226Ra and 228Ra in the mixing zones of the Pee Dee River-Winyah Bay,Yangtze River and Delaware Bay Estuaries

²²⁶Ra and ²²⁸Ra have non-conservative excess concentrations in the mixing zones of the Pee Dee River-Winyah Bay estuary, the Yangtze River estuary, and the Delaware Bay estuary. Laboratory experiments, using Pee Dee River sediment, indicate desorption of ²²⁶Ra to increase with increasing salinities up to 20‰. In Winyah Bay desorption from river-borne sediments could contribute almost all of the increases for both isotopes. Desorption adds only a portion of the excess ²²⁸Ra measured in the Yangtse River and adjacent Shelf waters and Delaware Bay. In the Yangtze River the mixing zone extends over a considerable portion of the Continental Shelf where ²²⁸Ra is added to the water column by diffusion from bottom sediments, while ²²⁶Ra concentrations decrease from dilution. Diffusion of ²²⁸Ra from bottom sediments in Delaware Bay primarily occurs in the upper part of the bay (< 22‰ water) where fine grained sediments predominate. A diffusive flux for ²²⁸Ra of 0·33 dpm cm^?2 year was determined for Delaware Bay.     

Ra and Ra in the mixing zones of the Pee Dee River-Winyah Bay, Yangtze River and Delaware Bay Estuaries

²²⁶Ra and ²²⁸Ra have non-conservative excess concentrations in the mixing zones of the Pee Dee River-Winyah Bay estuary, the Yangtze River estuary, and the Delaware Bay estuary. Laboratory experiments, using Pee Dee River sediment, indicate desorption of ²²⁶Ra to increase with increasing salinities up to 20‰. In Winyah Bay desorption from river-borne sediments could contribute almost all of the increases for both isotopes. Desorption adds only a portion of the excess ²²⁸Ra measured in the Yangtse River and adjacent Shelf waters and Delaware Bay. In the Yangtze River the mixing zone extends over a considerable portion of the Continental Shelf where ²²⁸Ra is added to the water column by diffusion from bottom sediments, while ²²⁶Ra concentrations decrease from dilution. Diffusion of ²²⁸Ra from bottom sediments in Delaware Bay primarily occurs in the upper part of the bay (< 22‰ water) where fine grained sediments predominate. A diffusive flux for ²²⁸Ra of 0·33 dpm cm⁻² year was determined for Delaware Bay.     

核电站周边海域鱼类与表层沉积物中的放射性水平调查

为科学评价核电站对周边海域生态环境的影响,文章选取4座我国沿海已运营的核电站即田湾核电站、秦山核电站、宁德核电站和福清核电站为研究对象,分别于2016年6-9月和2017年4-7月调查其周边海域鱼类和表层沉积物中主要放射性核素的比活度,并分析表层沉积物的来源。研究结果表明：核电站的运营未对周边海域鱼类和表层沉积物中的放...     

Factors controlling excess radium in the Nakdong River estuary,Korea: submarine groundwater discharge versus desorption from riverine particles

The activities of naturally occurring radium isotopes (²²⁶Ra and ²²⁸Ra) in estuarine water were measured downstream of the dam constructed in the Nakdong River, Korea. The sampling of surface waters for radium, silicate, and suspended solid (SS) analyses was conducted at 18 stations during three periods (July 1997, April 1998, and June 1999). In general, radium activities exceeded the value expected from the mixing of two freshwater and seawater endmembers. We characterized the responses of Ra and Si according to three different conditions: (1) when the freshwater discharge and the water level of the dam relative to the sea level at low tide were lower (April 1998), the excess Ra and Si contents were lower in the estuary; (2) when the fresh water discharge was larger following heavy precipitation (July 1997), both excess Ra and Si contents were higher in the estuary with conservative mixing of Si; and (3) when the water level of the dam relative to the sea level at low tide was highest under low freshwater discharge (June 1999), high excess Ra but low Si levels were observed. The occurrence of high Ra activity in June 1999 was likely due to the large submarine brackish groundwater discharge downstream of the estuary. Since brackish groundwater in general contains high concentrations of nutrients, Ba, Ra, etc, our result suggests an important role for the submarine groundwater discharge on the biogeochemistry of estuarine/coastal waters, especially when the water level of the dam (hydraulic head) is high.     

