Identification of Pb sources in Yellow Sea sediments using stable Pb isotope ratios

Rapid economic developments in East Asian countries have inevitably resulted in environmental degradation in the surrounding seas, and concern for both the environment and protection from pollutants is increasing. Identification of sources of contaminants is essential to environmental pollution management. In this study, the provenance of anthropogenic lead (Pb), a major pollutant of Yellow Sea sediments, was determined for river mouth sediments, including those of the Changjiang, Huanghe, Han, and Geum Rivers, and for age-determined shelf core sediments through the measurement of Pb isotope ratios in the HCl-leached fraction using multi-collector inductively coupled plasma-mass spectrometry (MC ICP/MS). Anthropogenic Pb has accumulated in shelf core sediments since 1910, and its isotope ratios were estimated as 0.863–0.866 and 2.119–2.125 for ²⁰⁷Pb/²⁰⁶Pb and ²⁰⁸Pb/²⁰⁶Pb, respectively, from the mixing relationships of the two endmembers. River mouth sediments exhibited enough distinction in anthropogenic Pb isotope ratios to be discriminated: 0.874 (2.144) in the Huanghe, 0.856 (2.129) in the Han, 0.857 (2.122) in the Geum, and 0.854 (2.101) in the Changjiang for ²⁰⁷Pb/²⁰⁶Pb (²⁰⁸Pb/²⁰⁶Pb), respectively. Although isotope ratios of geogenic Pb in sediments dating before 1910 showed narrow ranges (0.842–0.845 and 2.088–2.100 for ²⁰⁷Pb/²⁰⁶Pb and ²⁰⁸Pb/²⁰⁶Pb, respectively), distinct isotope ratios in each core permitted source identification of sediments in the Yellow Sea based on geographic locations and the geogenic Pb of each river. By comparing the isotope ratios of the estimated anthropogenic Pb to source-related materials, the provenances of anthropogenic Pb in Chinese river sediments were presumed to be Chinese coal or ore, which is also a major source of atmospheric particulate Pb. The anthropogenic Pb in the shelf core sediments in the northern Yellow Sea originated from northern Chinese cities such as Beijing and Tianjin through atmospheric pathways. Pb isotope ratios indicated that Pb in Korean river sediments was characteristic of local Korean ores.     

辽宁省黄海沿岸人工岸线潮间带大型海藻调查与分析研究

为调查辽宁省黄海沿岸人工岸线上潮间带大型海藻多样性情况, 于2011 年10 月至2012 年6 月在大连湾、獐子岛、旅顺及丹东进行采样, 并与其附近天然岸线上海藻进行对比。调查结果显示, 在人工岸线上共发现17 种海藻, 以红藻与绿藻为主, 其中11 种可在相邻天然岸线发现。海藻多样性天然岸线＞混合岸线＞人工岸线, 但人工岸线上绿藻种类与天然岸线上的基本相同。在大连湾及獐子岛地区, 无机氮低的海域, 海藻多样性高; pH 高的海域, 海藻多样性高。调查中发现有人工岸线与天然岸线共存的混合岸线, 此岸线可看作是生境岸线(living shoreline)的一个变形, 为生物保护及生态恢复提供了新思路。     

北部湾白龙半岛邻近海域沉积物中放射性核素含量水平

2016年在北部湾白龙半岛邻近海域采集了表层沉积物,用高纯锗γ能谱仪测量了沉积物中放射性核素的活度.沉积物中40K、210Pb、226Ra、228Th、228Ra、238U和137Cs比活度分别为354±125、89.2±41.2、32.40±9.38、49.2±14.7、42.8±12.6、48.3±20.2和0.74±0.33 Bq/kg.白龙半岛邻近海域沉积物238U、232Th、226Ra含量水平与我国其他近岸海域的含量水平接近,40K、137Cs含量低于我国其他近岸海域的含量.由沉积物放射性核素活度计算的平均γ辐射吸收剂量(D)和平均年有效剂量当量(AEDE)都与世界平均水平相当,镭当量比活度(Raeq)远低于UNSCEAR建议的最低限值.     

