Characteristics and controlling factors of submarine fluid escape in Tethys tectonic domain
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摘要: 海底流体逃逸活动会显著地改变海底地形地貌，产生麻坑、泥火山等地貌和冷泉羽状流现象。特提斯构造域是世界上油气最集中的构造域，流体逃逸活动广泛发育，形成的复杂流体逸出结构，对海洋油气勘探、全球气候变化研究等方面具有较好指示作用。本文选取特提斯构造域主要海域，系统总结其海底流体逃逸活动特征，发现特提斯构造域海底流体逃逸活动多分布在被动大陆边缘和弧后裂谷盆地等地质背景中，其中地中海、黑海和南海广泛发育海底冷泉、麻坑和泥火山等流体逃逸特征，而波斯湾和澳大利亚西北部近海大量发育碳酸盐岩。海底流体逃逸活动主要受控于活动断裂、沉积物超压、地震活动、海平面变化、潮汐活动和海底滑坡等海洋与地质因素。在不同海域，流体来源也不尽相同（热成因、生物成因以及天然气水合物分解），大多数通过断层、泥火山和气烟囱等通道运移。建议重视对特提斯构造域海底流体逃逸活动发育区的调查和探测，深入分析与之相关的海底流体逃逸地貌发育机制，以及其特殊海域背景下的海洋与地质因素控制作用，总结建立其海底流体逃逸活动模式及相关理论。Abstract: Seabed fluid escape may significantly change the seafloor topography, resulting in some geomorphic features such as pockmarks, mud volcanoes and cold seep plumes. The Tethys tectonic domain, the most hydrocarbon-rich domain in the world, hosts substantial fluid escape-related structures that can act as good indicators for offshore hydrocarbon exploration and global climate changes. Based on previous researches of major sea areas in the Tethys tectonic domain, this paper systematically summarized the characteristics of the seabed fluid flow, which shows that the seabed fluid escape activities of the Tethys tectonic area are mostly distributed in passive continental margins and back-arc rift basins. Seafloor manifestations of fluid escape including submarine cold seeps, pockmarks and mud volcanoes, are widely distributed in the Mediterranean Sea, the Black Sea and the South China Sea, however, massive carbonate-related structures are the prominent seabed fluid escape features in the Persian Gulf and the northwestern shelf of Australia. Seabed fluid flow is a dynamic process in the Tethys tectonic domain. The main marine and geological factors controlling fluid escape include active faults, sediment overpressure, seismic activities, sea-level changes, tidal activities and seabed landslides. Fluids are sourced from different intervals (thermal, biogenesis, and natural gas hydrate decomposition) in different sea areas, and the migration of fluids is mostly through fault planes, mud volcanoes and gas chimneys to the