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。     

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。     

白令海峡水团来源的镭同位素示踪

对白令海峡64.3°N纬向断面镭同位素的研究表明,水体中226Ra比活度、228Ra比活度和228Ra/226Ra)A.R.存在明显的纬向变化,反映出太平洋与北冰洋水体交换的多种路径.根据温度、盐度和镭同位素的水平与垂直分布,太平洋水进入北冰洋的路径可能主要有3支,分别为白令海峡西侧的阿拉德水、白令海峡东侧的阿拉斯加沿...     

中国近岸海域沉积物226Ra的分布特征

本文对中国7个近岸海域沉积物226Ra的分布进行了研究,结果表明珠江口表层沉积物的226Ra含量较高,其余6个近岸海域(黄河口、胶州湾、长江口、杭州湾、厦门湾、大亚湾)的226Ra含量相近。226Ra含量值显示了研究海域沉积物的“亲陆性”,但不同站位226Ra含量受物源区域、水动力作用及其他环境理化诸因素的影响。226Ra在况积物盐酸沥取相的放射性比度及总量均大于残渣相的相应数值,说明陆源物质在风化及向海迁移过程中绝大部分镭进入到水相中。元洪码头附近海域岩心中226Ra的垂直分布表明,镭发生了沉积后的再迁移。所有各相的活度比(238Ra/226U)_a.r、(226Ra/230Th)_a.r.均小于1.0,进一步证明中国近岸沉积物普遍存在226Ra-238U、226Ra-230Th不平衡现象。     

九龙江河口区水体中224Ra的分布及其应用

研究了九龙江河口区表层水体中224Ra的分布,发现同世界其他河口一样,224Ra在九龙江河口区呈非保守行为;同时发现224Ra-Ss关系受季节变化的影响显着;与世界其他河口相比,九龙江河口表层水体中224Ra含量偏高;用九龙江河口区海端溶解态224Ra估算九龙江河口水流向外海的流速在夏季为2.5cm/s,冬季为0.91cm/s.     

秋季红沿河核电站海域水龄分布及其对水母丰度分布的影响

本研究调查了秋季红沿河核电站海域镭、氡同位素的活度水平及分布情况，结合镭同位素表观年龄模型计算该海域的水体年龄，进而得出研究区域的水体运移方向，初步探讨了水母丰度分布与水体运移的相关关系。得到结论如下:(1)红沿河核电站海域表层水体中224Ra、226Ra及222Rn的活度水平分别为2.9～62.4 dpm/(100 L)，11.9～57.4 dpm/(100 L)及0.1～1.3 dpm/L，镭同位素活度呈现出近岸高、远岸低的分布趋势，氡同位素的分布则更大程度上受水温控制；(2)通过224Ra/226Ra表观年龄模型计算得出红沿河海域表层水体年龄范围介于0～16 d，平均年龄(10.9±3.6) d，水体主体流向为北偏东方向，流速为7.2 cm/s；(3)水母丰度分布与水体流向呈现出较为一致的对应关系，在主体流向方向上，水体年龄较大的海域水母丰度最高。     

九龙江河口区水体中238U、234Th地球化学行为的研究

对采自九龙江河口区盐度介于0～21.97的10个表层水样,铀、钍同位素的测定结果表明,九龙江河口区水体中溶解态的238U含量与盐度之间存在着良好的相关关系,其相关系数可达0.972,表明九龙江河口区水体中的238U呈现保守行为.当S=0时,溶解态234U/238U放射性比值为1.19和1.55(两份水样);而当S=0.90～21.97时,该比值=1.02～1.14,分别呈现河水及河口水铀同位素组成的特征.对于颗粒态铀,其238U含量则介于0.50～9.83×10-3Bq/dm3,且随盐度的增大而呈逐步降低的趋势.九龙江河口区水体中234Th的地球化学行为属于非保守行为,不可逆稳态清除模型计算的结果表明,当盐度介于9.76～17.07时,234Th相对于化学清除的停留时间为6～19d,远低于盐度为0和21.97所对应的停留时间(分别为203d及117d),反映了在该盐度范围内,胶体絮凝沉降对溶解态234Th的快速清除作用.     