Anthropogenic Pb in settling particulate matter in the Northwestern Pacific examined using stable isotopes of Pb

We have investigated Pb concentrations and isotopic compositions in settling particles collected by sediment traps experiments over a period of two years, from May 2005 to April 2007, at two depths, 770 and 5100 m, at station KNOT in the Northwestern Pacific Ocean (44°N, 155°E). To the identify provenances of Pb, the samples were separated into two fractions by chemical leaching techniques, with the leachate expected to contain Pb of anthropogenic origin. Isotopic compositions of Pb and concentrations of Pb, Sc, Mn, La, Yb, and Th were measured by quadrupole ICP-MS. The isotope ratios of leachable Pb in settling particles were ²⁰⁷Pb/²⁰⁶Pb = 0.860 ± 0.001; ²⁰⁸Pb/²⁰⁶Pb = 2.116 ± 0.002 (mean ± 95% confidence intervals), which are similar to those of aerosols in China that are greatly affected by pollution from coal combustion. We estimated the mean contribution from anthropogenic Pb sources to the Pb in settling particles, using the conventional binary (anthropogenic and natural Pb) mixing equation for Pb isotopes, as 90% in the upper trap and 78% in the lower trap. Furthermore, we found a significant negative correlation between the isotope ratios of Pb and concentrations of leachable Mn, normalized to those of leachable Pb, suggesting that manganese oxides play an important role in transporting Pb from the upper layers of the ocean to the deeper layers. Our results support the speculation published in a previous study that Pb might be scavenged by Mn oxides in the Northwestern Pacific Ocean.     

黄海表层沉积物的矿物组成特征及其物源分析

以黄海66个表层沉积物为研究对象,通过粒度、黏土矿物和碎屑矿物分析,研究了黄海表层沉积物的粒度分布与矿物组成特征,探讨了研究区沉积物的矿物组成特征对其物源、沉积环境的指示意义。黄海表层沉积物平均粒径为5.2Φ,分选较差;黏土矿物组合类型为伊利石-高岭石-蒙脱石-绿泥石,其中伊利石的含量最高,蒙脱石的含量最低;碎屑矿物（粒径为0.063～0.125 mm）平均含量为8.07%,标准偏差为4.03,分布趋势与平均粒径分布基本一致,轻矿物以石英和长石为主;重矿物以角闪石和绿帘石为主,其次是不透明矿物和片状矿物,重矿物主要集中分布于黄海南部。物源识别结果表明：黄海的东北部海域接受鸭绿江沉积物的供应;黄海北部主要为黄河源沉积物;南黄海西部沉积物主要为黄海沿岸流南下带来的现代黄河物质和再悬浮的老黄河沉积物;南黄海中部沉积物来源复杂以黄河沉积物为主,长江沉积物的供应较少。     

南黄海苏北近岸西洋水道水沙输运机制分析

基于2008 年3 月份在南黄海辐射沙脊群西洋水道内5 个站位大潮期间的观测数据（包括流速与悬沙质量浓度的垂向剖面）, 利用机制分解法计算了西洋水道内的水与悬沙通量。结果表明, 水体在多数时段内均处于分层向混合过渡的状态, 中下层水体的理查德森数（Ri）与瞬时悬沙输运量中的平均流输沙项及流速的潮周期变化相关项之间存在显...     

山东半岛北部滨浅海区表层沉积物铝物源鉴别

Surface sediment samples in the near shore area of the north Shandong Peninsula are collected for grain size and element analyses. The results indicate that the surface sediments in the study area are primarily composed of the silt-sized components similar to the Huanghe River. The total concentration of aluminum varies from 5.57% to7.37%(average(6.33 ± 0.40)%), and its spatial distribution is mainly controlled by the grain size. Correlations between the ratio of aluminum to titanium concentration and aluminum concentration, titanium concentration and the mean grain size indicate that aluminum in the near shore surface sediments is affected majorly by the terrigenous source, and partially by the anthropogenic source. The ratios of aluminum to titanium concentrations are larger than the background value of loess matter at some stations due to the existence of excess aluminum associated with human activities. Thus, the sources of aluminum should be identified firstly when aluminum is used as an index of terrigenous matter even in the near shore area dominated by terrigenous deposits.     