seafloor. To summarize and establish the model and theory of seabed fluid escape, it is suggested that more attention should be paid to the investigation and detection of the development areas of the seabed fluid escape activities in the Tethys tectonic domain. Moreover, the further analysis of the mechanism of the fluid escape-related geomorphic features, as well as the marine and geological controls in the special oceanic regions will provide basic support for the subsequent research.
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Keywords:
- Tethys /
- fluid escape /
- gas hydrate /
- oil and gas exploration /
- cold seep
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重金属元素广泛存在于自然界各种环境介质中[1]。重金属元素具有高隐蔽性、易富集性以及强生物毒性等特点，可通过食物链迁移并富集，会对动植物、人类健康以及生态系统多样性等造成严重危害[2-3]，因而受到广泛关注。例如，Ding等[4]研究表明，在水稻生长过程中Cd和Cr会在果实中累积，食用受污染的大米后会对人类健康造成威胁。
黄河三角洲湿地地处山东半岛东北部，是我国形成最晚、最广阔、保存最完整的暖温带河口湿地生态系统[5-6]，具有稳定海岸线、净化环境、水源涵养和保护生物多样性等多重生态系统服务功能[7]。近年来，随着社会经济的快速发展、工业生产规模不断扩大、人口快速增长等，大量污染物通过河流进入海洋，导致黄河三角洲出现不同程度的重金属污染[5,8]。例如，杨清香等[8]以黄河三角洲实验区表层沉积物为研究对象，运用地累积指数法和潜在生态风险指数评价法研究表明，Cd和Hg相较于其他元素污染较严重，且为主要的潜在生态风险因子。Yang等[9]对现代黄河三角洲表层土壤中Cr、Pb、Ni、Cd的分布及评价研究表明，该地区存在Cd中度污染和Pb轻度—中度污染，具有较强的生态危害性。
前人已对黄河三角洲地区进行了多方面的基础调查研究[10-13]，尤其是对黄河南北两岸以及黄河入海口的重金属元素研究较为深入[2-3,6,8]。尽管以往诸多学术成果为黄河三角洲湿地环境保护和生态建设等方面提供了翔实的史料，但是重点针对该地区北部湿地沉积物重金属元素污染风险评价和来源等方面的研究却屈指可数。因此，本文以黄河三角洲北部湿地为研究区，测定其表层沉积物中铜、铅、锌、铬、镍、镉、砷、汞的含量，分析这8种重金属的空间分布特征；进行重金属生态风险和污染程度评价，分析表层沉积物中重金属污染来源，阐明各环境因子对潜在生态危害指数RI值的解释程度，以期为黄河三角洲北部湿地重金属污染防治提供科学依据。
1. 研究区背景
研究区坐落于山东省东营市，位于黄河三角洲北部湿地（37°57′～38°5′N、118°37′～118°44′E）（图1），黄河故道西侧，地处渤海湾南岸。黄河三角洲湿地地处中纬度地区，属于暖温带季风气候类型，雨热同季，气候宜人，年平均气温为11.7～12.6℃，年平均日照时数为
2590 ～2830 h，年均降水量为530～630 mm，平均蒸散量为750～2400 mm。![]()
图 1 黄河三角洲北部湿地采样点分布图Figure 1. Distributionof wetland sampling points in the northern Yellow River Delta2. 材料与方法
2.1 样品采集与测定
2021年6月在黄河三角洲北部湿地开展外业调查，综合考虑当地实际地理情况以及土地利用方式，设置了39个采样点。用Garmin62SC手持GPS确定采样点经纬度，用木铲获取表层（0～5 cm）沉积物，并将样品装在聚乙烯样品袋中密封，外业调查结束后运回实验室。采样过程中用采集记录表记录采样点具体信息，用相机记录采样点周围环境。
沉积物样品室温风干，去除贝壳、草根等杂物，全部通过10目孔径试样筛处理，随后将样品用玛瑙球磨机研磨后过200目孔径试样筛。利用MS2000型激光粒度分析仪测定沉积物样品粒径，并按照砂、粉砂、黏土进行分级。样品用HF-HNO3-HCIO4混合溶液分解处理后，应用电感耦合等离子体质谱法（ICP–MS）测定Cu、Ni、Cd元素含量；样品采用粉末压片法制样后，应用X射线荧光光谱法（XRF）直接测定Cr、Pb、Zn元素含量；样品被王水分解后，应用氢化物-原子荧光光谱法（HG-AFS）测定As元素含量，应用冷原子-原子荧光光谱法（CV-AFS）测定Hg元素含量。
