS IN SHENHU AREAS, SOUTH CHINA SEA
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摘要: 自生黄铁矿是渗漏甲烷发生甲烷厌氧氧化和硫酸盐还原作用的产物之一，是海底甲烷渗漏活动的有效示踪剂。南海神狐海域是我国天然气水合物研究的重点区域，对神狐海域柱状沉积物中自生黄铁矿含量、分布、形貌等特征进行研究，结果发现自生黄铁矿的含量随深度增加而递增，存在两个异常富集峰段：在第一个黄铁矿富集峰段，黄铁矿以长条状为主，外形较粗，微晶形态以草莓状黄铁矿为主，且粒径均一；在第二个峰段主要以细长的条状黄铁矿为主，由带外壳结构的草莓球颗粒组成，晶粒大小不一，存在二次生长现象。另外还发现胶黄铁矿与自生黄铁矿共生。这些特征反映神狐海域沉积物中存在多期次的甲烷渗漏事件，高通量的甲烷渗漏发生在较浅的层位，可能发生甲烷的有氧氧化而变成缺氧环境，有利于黄铁矿富集在第一个峰段；较低的甲烷渗漏发生在较深的层位，甲烷厌氧氧化和硫酸盐还原作用而形成大量的黄铁矿保存在第二个峰段。因此，神狐海域沉积物中自生黄铁矿的异常富集可以作为地质历史时期甲烷渗漏通量和期次的指示矿物之一。Abstract: Sulfate reduction associated to anaerobic oxidation of methane (AOM-SR) is considered an important process of methane consumption in anoxic marine environments. This process results in the enrichment of authigenic pyrite, which may provide important information to active methane seepages. The Shenhu is one of the favorable areas for gas hydrate accumulation. We studied the content, distribution and morphology of the authigenic pyrite from two cores of sediments collected from the Shenhu area. Results show that the content of pyrite increases with depth and has two peaks. The pyrite in the shallow sediment is irregular tubelike and consists of pyrite framboids in similar size. In deep sediments, however, the pyrite occurs as straight tubes and consisting of framboidal cores and outer crusts. Microcrystals vary in different size. In addition, it is found that greigite always coexists with pyrite. Our results indicate a kind of temporal variation of methane flux occurs in the Shenhu sediment: relatively high methane flux occurs at the depth of shallow pyrite-rich peak, and the aerobic oxidation of methane influences bottom water redox conditions in the sea and promotes the precipitation of pyrite. Lower methane flux occurs in the deeper layers of sediments, AOM-SR is the main process to the precipitation of pyrite in the deep sediment. Overall, our results suggest that the anomalous enrichment of pyrite in sediment may be used as an indicator to methane seepage events in marine sediments.
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Keywords:
- authigenic pyrite /
- anomalous enrichment /
- methane seepage /
- Shenhu
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图 2 南海北部神狐柱状沉积物HS148站位硫酸盐和甲烷浓度(a)、有机碳(b)和黄铁矿含量(c)剖面变化
(硫酸盐-甲烷转换带以硫酸盐和甲烷浓度来确定，深度为707cmbsf)
Figure 2. Pore-water and sediment geochemistry of core sediment from site HS148. (a) Profiles of interstitial dissolved sulfate and methane. (b) Content of the total organic carbon. (c) Content of the hand-picked pyrite The current sulfate-methane transition zone (SMTZ) is defined by sulfate and methane concentrations, the depth is 707cmbsf
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图 3 南海北部神狐柱状沉积物HS328站位硫酸盐和甲烷浓度(a)、有机碳(b)和黄铁矿含量(c)随剖面变化
Figure 3. Pore-water and sediment geochemistry of core sediment from site HS328. (a) Profiles of interstitial dissolved sulfate and methane. (b) Content of the total organic carbon. (c) Content of the hand-picked pyrite
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图 4 南海北部HS148站位沉积物自生黄铁矿形貌图
(A-F为本文样品，G-H引自文献[37])
Figure 4. Typical habits of pyrite aggregates from the core sediment of the northern South China Sea
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图 5 自生黄铁矿的微观结构图
Figure 5. Scanning electron microscopic(SEM) images of authigenic pyrite
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图 6 自生黄铁矿扫描电镜图及其对应的能谱图
(样品号及深度：HS148: 303~313cmbsf)
Figure 6. SEM images and energy dispersive spectrometer (EDS) data of pyrite crystal
表 1 南海神狐海域两站位孔隙水及沉积物硫酸盐，甲烷，有机碳和自生黄铁矿的含量
Table 1 Concentrations of sulfate and methane in pore water, content of total organic carbon and authigenic pyrite in the two cores of sediment from Shenhu area
HS148
深度/cmSO42-/
mMCH4/
(μL/kg)TOC/% 黄铁矿/% HS328
深度/cmSO42-/
mMCH4/
mMTOC/% 黄铁矿/% 10 32.2 20.1 0.9 10 27.14 14.43 1.08 0.000 47.5 1.08 42.5 1.18 0.001 80 1.43 0.006 80 23.24 16.55 1.27 0.008 101.5 1.46 0.005 112.5 1.46 0.005 123 21.8 14.41 1.42 130 1.53 0.007 155.5 1.59 0.189 150 22.76 13.80 1.23 0.005 175.5 1.63 182.5 1.44 0.023 193 18.6 6.27 1.55 200 1.51 0.004 213 1.52 0.034 215 1.33 0.013 230.5 1.48 0.050 251 1.48 0.008 245.5 1.5 0.004 284.5 17.16 17.48 1.51 0.002 263 22.4 13.11 1.41 317 1.46 0.003 283 1.7 0.002 337 19.06 13.45 1.04 0.001 300.5 1.61 0.013 354.5 1.03 0.002 315.5 1.71 0.024 387 1.43 0.055 333 18.7 14.6 1.68 407 17.61 17.59 1.34 0.003 353 1.71 441 1.24 0.052 370.5 1.63 0.034 477 15.80 13.99 1.38 0.002 385.5 1.78 0.006 509.5 1.59 0.015 403 15.9 24.82 1.71 547 13.11 12.33 1.49 0.023 423 1.64 0.008 579.5 1.75 0.004 440.5 1.59 0.076 597 1.49 0.048 455.5 1.65 617 11.94 13.80 1.58 0.030 473 13.4 12.29 1.46 649.5 1.76 0.008 510.5 1.54 0.047 667 1.62 0.088 525.5 1.47 687 11.14 12.72 1.52 0.029 543 10.2 13.76 1.41 0.027 704.5 1.63 0.111 563 1.46 0.350 719.5 1.78 0.072 580.5 1.44 737 1.65 0.129 595.5 1.65 0.055 757 8.63 16.54 1.00 0.018 613 7.4 7.53 1.19 774.5 1.84 0.024 630.5 1.34 0.108 789.5 1.48 0.042 675.5 1.38 0.039 807 1.78 0.089 690 1.59 0.011 834.5 1.93 0.049 707 4.5 106.76 1.42 852 5.82 11.48 1.62 0.009 
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