北黄海表层沉积物中甲藻孢囊的分布特征

2009年和2010年采集北黄海15个站位的表层沉积物样品进行甲藻孢囊分析,共鉴定出甲藻孢囊28种(隶属13个属)和2种未定种,优势种为膝沟藻(Gonyaulax spp.)、塔马/链状亚历山大藻(Alexandriumcatenella/tamarense)和微小/相似亚历山大藻(Alexandrium minutu...     

Sulfur and iron speciation in surface sediments along the northwestern margin of the Black Sea

The speciation of sedimentary sulfur (pyrite, acid volatile sulfides (AVS), S⁰, H₂S, and sulfate) was analyzed in surface sediments recovered at different water depths from the northwestern margin of the Black Sea. Additionally, dissolved and dithionite-extractable iron were quantified, and the sulfur isotope ratios in pyrite were measured. Sulfur and iron cycling in surface sediments of the northwestern part of the Black Sea is largely influenced by (1) organic matter supply to the sediment, (2) availability of reactive iron compounds and (3) oxygen concentrations in the bottom waters. Biologically active, accumulating sediments just in front of the river deltas were characterized by high AVS contents and a fast depletion of sulfate concentration with depth, most likely due to high sulfate reduction rates (SRR). The δ³⁴S values of pyrite in these sediments were relatively heavy (−8‰ to −21‰ vs. V-CDT). On the central shelf, where benthic mineralization rates are lower, re-oxidation processes may become more important and result in pyrite extremely depleted in δ³⁴S (−39‰ to −46‰ vs. V-CDT). A high variability in δ³⁴S values of pyrite in sediments from the shelf-edge (−6‰ to −46‰ vs. V-CDT) reflects characteristic fluctuations in the oxygen concentrations of bottom waters or varying sediment accumulation rates. During periods of oxic conditions or low sediment accumulation rates, re-oxidation processes became important resulting in low AVS concentrations and light δ³⁴S values. Anoxic conditions in the bottom waters overlying shelf-edge sediments or periods of high accumulation rates are reflected in enhanced AVS contents and heavier sulfur isotope values. The sulfur and iron contents and the light and uniform pyrite isotopic composition (−37‰ to −39‰ vs. V-CDT) of sediments in the permanently anoxic deep sea (1494 m water depth) reflect the formation of pyrite in the upper part of the sulfidic water column and the anoxic surface sediment. The present study demonstrates that pyrite, which is extremely depleted in ³⁴S, can be found in the Black Sea surface sediments that are positioned both above and below the chemocline, despite differences in biogeochemical and microbial controlling factors.     

天然海藻场沿岸表层沉积物有机质的分布特征与来源

海藻场是生物多样性最高的生态系统之一, 其内部的沉积物有机质是支撑海藻场生物多样性的重要物质基础之一。本研究以浙江省嵊山岛北部无人村沿岸的天然海藻场为研究对象, 在大型海藻凋落期6~8月采集沉积物和端元生物样本, 分析了沉积物样本的粒径组成、总有机碳 (TOC)、总氮(TN)、碳氮比值(C/N)和碳氮稳定同位素(δ¹³C和δ¹⁵N), 通过贝叶斯稳定同位素混合模型评估了沉积物有机质的来源及变化规律。结果显示, 1)海藻场沿岸沉积物中粉砂占比最大, 砂的占比最低, 沉积物类型为黏土质粉砂; 2)沉积物TOC、TN、C/N、δ¹³C和δ¹⁵N范围分别为0.70%~2.41%、0.11%~0.41%、5.53~6.48、–21.79‰~–19.60‰和1.56‰~4.26‰, 在空间分布上, TOC与TN含量均随离岸距离增加而下降; 3)沉积物粒径组成、C/N比值、δ¹³C和δ¹⁵N之间的关系显示沉积物有机质主要来源于大型海藻和浮游植物的混合贡献; 4)根据贝叶斯同位素混合模型计算结果显示, 大型海藻对沉积物有机质贡献率在2.30%~45.60%, 在空间分布上, 大型海藻对沉积物有机质的贡献率随离岸距离增加而下降; 5)海藻碎屑产生量和沉积物有机碳沉积量评估结果显示, 大型海藻产生的碎屑有机质中有11.98%进入海藻场及沿岸海域的表层沉积物中。本研究为评估海藻场碎屑的产生规模和时空分布, 以及渔业资源养护功能提供了数据支撑。     