为保证测试的准确度和精密度，对样品进行5%的重复抽样，选用12个国家一级标准物质（水系沉积物GSD24、GSD25、GSD26、GSD27、GSD28、GSD31、GSD32，土壤GSS29、GSS31、GSS32、GSS34、GSS35）进行分析方法检验和质量控制，各项技术指标（检出限、报出率、准确度、精密度、检查分析合格率）均达到了《DZ/T 0130.5-2006 地质矿产实验室测试质量管理规范第5部分：多目标地球化学调查（1∶250000）土壤样品化学成分分析》及《DZ/T 0258-2014多目标区域地球化学调查规范》的要求，表明分析数据准确可靠。
2.2 土壤重金属污染风险评价方法
前人主要从沉积学角度对土壤重金属污染提出了诸多风险评价方法，主要包括潜在生态危害指数法、地累积指数法、单因子污染指数法、富集因子法等[14-15]。各评价方法优缺点不同，适用情况不同，本次研究主要应用地累积指数法和潜在生态危害指数法评价研究区表层沉积物中重金属的污染程度及其带来的生态风险。
2.2.1 地累积指数法
地累积指数（Igeo）又常被称为“Mull指数”，是一种应用环境介质中某元素实际含量及其对应地球化学背景值定量计算研究样品中重金属污染程度的方法[16-17]，计算公式如下：
$$ {I}_{\mathrm{g}\mathrm{e}\mathrm{o}}={\mathrm{l}\mathrm{o}\mathrm{g}}_{2}\left[{C}_{i}/\left(K\times {B}_{i}\right)\right] $$ (1) 公式中，K为修正系数，是指土壤层的沉积特征、岩石差异及其他影响所导致的背景值变化而设定的修正常数，一般取值1.5；Bi表示重金属元素i在沉积物中的背景参考值（mg·kg−1），滕彦国等[18]的研究表明，应用地累积指数法评价沉积物中重金属元素污染，选择与沉积物有直接联系的地球化学背景值得出的污染状况最为真实，故本文选择山东省东营市土壤环境背景值。地累积指数法一般分为7个级别，地累积指数法分级标准见表1[8,19]。
表 1 地累积指数法（Igeo）分级标准Table 1. Scaling of the land accumulation index (Igeo)地累积指数Igeo 等级 污染程度 Igeo＜0 0 无污染 0≤Igeo＜1 1 轻度—中度污染 1≤Igeo＜2 2 中度污染 2≤Igeo＜3 3 中度—重度污染 3≤Igeo＜4 4 重度污染 4≤Igeo＜5 5 重度—极度污染 5≤Igeo 6 极严重污染 2.2.2 潜在生态危害指数法
潜在生态风险指数是瑞典科学家Hakanson于1980年提出的一种基于环境学、生态学和生物毒理学的重金属污染评价方法，能够准确定量描述重金属的潜在危险程度，是目前研究评价沉积物重金属污染对生态环境影响常用的方法之一[8,17]，计算公式如下：
$$ {\rm{RI}}={\sum _{i=1}^{n}}{E}_{\rm r}^{i}={\sum _{i=1}^{n}}{T}_{\rm r}^{i}{C}_{\rm r}^{i}={\sum _{i=1}^{n}}{T}_{\rm r}^{i}\cdot{C}^{i}/{C}_{n}^{i} $$ (2) 公式中，Eir表示所采样品中重金属元素i的潜在生态危害指数；Tir表示所采样品中重金属元素i的生物毒性响应因子；Cin为样品中重金属元素i的背景参考值（mg·kg−1），本文采用山东省土壤元素背景值，重金属元素Hg、Cd、As、Pb、Cu、Ni、Cr、Zn的生物毒性响应因子分别为40、30、10、5、5、5、2、1，重金属潜在生态危害指数分级标准见表2[8,20]。
表 2 潜在生态危害指数法分级标准Table 2. Scaling of the potential ecological hazard index潜在生态危害单项系数Eir 单个污染物潜在生态风险程度 潜在生态危害指数RI 综合潜在生态风险程度 Eir＜40 轻微生态危害 RI＜150 轻微生态危害 40≤Eir＜80 中等生态危害 150≤RI＜300 中等生态危害 80≤Eir＜160 强生态危害 300≤RI＜600 强生态危害 160≤Eir＜320 很强生态危害 600≤RI＜ 1200 很强生态危害 Eir≥320 极强生态危害 RI≥ 1200 极强生态危害 2.3 地理探测器
地理探测器由分异及因子探测、交互作用探测、生态探测、风险区探测4个探测器共同组成，是探测并解译空间分层异质性影响机制的一系列统计学方法 [21]。此次研究主要应用分异及因子探测器分析影响因子对重金属元素潜在生态危害指数RI值的解释程度，应用交互作用探测器分析两影响因子在交互作用下对重金属元素潜在生态危害指数RI值的解释程度。分异及因子探测用q值度量，公式如下：
