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物探与化探, 2024, 48(2): 527-533 doi: 10.11720/wtyht.2024.1088

生态地质调查

防城港海域沉积物中正构烷烃分布和来源解析

庞国涛,1, 杨源祯1, 谢磊1, 李伟1, 张晓磊1,2, 闫兴国1

1.中国地质调查局 烟台海岸带地质调查中心,山东 烟台 264000

2.中国海洋大学 海洋地球科学学院,山东 青岛 266100

Distribution and sources of n-alkanes in sediments in the Fangchenggang sea area

PANG Guo-Tao,1, YANG Yuan-Zhen1, XIE Lei1, LI Wei1, ZHANG Xiao-Lei1,2, YAN Xing-Guo1

1. Yantai Center of Coastal Zone Geological Survey, China Geological Survey, Yantai 264000, China

2. College of Marine Geosciences, Ocean University of China, Qingdao 266100, China

责任编辑: 蒋实

收稿日期: 2023-02-28   修回日期: 2023-06-15  

基金资助: 中国地质调查局自然资源综合调查指挥中心项目(ZD20220131)
中国地质调查局项目(DD20191024)

Received: 2023-02-28   Revised: 2023-06-15  

作者简介 About authors

庞国涛(1990-),男,硕士,工程师,主要从事海岸带环境地质调查与评价工作。Email:pgt5241@163.com

摘要

正构烷烃由于其化学性质稳定,在自然界中普遍存在,是表征有机质来源的良好标志物。利用气质联用仪(GC/MS)对2021年9月采集的防城港海域表层沉积物中的正构烷烃进行检测,对其含量、分布特征进行分析,运用特征参数对其来源进行解析。结果表明:正构烷烃含量在(67.51~850.08)×10-9(干重)之间,均值为476.69×10-9(干重),高值区主要分布在企沙半岛南部海域;主要由连续分布的n-C14~n-C35正构烷烃同系物组成,呈双峰分布,前峰群偶碳数优势,后峰群奇碳数优势;陆、海源烷烃比(∑T/∑M)、碳优势指数(CPI)和陆、海源烷烃优势比(TAR)均指示研究区正构烷烃受陆源影响明显;平均链长(ACL)、烷烃指数(AI)和Pmar-aq进一步表明其主要来源于陆源草本植物;T-ALK/C16比值表明研究海域受到石油污染影响;姥鲛烷和植烷比值(Pr/Ph)表明研究海域沉积物中正构烷烃形成于氧化环境。

关键词： 沉积物; 正构烷烃; 特征比值; 来源

Abstract

n-alkanes, exhibiting stable chemical properties, are ubiquitous in nature. They are favorable indicators of the source of organic matter. Using the gas chromatography-mass spectrometry (GC/MS), this study detected n-alkanes in the surface sediments sampled from the Fangchenggang sea area in September 2021. It analyzed their content and distribution, as well as their source based on characteristic parameters. The results are as follows: ① The n-alkanes of the Fangchenggang sea area manifested a content range of (67.51~850.08)×10-9 (dw), averaging 476.69×10-9 (dw), with high values primarily distributed in the southern sea area of Qisha Peninsula; ② They were principally composed of extensive n-C14~n-C35 n-alkane homologues in a bimodal distribution. The former peak group displayed an even-carbon number advantage, while the latter showed an odd-carbon number advantage; ③ The terrestrial-marine alkane ratio (ΣT/ΣM), carbon predominance index (CPI), and terrestrial-marine alkane predominance ratio (TAR) all indicate a significant terrestrial influence on n-alkanes in the Fangchenggang sea area; ④ The average chain length (ACL), alkane index (AI), and Pmar-aq further suggest that n-alkanes were mainly from terrestrial herbs; ⑤ The T-ALK/C16 ratio implies that the Fangchenggang sea area experienced oil pollution; ⑥ The pristane/phytane ratio (Pr/Ph) reveals that n-alkanes in the sediments of the Fangchenggang sea area formed in an oxidizing environment.