A study on the distribution of 210Pb, 226Ra and total β radioactivity in estuary sediments

Determination on the content variation of 210Pb, 226Ra and total β radioactivity in estuary sediments of the Jiulongjiang River and the Changjiang River were made to study distributions of natural radioactive substances in the areas studied. Sources of radioactive substances were determined, and the transportation of bottom waters and sediments in the areas was searched according to the distributions.     

黄河下游及河口区表层沉积物中U,Ra,Th,40K和137Cs的测定

本文从地球化学和环境保护的角度,用8180—4Kγ谱仪直接测定方法确定了天然放射性元素U,Ra,Th,~(40)K,及人工核素~(137)Cs的含量,讨论了它们的分布特点及其影响因素,指出了河口区与下游段元素变化的差异及其制约条件。     

应用镭-226解读南极普里兹湾表层水的来源与运移

中国第22次南极科学考察航次(2005年12月至2006年1月)期间,利用Mn-纤维富集大体积表层海水中的Ra同位素,并通过222Rn直接射气法测量226Ra的比活度,结果表明,普里兹湾表层水的226Ra比活度变化为0.92~2.09 Bq/m3,平均值为1.61 Bq/m3,在深海区域表现出226Ra含量高的特征。从空间分布看,表层水226Ra比活度呈现出由湾内向湾外增加的反常态势,反映出不同Ra含量水团的混合影响2。26Ra比活度与盐度的关系证实研究海域表层水的Ra含量主要受三种端元水体的混合所控制:其一为具有镭含量高、盐度高特征的南极夏季表层水;其二为低镭、低盐特征的冰融水;其三为高盐、中等镭含量的普里兹湾中深层水,该水体的226Ra纯粹由海底沉积物间隙水向上扩散所维持。结合S-226Ra示踪体系及上述三端元混合模型,计算出各组成水体的比例并描绘出它们的空间分布。南极夏季表层水的份额由湾外向湾内逐渐降低,并且在68°E断面向南影响范围较大;冰融水的比例由湾内向湾外降低,并且在湾内东部的高温水体中具有最大贡献;普里兹湾中深层水中受沉积物镭来源影响比较显著的区域出现在湾内西北部,其影响向湾外逐渐降低。冰融水与普里兹湾中深层水份额分别于普里兹湾湾顶东、西部出现高值的分布特征证实埃默里冰架前沿海流东进、西出的运移规律。     

鸭绿江河口地区沉积物的粒度变化及影响因素

通过对比鸭绿江河口不同地区柱状样的粒度参数及敏感组分变化规律,分析了河口不同地区沉积动力环境和沉积特征的差异;结合代表性柱状样的210Pb测年,分析了柱状样在不同时期自然和人类活动影响下的沉积特征变化。结果表明,西水道主要受潮流作用而含有泥沙互层,粒度参数变化小;西岸潮滩受潮流和波浪作用含有贝壳碎屑,并在顶部出现粗化层。近几十年来,鸭绿江河口地区沉积特征的变化主要由于人类活动对水沙入海通量的影响:1941年以前柱状样的波动沉积特征反映了河流山溪性特征;1941—1970(1980)年随水沙入海通量减少而呈现砂含量降低、粉砂增加的特征;1970(1980)—1990年由于水沙入海通量变化较小,而呈现沉积物组成和敏感组分保持稳定的特征;但1990年后随水沙入海通量的进一步降低,邻近河口区域的沉积物出现明显的粗化。     

Geochemical cycling in the Hooghly estuary, India

U–Th decay series isotopes, δ¹⁸O and Si measurements in the river estuarine waters and sediments of the polluted Hooghly estuary as well as the surface waters of the Bay of Bengal, its high salinity end member, are reported. Dissolved Si indicates that there are probably two mixing regimes, dissolved U behaviour is nonconservative and δ¹⁸O behaves conservatively in the overall estuarine region. Isotopes of reactive elements, viz. ²³⁴Th and ²¹⁰Po, are removed from the estuarine waters in <2 days and <1 month, respectively, which is due to high suspended matter (30–301 mg l⁻¹). ²²⁸Ra and ²²⁶Ra are profusely released into the estuarine waters in the low to mid-salinity regions.As expected, the opposite trend is observed in the case of estuarine sediments and suspended matter. Reactive isotopes of Th, ²¹⁰Pb and ²¹⁰Po are enriched, whereas Ra isotopes are depleted with respect to their parent nuclides in the estuarine sediments and suspended matter. ²³²Th/Al ratio appears well suited to study the distribution and mixing of the bed load sediments of the Ganga–Brahmaputra (G–B) and the Hooghly rivers with those from other rivers on the Bay of Bengal floor.     