$$ q=1-\frac{{\sum }_{i=1}^{n}{m}_{i}{\sigma }_{i}^{2}}{m{\sigma }^{2}} $$ (3) 式中，q为因子对潜在生态危害指数RI值的解释力；n为变量Y或因子X的分层; mi为i层的单元数；σi2是i层的变量Y的方差；m为全区的单元数；σ2是全区的变量Y的方差。q∈[0,1]，q值越接近1表明变量Y的空间分层异质性越强，反之则越弱。
基于分异及因子探测器的交互作用探测器，分析两因子共同作用时q值的变化，以对应两因子共同作用增强或减弱对变量Y的解释力，亦或这些因子对变量Y的作用是互不影响的。因子协同作用类型可划分为非线性增强、独立、双因子增强、单因子非线性减弱以及非线性减弱。本文共选取黏土含量、TOC、含水率、距河距离、盐度、植被类型、距公路距离、距海距离等 8个环境因子。
2.4 数据分析与统计
本文使用ArcGIS10.8软件绘制重金属空间分布特征图，使用IBM SPSS Statistics 27软件进行数据处理和分析，利用地理探测器分析各环境因子对潜在生态危害指数RI值的解释程度。
3. 结果与讨论
3.1 沉积物重金属含量特征
黄河三角洲北部湿地表层沉积物重金属元素含量测定与统计结果如表3所示。由表3可知，研究区表层沉积物重金属平均含量由高到低顺序为：Cr＞Zn＞Ni＞Pb＞Cu＞As＞Cd＞Hg，且本文重金属元素平均含量与贾少宁等[6]的研究结果相当，略低于Cheng等[22]的研究结果。重金属元素变异程度表现为：Cd＞Cu＞Hg＞As＞Pb＞Zn＞Ni＞Cr（其中Zn变异系数为0.153，Ni变异系数为0.152）。据表3可知，研究区表层沉积物中重金属元素平均含量均低于国家土壤环境质量标准的一级标准[23]。与国内其他学者在不同区域的研究结果相比，元素Cu、Pb、Zn、Cr、Cd、As平均含量均低于珠江流域[24]；除As元素外，其他7种重金属元素含量平均值均低于长江三角洲[25]；除Zn元素含量略高于莱州湾，其他6种重金属元素含量平均值均略低于莱州湾[26]。研究区表层沉积物中重金属元素含量最大值均超过山东省土壤背景值[27]，其中只有As的平均值大于山东省土壤背景值。As的平均含量是山东省土壤背景值的1.06倍，表明研究区内出现了As富集现象，其变异系数属于中度变异（CV=0.21，中度变异范围为0.16～0.36[29]），由此看出，重金属元素As在研究区的分布具有分异性，表明砷污染与采样点周围环境密不可分。其中Cu、Pb、Cd、Hg只有极少部分采样点超出山东省土壤背景值，且变异系数为中度变异（CV范围为 0. 16～0. 31），表明这些重金属元素的主要来源可能是成土母质或采样点周边环境[6]。其中重金属元素Zn、Cr、Ni变异系数分别为0.15、0.10、0.15，属于低度变异（CV＜1.6），表明这3种重金属元素相对于其他元素受外界影响较小。
表 3 黄河三角洲北部湿地沉积物重金属含量Table 3. Contents of heavy metals in surface sediments of wetlands in northern Yellow River Delta项目 Cu Pb Zn Cr Ni Cd As Hg 最小值 7.70 13.20 43.50 45.50 18.00 0.06 5.66 0.01 最大值 28.60 26.80 81.80 75.70 35.00 0.20 14.70 0.03 平均值 17.60 17.70 58.20 59.00 23.40 0.09 9.07 0.02 中值 17.10 18.09 58.17 60.32 24.04 0.11 9.09 0.02 变异系数/% 0.29 0.16 0.15 0.10 0.15 0.31 0.21 0.28 国家一级标准值[23] 35.00 35.00 100.00 90.00 40.00 0.20 15.00 0.15 珠江流域[24] 48.72 63.97 186.60 67.44 – 2.76 49.29 – 长江三角洲[25] 29.94 31.95 86.17 75.39 30.85 0.18 8.30 0.15 莱州湾[26] 19.06 20.30 55.98 60.10 – 0.11 11.72 0.04 山东省背景值[27] 22.60 23.60 63.30 62.00 27.10 0.13 8.60 0.03 东营市背景值[28] 21.00 19.40 62.20 65.50 27.50 0.13 10.30 0.02 注：表中除变异系数外，其他单位均为mg/kg。 3.2 沉积物重金属空间分布特征