Keywords： sediment; n-alkane; characteristic ratio; source

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本文引用格式

庞国涛, 杨源祯, 谢磊, 李伟, 张晓磊, 闫兴国. 防城港海域沉积物中正构烷烃分布和来源解析[J]. 物探与化探, 2024, 48(2): 527-533 doi:10.11720/wtyht.2024.1088

PANG Guo-Tao, YANG Yuan-Zhen, XIE Lei, LI Wei, ZHANG Xiao-Lei, YAN Xing-Guo. Distribution and sources of n-alkanes in sediments in the Fangchenggang sea area[J]. Geophysical and Geochemical Exploration, 2024, 48(2): 527-533 doi:10.11720/wtyht.2024.1088

0 引言

正构烷烃(n-alkanes)指没有碳支链的饱和碳氢化合物,在海洋表层沉积物中具有普遍存在性和较高的稳定性,主要来自石油污染、生物质以及化石燃料的燃烧等[1-2]。由于其化学性质稳定,能够经过长期搬运稳定保存在沉积物中,因此可通过沉积物中正构烷烃的碳数来判断其来源及沉积环境[3-4]。目前,国内外学者利用正构烷烃组分比值和特征参数等对沉积物有机质进行源解析的研究已相当成熟,Venturini等[5]通过正构烷烃总量/C16、低/高分子量比值L/H及主峰碳MH值等来判断沉积物中正构烷烃的来源;Eglinton等[6]通过对沉积物中正构烷烃的前、后峰群含量研究来判断其陆源或海源;此外,还有学者利用正构烷烃陆源与海源比值(∑T/∑M)、优势正构烷烃比值(TAR)、Pmar-aq指标、平均链长(ACL)和烷烃指数(AI)等参数对正构烷烃进行溯源研究[7⇓⇓-10]。

防城港是我国西南地区第一大港,也是我国的深水良港,是我国西南地区走向世界的海上主门户[11]。近年来随着中国—东盟自由贸易区建设和人类活动增加,货轮航运随之增加,加之沿岸养殖业、工业的无序扩张,河流污染物质的持续输入,导致港口近岸海域的环境问题日益受到关注,生态系统遭受威胁。目前国内外学者对海洋沉积物中的正构烷烃组成及来源研究颇多[8⇓⇓-11],但对防城湾海域正构烷烃的研究还是空白,面对日益增长的有机质污染威胁,对该地区海域沉积物中正构烷烃的源汇研究显得尤为重要。本文以防城港海域表层沉积物中的正构烷烃为研究对象,研究其含量、组成、分布特征,并运用正构烷烃的多参数比值特征来判断沉积区有机质的来源,以期为港口近岸海域的有机质控制和环境治理提供必要的数据支撑和理论指导。

1 材料与方法

1.1 样品采集

2021年9月在防城港海域采用抓斗取样器采集表层沉积物样品21件,水深变化范围为6.5~29 m,站位分布如图1所示。抓斗出水后先将沉积物表层杂物清理干净,测试并记录样品物理性质、测深信息,而后用洁净木铲取表层0~5 cm的沉积物,去除样品中的杂质后,快速装入准备好的洁净锡纸样品袋中,密封冷冻保存直至送样。样品的采集、保存及后期处理等均按照GB 17378.3—2007[12]的相关规定进行。

图1

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图1   防城港海域采样位置

Fig.1   Sampling location of Fangchenggang sea area


1.2 样品处理与仪器分析

样品测试在青岛海洋地质研究所海洋地质实验检测中心完成。样品经解冻干燥后,称取约4.0 g放入锥形瓶中,加入适量二氯甲烷与甲醇(3∶1)混合溶液,采用加速统计萃取仪(ASE,200)在100 ℃、10 MPa下静态萃取2次(10 min/次),收集得到总可萃取有机质。萃取液经柔和N2吹干后用3 mL氢氧化钠—甲醇溶液(浓度6%)进行碱水解,而后室温反应12 h,反应完全后再用正乙烷萃取得到中性有机类脂质。正乙烷萃取组分浓缩后,用硅胶层析柱进行净化,而后用8 mL正乙烷淋洗得到正构烷烃组分,再经12 mL二氯甲烷与甲醇(95∶5)混合液淋洗得到醇酮组分。淋洗液浓缩至80 μL,利用气质联用仪(GC/MS)对正构烷烃组分进行分析。