冬季黄、东海一断面表层砂壳纤毛虫群落

于2012年11月18日至12月21日,在黄、东海沿从南向北(26~36°N)一个断面24个站采样调查了表层(4 m)砂壳纤毛虫群落。共发现砂壳纤毛虫17属,32种。各站砂壳纤毛虫种丰富度为2~15种,砂壳纤毛虫总丰度为2 478~88 550个/m3。整个断面优势种为筒状拟铃虫、白领细壳虫、小领细壳虫和钝囊坎虫。巴西拟铃虫仅出现在青岛近岸(24号站),但丰度很高(10 960个/m3)。砂壳纤毛虫种类多样性从南向北降低,从近岸向远岸增加,黏着壳的比例在近岸水浅处较多,在水深大于50 m的站位,透明壳所占比例大大增加。不同种类的砂壳纤毛虫有着不同的分布区域,根据分布区域的不同,可分为南方种,北方种和广布种等。聚类分析结果显示,调查区的砂壳纤毛虫可以分为3个群落。     

福建沿海下更新统的磁性地层学研究

通过对下更新统海湾相的“镇海组”（Q1^m？）建组剖面--福建龙海市关头剖面进行古地磁测量，配合K-Ar法测年、粒度、矿物和孢粉等分析资料，确认该剖面中部的灰绿色粘土粉砂质砂层属于早更新世，其沉积相应为冲-洪积相，仍沿用“镇海组”（Q1^al pl）之名。研究表明第四纪下界存在于该剖面的灰绿色粘土粉砂质砂层与红褐色粉砂粘土质砂层之间（即M/G面上）。这是福建首次用年代地层学手段发现的第四纪下界。     

Distribution of dinoflagellate cysts in Yellow Sea sediments

To investigate the distribution,abundance,and species composition of dinoflagellate cysts in the Yellow Sea,surface sediment samples were collected at 37 sites,including the Korean dump site.Twenty-one dinoflagellate cyst taxa were identified,with the assemblages dominated mainly by Spiniferites bulloideus,Operculodinium centrocarpum,and cyst of Alexandrium catenella/tamarense type.A high frequency of O.centrocarpum in the Yellow Sea was observed for the first time,and it is likely that this can be attributed to the dynamics of the Yellow Sea Cold Water Mass and the Changjiang(Yangtze) River runoff.Total cyst concentrations ranged from 23 to 48 442 cysts/g dry weight,and high cyst concentrations were recorded adjacent to the dumping site.This result suggests that anthropogenic activities such as ocean dumping stimulate the growth of dinoflagellates in the Yellow Sea,which in turn leads to high levels of dinoflagellate cyst production.     