钦州湾河流沉积物中镭的解吸行为

放射性镭同位素在海底地下水排放（SGD）等海洋物质变化过程的研究中具有优良的示踪作用，估算SGD通量时需要计算河流悬浮颗粒物的解吸通量。因此，对河流沉积物/悬浮颗粒物中镭同位素解吸行为的研究不可或缺，而目前对于粒度较小范围内镭同位素的解吸特征及其机理的研究依然不足。本文选用钦州湾河流沉积物，通过室内实验探究粒度和盐度对沉积物中镭同位素解吸行为的影响。结果表明，在沉积物平均粒径0.9~136.0 μm范围内，随着粒径增大，沉积物中镭同位素在海水（盐度为33.9）中解吸活度逐渐减小，且变化趋势也逐渐变缓，平均粒径大于43.7 μm后，解吸量几乎不变；在海水盐度4.9~33.9范围内，随着盐度增大，沉积物中镭同位素解吸活度逐渐增大，盐度大于24.9后，解吸量趋于不变。本文创新性地建立了沉积物表面分形结构的镭解吸理论模型，拟合得到钦州湾河流沉积物表面最大可交换态224Ra、226Ra和228Ra活度分别为1.13 dpm/g、0.17 dpm/g和0.85 dpm/g，以干重计；沉积物中224Ra、226Ra和228Ra最大解吸比分别为30%、7%和18%。钦州湾河流沉积物颗粒表面最大可交换态224Ra和226Ra活度分别处于全球中等水平和较低水平，而其最大解吸比分别处于全球较高水平和较低水平。本研究结果有助于更好地理解镭同位素的解吸行为，以帮助更准确地估算SGD通量。     

长江口及其邻近陆架沉积物中226Ra和210Pb的分布特征

本文利用放射化学分析法测定了长江口及其邻近陆架沉积物中~(226)Ra和~(210)Pb的含量。结果表明,在该海区的沉积物中,~(226)Ra含量的水平分布随经度增加而直线下降,而~(210)Pb含量的水平分布则随经度增加而直线上升,二者形成明显的同步反向分布。     

盐度对镭同位素在海南红树林沉积物解吸行为的影响

天然放射性镭同位素在沉积物上的解吸行为是影响其在陆-海交换过程中的关键所在。采用沉积物室内解吸实验和现场采集间隙水测量224Ra含量两种方法,对水体盐度梯度控制镭在海南八门湾红树林沉积物的解吸行为进行了讨论。结果表明:沉积物上可交换态224Ra的最大量为0.44dpm/g,解吸比为35%。利用间隙水的224Ra含量确定镭的分配比Kd与水体盐度S呈反比例函数:Kd=8.4×102/S,与室内解吸实验的结果相比更能代表镭在沉积物上的真实解吸行为。在深度25—40cm内,湿地沉积物的224Ra处于与其母体228Th的平衡状态,但223Ra很可能处于相对其母体227Th亏损状态。     

南海东北部表层沉积物天然放射性核素与137Cs

用HPGeγ谱仪测定了南海东北部表层沉积物中的放射性核素.结果给出7种核素的平均比活度分别为40K:538Bq/kg,210Pb:116Bq/kg,226Ra:27.7Bq/kg,228Ra:4.49Bq/kg,228Th:42.0Bq/kg,238U:35.4Bq/kg和137Cs:1.16Bq/kg,210Pb的比活度随离岸距离增大,226Ra比活度随离岸距离没有明显变化,其余核素比活度随离岸距离减小.与对我国近海其他海域报道的沉积物放射性核素含量相比,40K和137Cs稍低于其他海域,其余核素为中等水平.     