GC/MS型号为Agilent7890A/5975C MS,配有自动进样器。石英毛细管色谱柱:HP-5(30 m×0.25 mm×0.25μm)。气相色谱柱条件:进样量1 μL,采用不分流模式进样,载气为高纯氦气,流速1.0 mL/min,恒流。升温程序:进样口温度为290 ℃,80 ℃保持1 min,10 ℃/min升至200 ℃,5 ℃/min升至250 ℃,2 ℃/min升至290 ℃,保持10 min。质谱条件:电子轰击离子源(EI,70 eV),全扫模式,质量扫描范围50~600 amu。根据组分保留时间和特征离子进行定性,采用内标法和多点校准曲线进行定量。

质量控制:测定过程中所用的试剂均为优级纯,每次分析需至少做一个全程序空白样品、平行样品和加标回收样品的测定。测定结果中空白测试样品应低于方法检出限(表1),正构烷烃加标回收率为70%~120%,平行双样测定结果的相对偏差小于30%。经统计,本次测试数据均满足质量要求。

表1   正构烷烃检出限

Table 1  Detection limit of n-alkanes

名称检出限/
10-9		名称检出限/
10-9		名称检出限/
10-9
C141.2C200.3C280.4
C151.0C210.5C290.5
C160.8C220.6C300.5
C170.3C230.6C310.6
Pr0.2C240.5C320.5
C180.5C250.5C330.5
Ph0.6C260.4C341.0
C190.6C270.5C351.5

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2 结果与讨论

2.1 正构烷烃含量和组成特征

防城港海域各个站位表层沉积物中正构烷烃含量范围为(67.51~850.08)×10-9(干重),平均值为476.69×10-9(干重),其中高值区主要分布在研究区东北部,由东北向西南含量逐渐降低(图2)。前人研究表明,研究区潮流为往复流,落潮流大于涨潮流,潮流方向为NE—SW走向[13],防城港海域沉积物正构烷烃分布和潮流方向一致,推测高值区主要是由落潮时潮流携带有机质沉积形成。

图2

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图2   研究区沉积物正构烷烃分布

Fig.2   Distribution of n-alkanes in sediments of the study area


防城港海域各个站位沉积物中正构烷烃峰型相似,说明该海域表层沉积物的正构烷烃来源基本一致,正构烷烃分子数分布范围为n-C14~n-C35。为了更好地了解其组合特征,选取典型代表性站位(FC28)对其正构烷烃含量碳数作图分析(如图3所示),可以发现,研究区海域沉积物中正构烷烃呈双峰型分布,前峰群链长在n-C14~n-C21,以n-C14、n-C16和n-C18为主峰,具有明显的偶碳数优势;后峰群碳链在n-C22~ n-C35,其中n-C29、n-C31、 n-C33正构烷烃含量明显高于其他碳数的正构烷烃,具有明显的奇碳数优势。后峰群含量高于前峰群,初步判断研究区沉积物中正构烷烃受陆源影响较强[14⇓-16]。前人研究表明,木本植物输入源的正构烷烃多以n-C29为主峰,草本植物输入源的正构烷烃多以n-C31为主峰[17-18]。研究区站位正构烷烃后峰群链多以n-C31为主峰,n-C29含量略低于n-C31,可以看出,防城港海域表层沉积物中草本植物源高于木本植物源。研究区所有站位正构烷烃分布中均检测出了植烷(Ph)和姥鲛烷(Pr),说明该海域可能受到了石油及其衍生品的影响。

图3

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图3   典型站位不同链长烷烃含量的直方图

Fig.3   Histogram of n-alkane content with different chain length at typical stations


正构烷烃的前峰群中n-C15~n-C21的总量∑C15-21可代表海源(浮游藻类和细菌)烷烃含量[19],后峰群中n-C25~n-C35的总量∑C25-35可代表陆源烷烃含量[20]。二者空间分布情况如图4所示,∑C15-21的变化范围为(16.30~370.80)×10-9,平均值140.52×10-9,其高值区主要分布在研究区中东部,其他区域值均较小;∑C25-35的变化范围为(45.71~488.0)×10-9,平均值291.74×10-9,其高值区主要分布在企沙半岛南部海域,受防城江入海及东部钦州湾的影响较为明显。陆源正构烷烃呈现出较为明显的近岸高值向海逐渐降低的趋势。