Relationships between the sound speed ratio and physical properties of surface sediments in the South Yellow Sea

Building empirical equations is an effective way to link the acoustic and physical properties of sediments. These equations play an important role in the prediction of sediments sound speeds required in underwater acoustics.Although many empirical equations coupling acoustic and physical properties have been developed over the past few decades, further confirmation of their applicability by obtaining large amounts of data, especially for equations based on in situ acoustic measurement techniques, is required. A sediment acoustic survey in the South Yellow Sea from 2009 to 2010 revealed statistical relationships between the in situ sound speed and sediment physical properties. To improve the comparability of these relationships with existing empirical equations, the present study calculated the ratio of the in situ sediment sound speed to the bottom seawater sound speed, and established the relationships between the sound speed ratio and the mean grain size, density and porosity of the sediment. The sound speed of seawater at in situ measurement stations was calculated using a perennially averaged seawater sound speed map by an interpolation method. Moreover, empirical relations between the index of impedance and the sound speed and the physical properties were established. The results confirmed that the existing empirical equations between the in situ sound speed ratio and the density and porosity have general suitability for application. This study also considered that a multiple-parameter equation coupling the sound speed ratio to both the porosity and the mean grain size may be more useful for predicting the sound speed than an equation coupling the sound speed ratio to the mean grain size.     

砷在贝类养殖区表层沉积物及贝类体中的积累和分布

2003—2004年福建近岸海域海洋环境和海洋生物质量的监测资料表明,福建沿海主要贝类养殖区表层沉积物和4种养殖贝类(僧帽牡蛎、太平洋牡蛎、缢蛏和泥蚶)体中砷含量分别为(4.15—13.7)×10-6(干重)和(1.28—3.56)×10-6(湿重),总平均值分别为9.06×10-6(干重)和2.22×10-6(湿重),均低于海洋环境污染评价标准限值。总体上看,福建沿海潮间带滩涂贝类养殖区表层沉积物和养殖贝类体中砷含量高于浅海贝类养殖区的含量,且呈闽东和闽南贝类养殖区高、闽中养殖区低的格局。贝类养殖区表层沉积物中砷含量的多寡与表层沉积物的类型密切相关,并与僧帽牡蛎、缢蛏体砷含量之间总体成正相关。     

黄东海表层沉积物中磷的赋存形态和分布特征及其对生态系统的潜在影响

For better understanding the phosphorus(P) cycle and its impacts on one of the most important fishing grounds and pressures on the marine ecosystem in the Yellow Sea(YS) and East China Sea(ECS), it is essential to distinguish the contents of different P speciation in sediments and have the knowledge of its distribution and bioavailability. In this study, the modified SEDEX procedure was employed to quantify the different forms of P in sediments. The contents of phosphorus fractions in surface sediments were 0.20–0.89 μmol/g for exchangeable-P(Exch-P), 0.37–2.86 μmol/g for Fe-bound P(Fe-P), 0.61–3.07 μmol/g for authigenic Ca-P(ACa-P), 6.39–13.73μmol/g for detrital-P(DAP) and 0.54–10.06 μmol/g for organic P(OP). The distribution of Exch-P, Fe-P and OP seemed to be similar. The concentrations of Exch-P, Fe-P and OP were slightly higher in the Yellow Sea than that in the East China Sea, and low concentrations could be observed in the middle part of the ECS and southwest off Cheju Island. The distribution of ACa-P was different from those of Exch-P, Fe-P and OP. DAP was the major fraction of sedimentary P in the research region. The sum of Exch-P, Fe-P and OP may be thought to be potentially bioavailable P in the research region. The percentage of bioavailable P in TP ranged from 13% to 61%. Bioavailable P burial flux that appeared regional differences was affected by sedimentation rates, porosity and bioavailable P content, and the distribution of bioavailable P burial flux were almost the same as that of TP burial flux.     

黄东海沉积物中的还原无机硫

Cold diffusion methods are used to separate and quantify the three reduced inorganic sulfur species into acid volatile sulfide(AVS), pyrite–S and element sulfur(ES) in the sediments of the Yellow and East China Seas. The results show that up to 25.02 μmol/g of AVS, 113.1 μmol/g of pyrite–S and 44.4 μmol/g of ES are observed in the sediments of the Yellow Sea and East China Sea. Pyrite–S is the predominant sulfide mineral in the sediments, while the concentration of AVS is quite low at most stations in the study area. The amounts and reactivity of organic matter are the primary limited factor for the sulfide formation, while an iron limitation and a sulfate limitation are not observed in the sediments of the Yellow Sea and East China Sea. The irregular profiles of the three reduced inorganic sulfur species also reflected the comprehensive influence of sediment composition and sedimentation rates.     