北部湾沉积物中放射性核素的分布特征与控制因素

北部湾是我国大西南地区重要的海上通道，也是我国重要的渔场之一。本研究利用高纯锗γ谱仪系统分析北部湾表层和柱状沉积物中4种最主要的天然放射性核素(238U、226Ra、228Ra、40K)含量和分布特征。结果显示，北部湾沉积物中放射性核素含量低于我国大部分海域的结果，高于珊瑚礁区的极低放射性水平的结果。北部湾沉积物中4种核素都存在“蝴蝶”状空间分布特征，该特征主要源于沉积物粒径的非线性调控，且与沉积物总有机碳浓度存在正相关。此外，利用Mn和210Pb所指示的氧化还原状态和物理/生物扰动过程也可以对柱状沉积物中氧化还原敏感型核素(比如，238U)分布产生一定的影响。本文从232Th/238U、40K/238U、226Ra/238U活度比值角度，发现北部湾沉积物具有典型的陆源沉积物特征，且显著不同于南海珊瑚礁区中生源沉积物特征。本研究有利于掌握滨海核电发展背景下的北部湾海洋环境中放射性核素水平，揭示核素的“蝴蝶”状分布特征和控制因素，探索基于放射性核素的地球化学新指标在海洋沉积过程中的应用。     

Seasonal variation in the Ra/Ra ratio of coastal water within the Sea of Japan: Implications for the origin and circulation patterns of the Tsushima Coastal Branch Current

In the current study, low-background γ-spectrometry was employed to determine the ²²⁸Ra/²²⁶Ra activity ratio and ¹³⁷Cs activity of 84 coastal water samples collected at six sites along the main island of Japan (Honshu Island) within the Sea of Japan, including the Tsushima Strait, and two other representative sites on Honshu Island (a Pacific shore and the Tsugaru Strait) at 1-month intervals in 2006.The ²²⁸Ra/²²⁶Ra ratio of coastal waters in the Sea of Japan exhibited similar patterns of seasonal variation, with minimum values during early summer (²²⁸Ra/²²⁶Ra = 0.6–0.8), maximum values during autumn (²²⁸Ra/²²⁶Ra = 1.5–3), and a time lag in their temporal changes ( 2.5 months and over  1300 km distance). However, the 2 other sites represented no clear periodic variation.In contrast to the positive correlation between ¹³⁷Cs activity (0.6–1.7 mBq/L) and salinity (15–35), the ²²⁸Ra/²²⁶Ra ratio of coastal water samples from the Sea of Japan was not observed to correlate with salinity, and the increase in the ²²⁸Ra/²²⁶Ra ratio was not as marked (0.5–1; May–June 2004 and 2005) during the migration along Honshu Island. The input of land-derived water and/or the diffusion of radium from coastal sediments is unlikely to have affected the wide seasonal variation in the ²²⁸Ra/²²⁶Ra ratio observed in these water samples.The seasonal variation in the ²²⁸Ra/²²⁶Ra ratio recorded for the coastal waters of the Sea of Japan is considered to be mainly controlled by the remarkable changes in the mixing ratio of the ²²⁸Ra-poor Kuroshio and the ²²⁸Ra-rich continental shelf waters within the East China Sea (ECS). After passing through the Tsushima Strait, this water mass moves northeast along the coastline of the Sea of Japan as the Tsushima Coastal Branch Current (TCBC).     

大洋表层水中~(226)Ra的分布

采用碳酸盐富集－EDTA纯化－Ba（Ra）SO4制源－α计数法，测定了我国第13,14 次南极科学考察期间，从西太平洋、南大西洋和东印度洋采集的 16个表层水样中的226 Ra比活度。测定结果表明，表层水中溶解态226Ra的比活度范围：西太平洋为 0．46──0．95Bq·m－3，平均值为 0．66Bq·m-3；东印度洋为0．5 6──1．2 7 Bq·m-3，平均值为0．81 Bq·m-3；南大西洋为1．17──1．63Bq·m－3，平均值为 1．45 Bq·m－3。还测定了上述海域 5个表层水样中颗粒态226Ra比活度为0.006──0．030Bq·m－3，颗粒态226Ra很低，只占溶解态的1．0％──2．6％，说明226Ra主要以溶解态形式存在于上述洋区。测定结果还表明，52°S以南离南极较近的测站226Ra比活度较高，特别是 60°Ｓ以南的南大洋海域，226Ra比活度更高，与其他作者的测定结果一致。     