图4

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图4   表层沉积物中海源正构烷烃∑C15-21、陆源正构烷烃∑C25-35含量的空间分布

Fig.4   Spatial distribution of marine and terrestrial n-alkanes ∑C15-21 and ∑C25-35 contents in surface sediments


为了解研究区海域正构烷烃浓度水平,将防城港海域表层沉积物中正构烷烃的浓度与国内典型海域进行对比,如表2所示,研究区海域表层沉积物中正构烷烃浓度水平远低于锦州湾、东海近岸、厦门海域和渤海及邻近海域。与其他区域相比,研究区仅有防城江有机质输入,且受防城湾的影响只有少部分能到达研究海域;此外,防城港港口建设起步较晚,海洋产业相对其他地区欠发达有关。

表2   近岸海域表层沉积物中正构烷烃浓度比较

Table 2  Comparison of n-alkane concentrations in surface sediments of offshore waters

位置碳数总量/
10-9		均值/
10-9		参考文献
锦州湾n-C8~ n-C381900~42002600[2]
东海近岸n-C14~n-C34530~22001515[21]
厦门海域n-C9~n-C361800~42702749[22]
渤海及邻近海域n-C11~n-C36900~51002250[23]
防城港海域n-C14~n-C3567.51~
850.08		476.69本研究

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2.2 正构烷烃特征参数及来源解析

利用地球化学特征比值对正构烷烃来源进行解析已相当成熟,研究区沉积物中正构烷烃特征参数如表3所示。

表3   研究区表层沉积物正构烷烃特征参数

Table 3  The geochemical proxies of n-alkanes alkanes in surface sediments of study areas

分析项目T-ALK/10-9CPI1CPI2∑T/∑MACLTART-ALK/C16AIPmar-aqPr/Ph
FC01286.710.482.383.6030.134.2516.180.610.141.67
FC03197.340.512.272.0630.032.4310.160.570.151.41
FC0567.510.902.543.1730.112.9720.740.570.122.02
FC07544.790.372.492.9430.164.4512.960.580.131.57
FC09505.390.382.841.9730.153.039.820.590.131.57
FC11338.780.431.706.1629.678.9522.980.510.102.99
FC14457.410.573.486.6129.7610.1427.850.570.172.31
FC16474.880.432.002.2329.853.2211.970.540.131.58
FC18263.640.911.535.3829.484.8528.820.460.102.34
FC20393.220.642.262.3429.122.4514.030.540.322.95
FC22655.350.282.361.7729.433.659.380.490.191.90
FC24295.590.981.3410.6629.169.4858.370.420.101.67
FC26551.380.413.462.9830.364.0313.070.630.120.99
FC28747.270.332.781.7630.322.9711.210.610.151.37
FC30637.120.342.791.4030.312.319.330.590.160.87
FC32598.350.362.991.3530.162.318.290.580.161.43
FC34462.930.862.656.3630.187.3633.620.590.151.65
FC36743.530.472.342.6430.043.7413.010.570.121.78
FC38850.080.332.581.1530.042.148.240.570.161.71
FC40499.430.392.411.2730.031.867.510.570.181.36
FC42439.830.332.691.6329.522.819.140.520.211.50
平均值476.690.512.473.3129.914.2616.980.560.151.74

注:T-ALK为正构烷烃总量;CPI1=(C15+C17+C19+C21)/(C14+C16+C18+C20);CPI2=(C27+C29+C31+C33)/(C28+C30+C32+C34);∑T/∑M =(∑C25-35)/(∑C15-21);ACL=(∑[Ci]×i)/∑[Ci],Ci为第i个碳原子对应的正构烷烃总量; TAR=(C27+C29+C31)/(C15+C17+C19); AI=C31/(C29+C31);Pmar-aq=(C23+C25)/(C23+C25+C27+C29+C31)。

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利用碳优势指数CPI值可以判断烷烃的来源,其中CPI1可以用来判断正构烷烃前峰链群的浮游生物源和石油源烷烃,当CPI1≤1时,主要来源于石油烃;大于1时,则主要来源于浮游植物。而CPI2则代表后峰链群受陆源高等植物源输入的影响程度[24-25]。防城港海域沉积物中CPI1值均小于1,平均值为0.51,说明研究区正构烷烃前峰链群主要来源于石油烃;CPI2值范围1.34~3.48,平均值2.47,表明受陆源物质影响较大。