Pb和As在研究区内均有分布且空间分布特征较为相似，其呈现从西北向东南逐渐增加、从中间区域分别向西南和东北逐渐降低的空间分布特征，高值区出现在研究区东南部。Cu和Zn在研究区内均有分布且空间分布特征较为相似, 高值区出现在研究区东南部，低值区出现在研究区西南部。Cr、Ni、Cd、Hg在研究区内均有分布，Cr、Ni、Cd高值区均出现在研究区东南部，Cr、Ni低值区出现在研究区东北部，且Cr呈现从西北向东南逐渐增加的空间分布特征；Hg呈现从中间区域分别向西北和东南逐渐增加的空间分布特征，高值区出现在研究区西北部和东南部，低值区出现在研究区西南部（图2）。
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图 2 黄河三角洲北部湿地沉积物重金属分布示意图Figure 2. Distribution of heavy metals in surface sediments of wetlands in northern Yellow River Delta由Pearson相关系数矩阵（表4）可知，黏土含量与8种重金属元素含量均呈显著正相关，表明黏土对重金属元素吸附能力较强。由图3可知，32个采样点为砂质粉砂，4个采样点落于粉砂区、3个采样点落于粉砂质砂区。研究表明，在沉积物粒径为0.2～0.63 μm时，沉积物中重金属元素的分布与含量受到沉积物粒度影响，沉积物颗粒越细，比表面积越大，表面吸附能力越强，重金属元素含量越高[30-31]。故而研究区内8种重金属元素空间分布特征相似，可能是因为受到研究区内“粒度效应”影响。
表 4 黄河三角洲北部湿地沉积物中8种重金属含量及其与粒径相关性Table 4. The contents of 8 heavy metals in wetland sediments in the northern Yellow River Delta and their correlation with particle sizeCu Pb Zn Cr Ni Cd As Hg 砂 粉砂 黏土 Cu 1 Pb 0.74** 1 Zn 0.93** 0.83** 1 Cr 0.50** 0.70** 0.68** 1 Ni 0.42** 0.39* 0.45** 0.26 1 Cd 0.36* 0.52** 0.47** 0.28 0.79** 1 As 0.86** 0.73** 0.88** 0.69** 0.36* 0.28 1 Hg 0.87** 0.85** 0.93** 0.66** 0.50** 0.58** 0.81** 1 砂 –0.67** –0.46** –0.67** –0.29 –0.19 –0.15 –0.62** –0.58** 1 粉砂 0.50** 0.24 0.49** 0.09 0.08 0.02 0.43** 0.40* –0.95** 1 黏土 0.79** 0.76** 0.82** 0.60** 0.37* 0.37* 0.80** 0.77** –0.74** 0.50** 1 注：**表示在p＜0.01水平，相关性显著；*表示在p＜0.05水平，相关性显著。 ![]()
图 3 黄河三角洲北部湿地沉积物粒度三角图Figure 3. Grain size triangle diagram for surface sediments nomenclature in northern Yellow River Delta wetland3.3 沉积物重金属风险评价
3.3.1 地累积指数法评价
地积累指数评价结果显示（表5），8种重金属元素的Igeo平均值均小于0，重金属元素Cu、Pb、Zn、Cr、Ni、As在黄河三角洲北部湿地各采样点的污染等级均为无污染，重金属元素Cd、Hg在黄河三角洲北部湿地采样点中各有一个采样点的污染等级为轻度—中度污染，占比3%，其他采样点的污染等级均为无污染，占比97%，由此可知，重金属元素Cd、Hg为黄河三角洲北部湿地表层沉积物中的主要污染物。
表 5 黄河三角洲北部湿地沉积物重金属地累积指数评价结果Table 5. Evaluation results of heavy metal land accumulation index in wetland sediments in northern Yellow River DeltaCu Pb Zn Cr Ni Cd As Hg 最小值 –2.03 –1.14 –1.10 –1.11 –1.20 –1.63 –1.45 –1.72 最大值 –0.14 –0.12 –0.19 –0.38 –0.24 0.04 –0.07 0.00 平均值 –0.94 –0.70 –0.70 –0.71 –0.79 –0.95 –0.80 –0.84 标准偏差 0.44 0.22 0.21 0.15 0.21 0.41 0.30 0.39 无污染比例/% 100 100 100 100 100 97 100 97 轻度—中度污染比例/% 0 0 0 0 0 3 0 3 3.3.2 潜在生态危害指数法评价