Sea level rise along China coast in the last 60 years

Based on long-term tide gauge observations in the last 60 years, the temporal and spatial variation characteristics of sea level change along the coast of China are analyzed. The results indicate that the sea level along the coast of China has been rising at an increasing rate, with an estimated acceleration of 0.07 mm/a2. The rise rates were 2.4 mm/a, 3.4 mm/a and 3.9 mm/a during 1960–2020, 1980–2020 and 1993–2020, respectively. In the last 40 years, the coastal sea level has risen fastest in the South China Sea and slowest in the Yellow Sea. Seasonal sea levels all show an upward trend but rise faster in winter and spring and slower in autumn. Sea level change along the coast of China has significant periodic oscillations of quasi-2 a, 4 a, 7 a, 11 a, quasi-19 a and 30–50 a, among which the 2–3 a, 11 a, and 30–50 a signals are most remarkable, and the amplitude is approximately 1–2 cm. The coastal sea level in the most recent decade reached its highest value in the last 60 years. The decadal sea level from 2010 to 2019 was approximately 133 mm higher than the average of 1960–1969. Empirical orthogonal function analysis indicates that China’s coastal sea level has been changing in a north-south anti-phase pattern, with Pingtan and Fujian as the demarcation areas. This difference was especially obvious during 1980–1983, 1995–1997 and 2011–2013. The coastal sea level was the highest in 2016, and this extreme sea level event was analyzed to be related mainly to the anomalous wind field and ENSO.     

南海北部沿岸海域潮汐的调和分析

采用t_tide潮汐分析工具对南海北部的5个验潮站2009年全年的逐时潮高资料进行调和分析,计算出各站的调和常数,评估调和常数的准确性、稳定性,并总结了广东沿岸海域潮汐特征.利用对2009年逐时潮高的调和分析结果对2010年全年的潮高进行预测,将各站预测结果与同时间的实测数据进行全年和分季节进行比较,对预测结果与实测数据的残差进行统计分析.通过对残差的散点分布、概率分布、置信区间等统计结果进行分析,检验预测结果的准确性、稳定性和可靠性.结果表明：广东沿岸海域潮汐是以M2分潮为主,K1、O1、S2为次结合的潮汐机制,采用t_tide潮汐分析工具对南海北部潮高的预测结果与实测数据拟合较好,相位预测准确,潮高预测除在时间序列尾部（年尾）有些许较大的误差外,t_tide工具在南海北部潮汐预报中具有较高的准确性和稳定性.预测残差的整体服从正态分布,残差均值小于10-2m量级,方差最大为0.229 4,最小为0.173 2,95%置信区间长度小于10-2.各站季节分析主要分潮的离散度小于0.04的结果充分证明不同季节的分析区别不明显,3个月资料与整年资料的调和分析结果几乎一致,与所选取的季节资料几乎无关.虽然在预测值中,有极个别的残差将近1 m,但并不足以影响到预测的准确性.     

冬、夏季渤黄海表层沉积物粒度特征差异及其成因分析

对渤海、黄海海域冬、夏两季表层沉积物取样,通过激光粒度仪得出粒度参数,进而分析讨论冬季强的沿岸流的作用、黄海暖流、夏季冷水团的影响以及地形、海底地貌特征、物源特征等对表层沉积物分布造成的影响。结果表明,冬、夏两季渤黄海表层沉积物粒度特征总体上相差不大,但部分海域如渤海中北部、渤海中南部、北黄海西北部近渤海海峡北部海域、山东半岛东北部海域、南黄海中部沉积物粒度特征存在明显季节性差异。表层沉积物粒度特征季节性差异与地形地貌、沿岸流、黄海暖流、黄海冷水团及物源密切相关。本研究对于探讨渤黄海不同季节表层沉积物沉积特征的影响机制、了解渤黄海区海洋动力过程的季节差异有积极意义。