New perspectives on radium behavior within a subterranean estuary

Over the past decade, radium isotopes have been frequently applied as tracers of submarine groundwater discharge (SGD). The unique radium signature of SGD is acquired within the subterranean estuary, a mixing zone between fresh groundwater and seawater in coastal aquifers, yet little is known about what controls Ra cycling in this system. The focus of this study was to examine controls on sediment and groundwater radium activities within permeable aquifer sands (Waquoit Bay, MA, USA) through a combination of field and laboratory studies. In the field, a series of sediment cores and corresponding groundwater profiles were collected for analysis of the four radium isotopes, as well as dissolved and sediment associated manganese, iron, and barium. We found that in addition to greater desorption at increasing salinity, radium was also closely tied to manganese and iron redox cycling within these sediments. A series of laboratory adsorption/desorption experiments helped elucidate the importance of 1) contact time between sediment and water, 2) salinity of water in contact with sediment, 3) redox conditions of water in contact with sediment, and 4) the chemical characteristics of sediment on radium adsorption/desorption. We found that these reactions are rapid (on the order of hours), desorption increases with increasing salinity and decreasing pH, and the presence of Fe and Mn (hydr)oxides on the sediment inhibit the release of radium. These sediments have a large capacity to sorb radium from fresh water. Combined with these experimental results, we present evidence from time series groundwater sampling that within this subterranean estuary there are cyclic periods of Ra accumulation and release controlled by changing salinity and redox conditions.     

High 226Ra and 228Ra activities in Nueces Bay,Texas indicate large submarine saline discharges

We have investigated submarine groundwater discharge to Nueces Bay (Texas) using naturally occurring Ra isotopes. Dissolved Ra activities in Nueces Bay are among the highest observed in coastal estuaries; as great as 2600 dpm m^− 3 for ²²⁸Ra and 1000 dpm m^− 3 for ²²⁶Ra. Using a combination of salt and Ra mass balances, we demonstrate that river discharge and bay bottom sediments cannot supply the Ra needed to balance tidal export. In the case of ²²⁶Ra there is an additional source of 218 × 10⁶ ± 105% dpm day^− 1 which is 9 times the maximum supply from bay bottom sediments and 50 times the Ra supplied by the Nueces River. A groundwater flux of 310,000 m³ day^− 1 is required to supply the needed ²²⁶Ra, based on the measured maximum Ra activity of local groundwater. Though as little as 10% of this flux may be advecting terrestrial groundwater this would still represent 160% of the Nueces River discharge. This makes it unlikely that groundwater discharge alone is supplying all of the additional ²²⁶Ra. Oil-field brine could potentially account for the remainder. Leakage of 6290 m³ day^− 1 of oil-field brine from the submerged petroleum wells and pipelines within the bay could supply all of the needed ²²⁶Ra. Such large fluxes of brackish groundwater and oil-field brine could significantly affect bay nitrogen budgets, salinities, and dissolved oxygen concentrations and should be considered when determining the freshwater inflow requirements for Nueces Bay and similar estuaries.     

南极普里兹湾及其邻近海域表层水镭同位素的分布及应用

中国第27次南极科学考察期间(2010年12月30日至2011年1月16日),对普里兹湾及其邻近海域表层海水进行了226Ra和228Ra的分析,结果表明:226Ra和228Ra比活度的变化范围分别为1.47—2.43Bq/m3和0.17—0.45Bq/m3,平均值分别为2.13Bq/m3和0.29Bq/m3,228Ra/226Ra)A.R.(228Ra与226Ra的活度比)的变化范围为0.08—0.20,平均值为0.14。根据盐度和226Ra的质量平衡方程,计算出研究海域表层水中冰融水、南极夏季表层水和普里兹湾中深层水的份额。研究海域表层水中温度、盐度、226Ra、228Ra、228Ra/226Ra)A.R.和冰融水份额的空间分布显示,在埃默里冰架前沿海域,西侧海域较东侧海域具有低温、高盐、高226Ra、低228Ra、低228Ra/226Ra)A.R.、低冰融水份额的特征,证实埃默里冰架下水体东进西出的运动规律。根据埃默里冰架前沿东、西侧水体228Ra/226Ra)A.R.的差异,估算出埃默里冰架下表层水体东进西出所经历的时间为1.85a。此外,在普里兹湾湾口中部海域(66.5—67.5°S,72°—74°E),观察到次表层水的上升通风作用,该区域较高的228Ra含量和228Ra/226Ra)A.R.证明这些表层水体并非来自湾外绕极深层水的上涌,而可能来自湾内埃默里冰架输出水体。