重金属潜在生态环境风险分析显示，Cu、Pb、Zn、Cr、Ni、Cd、As、Hg 重金属元素的Eir值排序为Cd＞Hg＞As＞Ni＞Pb＞Cu＞Cr＞Zn（表6）。研究区内，虽然Hg和 Cd呈现轻微生态危害等级，采样点占比分别为97%、95%，但是Cd呈现中等生态危害等级的采样点占比5%，比同一等级的Hg的占比（3%）要高，因此Cd的潜在生态风险高于Hg；重金属元素Cu、Pb、Zn、Cr、Ni和As的潜在生态危害指数均小于40，属于轻微生态危害等级。研究区表层沉积物重金属元素的RI值为47.15～119.36，平均值为72.86（表6），潜在生态风险等级均为轻微生态危害等级。
表 6 黄河三角洲北部湿地沉积物重金属潜在生态危害指数评价结果Table 6. Evaluation results of potential ecological risk index of heavy metals in surface sediments of wetlands in northern Yellow River DeltaEir RI Cu Pb Zn Cr Ni Cd As Hg 最小值 1.70 2.80 0.69 1.47 3.32 14.54 6.58 12.13 47.15 最大值 6.33 5.68 1.29 2.44 6.46 46.15 17.09 40.00 119.36 平均值 3.78 3.83 0.92 1.95 4.44 24.26 10.57 23.11 72.86 轻微生态危害比例/% 100 100 100 100 100 95 100 97 100 中等生态危害比例/% – – – – – 5 – 3 – 8种重金属元素对黄河三角洲北部湿地表层沉积物RI值的贡献比例和整体潜在生态危害指数与Cd、Hg的单项潜在生态危害指数之间的关系显示，在黄河三角洲北部湿地表层沉积物中，Cd对潜在生态危害指数RI值的贡献率最高，高达33.30%，其单项潜在生态危害指数Eir值部分达到中等生态危害比例。Hg对潜在生态危害指数RI值的贡献率也较高，高达31.73%，其单项潜在生态危害指数Eir值也部分达到中等生态危害比例。As、Ni、Pb、Cu、Cr、Zn对潜在生态危害指数RI值的贡献率分别为14.50%、6.09%、5.26%、5.19%、2.67%、1.26%，明显低于Cd和Hg，潜在生态风险等级仅达到轻微生态危害等级。由图4b可以看出，RI值与Cd、Hg的Eir值变化走向较为相似，再次证明Cd、Hg是黄河三角洲北部湿地表层沉积物重金属污染的主要生态危害因子。大量研究表明，Cd、Hg是由喷洒农药以及施有机肥等农业活动、工业生产、大气沉降、交通运输、污水灌溉等污染输入[20,32]，对滨海湿地具有一定的影响[8,17,19,26]。
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图 4 8种重金属元素对黄河三角洲北部湿地沉积物RI值的贡献比例(a)和整体潜在生态危害指数与Cd、Hg的单项潜在生态危害指数之间的关系图(b)Figure 4. The contribution ratio of 8 heavy metal elements to the RI value of wetland sediments in the northern Yellow River Delta (a); and the relationship between the overall potential ecological hazard index and the single potential ecological hazard index of Cd and Hg (b)3.3.3 两种评价结果的对比
利用地累积指数法得出的污染程度排序为Cd＜Cu＜Hg＜As＜Ni＜Cr＜Pb＜Zn，重金属元素Cd、Hg为主要污染物，利用潜在生态危害指数法得出的潜在生态危害程度排序为Zn＜Cr＜Cu＜Pb＜Ni＜As＜Hg＜Cd，重金属元素Cd、Hg为主要生态危害因子。可见，两种分析方法既存在一定的一致性，又存在明显的差异性。首先，可能是因为参考背景值不同，地累积指数法采用山东省东营市土壤环境背景值为参考值，潜在生态危害指数法采用山东省土壤元素背景值为参考值。其次，可能是因为潜在生态危害指数法不仅采用了重金属元素的实测含量，而且采用了重金属元素的生物毒性响应因子。
3.4 沉积物重金属污染源分析
为了分析黄河三角洲北部湿地表层沉积物中元素来源的相似性，使用IBM SPSS Statistics 27软件对表层沉积物中8种重金属元素进行相关性分析，结果见表4。
土壤中重金属元素的赋存主要受自然和人为因素的影响，其来源或地球化学过程的相似性可能导致不同元素之间存在一定的相关性，因此分析重金属元素之间的相关性是推断重金属来源的重要依据[33-34]。由表4可知，Cu、Pb、Zn、Cr、As、Hg之间具有极显著的正相关关系（P＜0.01），相关系数为0.50～0.93，说明在黄河三角洲北部湿地表层沉积物中Cu、Pb、Zn、Cr、As、Hg具有相似的地球化学行为[17]。Ni和Cd之间呈现极显著正相关（P＜0.01），相关系数为0.79，说明在黄河三角洲北部湿地表层沉积物中Ni和Cd可能具有同源性或有相似的地球化学行为[33]。研究表明，Ni是植物生长必需的微量元素之一，磷肥中含有矿质成分Ni，磷肥生产原料磷矿石的加工过程也会引入 Cd[3,6,35]，故而Ni和Cd的污染源可能是磷肥的使用。