利用∑T/∑M值和TAR值可以消除沉积速率和粒度等的影响,更为准确地判断沉积物中烷烃的来源及陆源、海源烷烃的相对贡献[8,26]。防城港海域∑T/∑M比值范围为1.15~10.66,平均值为3.31,指示受陆源输入影响明显;TAR值范围为1.86~10.14,平均值为4.26,表明研究海域沉积物中的正构烷烃主要来自于陆源高等植物的碎片。二者空间分布如图5所示,高值区均近似SN向分布在白龙半岛南部海域,该高值区位于防城江入海河口沉积区及防城港航道区域,研究区海域潮流基本上为与航道一致的往复流[11],且落潮最大流速可达0.9 m/s,这就导致陆源物质经防城江入海后部分沉积,部分随潮流向南迁移。

图5

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图5   表层沉积物∑T/∑M、TAR空间分布

Fig.5   Spatial distribution of surface sediment ΣT/ΣM and TAR


正构烷烃指标Pmar-aq可以区分植物源的种类,当Pmar-aq值在0.01~0.25时指示陆源植物输入,浮水植物输入指数为0.4~0.5,海洋大型植物的输入值大于0.6 [9]。研究海域所有站位Pmar-aq值均小于0.25,说明其植物源较为统一,均为陆源植物来源。平均链长(ACL)和烷烃指数(AI)可以用来指示陆域来源沉积母质植物的类型和种类[10],前人研究表明木本植物正构烷烃以n-C29含量最高,草本植物则以n-C31为主峰,可根据ACL值来判断输入源,研究区ACL变化范围在29.12~30.36,平均值为29.91,说明研究区陆源输入植物以草本植物为主;利用烷烃指数(AI)可进一步确定陆源输入植物类型,当AI小于0.5时表明陆源沉积中的正构烷烃主要来自于木本植物,大于0.5则为草本植物,研究区AI值范围在0.42~0.63,平均值为0.52,进一步表明区内陆源输入主要为草本植物。

n-C16常在受石油污染海域出现,前人研究常用T-ALK/C16比值来判断沉积物是否受到石油污染,比值<30说明受到石油污染,>50则未受到石油污染[27]。本次研究中各站位均有n-C16检出,且n-C16多为前峰链群的优势组分,除FC24和FC34站位外,其他站位T-ALK/C16比值均小于30,研究区平均值为16.98,远小于30,推测研究海域普遍受到石油污染。结合研究海域位置来看,研究区位于防城港港口南部的航道和锚地处,受港口贸易行船的影响较大,石油污染可能与之有关。

前人研究表明姥鲛烷是氧化环境产物,植烷是还原环境产物,因此可利用姥鲛烷Pr和植烷Ph的比值来判断沉积物所处的氧化还原环境[28]。Pr/Ph比值高(>1)指示正构烷烃形成于氧化环境,反之则为还原环境,当其值接近于1时说明沉积区形成于氧化与缺氧条件交替出现时期[29-30]。研究区仅有FC26和FC30站位Pr/Ph比值小于1,其他站位均值为1.83,指示防城港海域沉积环境为氧化环境。

3 结论

1)防城港海域表层沉积物正构烷烃碳数范围为n-C14~n-C35,浓度范围为(67.51~850.08)×10-9,平均值为476.69×10-9。各站位峰型相似,均呈双峰型分布,前峰以n-C14、n-C16、n-C18为主峰,偶碳数优势;后峰以n-C29、n-C31、n-C33为主峰,奇碳数优势。后峰群含量高于前峰群,指示了陆源高于海源。

2)沉积物中正构烷烃的碳数奇偶优势指数特征参数比值∑T/∑M和ACL均指示研究区正构烷烃以陆源植物输入为主;特征参数比值TAR、Pmar-aq和AI均表明其主要源于陆源非浮水草本植物。

3)通过T-ALK/C16比值并结合研究区位置推测研究海域受到石油污染影响;Pr/Ph比值表明研究海域沉积物中正构烷烃形成于氧化环境。

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