为更加准确地识别黄河三角洲北部湿地表层沉积物中重金属元素来源，使用因子分析和聚类分析对重金属元素进行分析（表7、图5）。
表 7 黄河三角洲北部湿地沉积物中重金属元素因子分析Table 7. Factor analysis of heavy metal elements in wetland sediments in the northern Yellow River Delta元素 因子1 因子2 As 0.921 0.117 Zn 0.918 0.305 Cu 0.874 0.248 Hg 0.850 0.431 Pb 0.829 0.364 Cr 0.763 0.094 Cd 0.197 0.940 Ni 0.184 0.879 黏土 0.859 0.208 TOC 0.521 0.447 特征值 5.529 2.394 方差百分比/% 55.293 23.937 累积方差百分比/% 55.293 79.230 注：旋转方法采用凯撒正态化最大方差法。 ![]()
图 5 黄河三角洲北部湿地沉积物中重金属元素聚类分析Figure 5. Cluster analysis of heavy metal elements in surface sediments of wetlands in northern Yellow River Delta在因子分析中KMO检验值为0.85，Bartlett球形检验值显著性水平P＜0.001，表明其适合进行因子分析。因子分析结果如表7所示，存在两个结果特征值大于1，共可以提取出2个因子，这两个因子可以解释总变量方差的55.293%和23.937%，旋转后累计方差贡献率达到79.230%，反映了数据的大部分信息。其中As、Zn、Cu、Hg、Pb、Cr、黏土、TOC在因子1中具有较高的载荷，表明As、Zn、Cu、Hg、Pb、Cr具有相似的来源，且受到TOC和黏土的影响。相关研究表明，有机碳是重金属元素迁移的重要载体[36]，前文亦已证明重金属元素受“粒度效应”影响；Cd、Ni在因子2中具有较高的载荷，分别为0.940、0.879。该因子分析结果与上述相关性分析结果一致。研究区周边有油田建设，存在工业生产、农业活动以及水产养殖等，且有研究表明，Cd是农业活动的标识元素，Cu、Ni是油田开采的标识元素[37]，结合相关性分析和重金属含量特征可知，因子1代表来源可能是成土母质、工业活动以及油田开采，因子2代表来源可能是农业活动、水产养殖以及油田开采。
为了验证并深入研究因子分析的结果,识别出黄河三角洲北部湿地表层沉积物中重金属元素更详细的来源划分，对黄河三角洲北部湿地表层沉积物重金属元素含量进行了聚类分析（图5），聚类分析将8种重金属元素分为与因子分析相同的Zn、As、Cu、Hg、Pb、Cr与Cd、Ni两大类，同时可以将其划分的更加细微，将Zn、As、Cu、Hg、Pb、Cr一大类中的Cr单独分为一类，共分为3类：① Zn、As、Cu、Hg、Pb，② Cr，③ Cd、Ni，分为一类的重金属元素可能有更相似的来源、性质或地球化学行为。
3.5 潜在生态危害指数影响因素分析
3.5.1 因子探测
利用因子探测器探测8个因子对黄河三角洲北部湿地表层沉积物重金属元素潜在生态危害指数RI值的影响程度（图6），结果表明不同影响因子对潜在生态危害指数RI值解释力不同，各环境因子的q值从高到低顺序为黏土含量（0.589）＞TOC（0.585）＞含水率（0.550）＞距河距离（0.443）＞盐度（0.402）＞植被类型（0.387）＞距公路距离（0.248）＞距海距离（0.114）。黏土含量、TOC、含水率对表层沉积物重金属元素潜在生态危害指数RI值解释力较大（q值均在0.5以上），可能是因为这几种环境因子均属于自然条件因子，黏土含量、TOC、含水率等自然条件可以影响成土母质的形成、重金属元素的迁移和转化等，从多个方面影响重金属元素含量，进而影响重金属元素潜在生态危害指数RI值。综合8个因子探测结果可知，重金属元素潜在生态危害指数RI值不止受到自然过程影响，还受控于人类活动，主要影响因素是自然条件因子。
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图 6 各影响因子对RI值影响的解释力Figure 6. Explanatory power of the effect of each influence factor on RI values3.5.2 交互作用探测
沉积物中重金属元素的空间分布不只受单一因素控制，而是由人类活动、自然环境等多种影响因素共同作用的结果[38]。故而，本研究采用交互作用探测器探测8种影响因子对黄河三角洲北部湿地表层沉积物重金属元素潜在生态危害指数RI值交互作用程度。如图7所示，任意两个影响因子交互作用的解释力q均高于单个影响因子，全部为双因子增强、非线性增强，不存在减弱和独立的交互作用类型，表明复杂的环境将加剧湿地的潜在生态危害。其中，距公路距离与黏土含量、距河距离与TOC、距河距离与含水率、距河距离与盐度、距河距离与距海距离、距河距离与距公路距离、距公路距离与盐度对重金属元素潜在生态危害指数RI值交互作用较为显著；距公路距离、植被类型两个人类活动因子在交互探测中对其他自然条件因子也有着显著的增强作用，表明重金属元素潜在生态危害指数RI值受自然条件和人类活动等多种因素共同影响。
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图 7 各影响因子对RI值影响的交互作用Figure 7. Interaction of the effect of each influencing factor on the RI value4. 结论
本文以黄河三角洲北部湿地39个表层沉积物样品为研究对象，基于地累积指数法、潜在生态危害指数法、相关性分析、因子分析和聚类分析等方法，对黄河三角洲北部湿地沉积物进行了重金属污染风险评价及来源分析，取得以下几点认识：
（1）黄河三角洲北部湿地表层沉积物8种重金属元素除As外平均含量均低于山东省土壤背景值，其平均含量由高到低顺序为Cr＞Zn＞Ni＞Pb＞Cu＞As＞Cd＞Hg。东南部均出现高值区，可能受到“粒度效应”的影响。
（2）地累积指数法和潜在生态危害指数法表明，Cd、Hg为研究区主要污染物和重要的潜在生态危害因子。
（3）相关性分析和因子分析表明，Cu、Pb、Zn、Cr、As、Hg可能来源于成土母质、工业活动以及油田开采， Ni、Cd可能来源于农业活动、水产养殖以及油田开采；聚类分析可进一步把Cr单独划分为一类。
（4）因子探测分析结果显示黏土含量、TOC、含水率对潜在生态危害指数（RI值）解释力较大，表明其对RI值的影响较大；交互作用探测发现，任意两个影响因子交互作用后结果为双因子增强或非线性增强，表明复杂的环境将加剧湿地的潜在生态危害，重金属元素潜在生态危害指数RI值受自然条件和人类活动等多种因素共同影响。
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图 1 特提斯构造域展布范围
据http://tethys.ac.cn。
Figure 1. The distribution of Tethyan tectonic domain
From http://tethys.ac.cn.
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图 6 南海及周边地区的构造背景和海底流体逃逸特征分布[6, 47, 67, 130]
据南海地质地球物理图系-地貌图。a. 海底生物和逃逸的气泡[124]，b. 麻坑[72]，c. 海底泥火山[125]。
Figure 6. The tectonic setting and distribution of fluid escape-related features in the South China Sea and surrounding areas[6, 47, 67, 130]
From the geomorphological map of the atlas of geology and geophysics of the South China Sea.a. the gas bubble and benthic organism[124], b. pockmark[72], c. submarine mud volcano[125].
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表 1 特提斯构造域海底流体逃逸
Table 1 Seabed fluid escape in the Tethys tectonic domain
研究区域 构造背景 主要逃逸特征 流体来源 运移通道 地质控制作用 主要参考文献 波斯湾 裂谷盆地 碳酸盐岩 热成因 断层 褶皱活动 [121-122] 地中海 俯冲带、被动大陆边缘 泥火山、麻坑、活动冷泉 热成因、生物成因、
天然气水合物分解断层、泥火山、气烟囱 海底滑坡、沉积物超压、高沉积速率、挤压构造、孔隙压力升高 [3,86,103] 黑海 弧后裂谷盆地 泥火山、麻坑、活动冷泉 生物成因、天然气水
合物分解断层、泥火山、气烟囱 海底滑坡、海平面升降、活动断层、海底峡谷、地震活动 [16,114] 南海 主动、被动与走滑大陆边缘 泥火山、麻坑、活动冷泉、碳酸盐岩 生物成因、热成因、
天然气水合物分解断层、泥火山、气烟囱 地震活动、深部底辟运动、倾斜断层和沉积边界 [44,47] 澳大利亚西北近海 被动大陆边缘 碳酸盐岩 热成因 断层 断层、海平面升降、潮汐活动 [21] 
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