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.     

北黄海水体的226Ra和228Ra

用锰纤维富集-射气法测定了北黄海海水中的镭同位素226Ra和228Ra,研究了该海域水体中镭同位素的含量和分布.研究结果表明北黄海水体夏季226Ra的比活度为1.80～4.35 Bq/m3,平均值为3.06 Bq/m3;冬季226Ra的比活度为2.08～5.20 Bq/m3,平均值为3.28 Bq/m3.北黄海夏季228Ra的比活度为3.85～25.60 Bq/m3,平均值为10.60 Bq/m3;冬季228Ra的比活度为3.14～15.60Bq/m3,平均值为7.66 Bq/m3.该数据范围和中国近海其他海域、孟加拉湾、泰国昭披耶河口、濑户内海等海域相近.北黄海东北部海域,渤海海峡靠近山东半岛的海区和中北部海区表层镭同位素活度较高.C1断面镭同位素的分布特征从镭同位素的方面证实了渤海海峡水交换表现为北进南出特征这一结论的正确性.226Ra和228Ra的垂直分布较为复杂,大部分站位呈现出底层活度变高的趋势,其他少数站位呈现出中间层活度高的分布特征,不同来源的镭同位素输入至该海域形成了这样的分布特征.     

北黄海水体的~(226)Ra和~(228)Ra

用锰纤维富集-射气法测定了北黄海海水中的镭同位素226Ra和228Ra,研究了该海域水体中镭同位素的含量和分布.研究结果表明北黄海水体夏季226Ra的比活度为1.80～4.35 Bq/m3,平均值为3.06 Bq/m3;冬季226Ra的比活度为2.08～5.20 Bq/m3,平均值为3.28 Bq/m3.北黄海夏季228Ra的比活度为3.85～25.60 Bq/m3,平均值为10.60 Bq/m3;冬季228Ra的比活度为3.14～15.60Bq/m3,平均值为7.66 Bq/m3.该数据范围和中国近海其他海域、孟加拉湾、泰国昭披耶河口、濑户内海等海域相近.北黄海东北部海域,渤海海峡靠近山东半岛的海区和中北部海区表层镭同位素活度较高.C1断面镭同位素的分布特征从镭同位素的方面证实了渤海海峡水交换表现为北进南出特征这一结论的正确性.226Ra和228Ra的垂直分布较为复杂,大部分站位呈现出底层活度变高的趋势,其他少数站位呈现出中间层活度高的分布特征,不同来源的镭同位素输入至该海域形成了这样的分布特征.     

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.     

Adsorption–desorption reactions and bioturbation transport of Ra in marine sediments: a one-dimensional model with applications

The distribution of trace metals in sediments and their exchange between sediments and overlying water is governed by multiple processes including molecular diffusion, bioturbation (porewater advection, porewater mixing, and particle mixing), chemical reactions and adsorption–desorption. To understand these processes and their relative contributions, a one-dimensional model was built, which includes bioturbation and adsorption–desorption processes, to describe the transport of ²²⁴Ra. Because ²²⁴Ra is adsorbed on MnO₂, ²²⁴Ra may serve as a proxy for trace metal transport. Three sites were sampled and both dissolved and adsorbed ²²⁴Ra were analyzed and modeled to understand the transport and exchange processes. It was found that particle transport of adsorbed ²²⁴Ra followed by desorption at the sediment/water interface typically represents the dominant flux. We have further been able to define conditions where the porewater transport for adsorption reactive metals like ²²⁴Ra (and other metals) may be out of the sediments whereas the active scavenging of ²²⁴Ra from the water column at the sediment water interface via adsorption reactions can result in a flux of ²²⁴Ra into the sediment. These processes are both predicted by the model and observed in sediment samples.     

Adsorption–desorption reactions and bioturbation transport of 224Ra in marine sediments: a one-dimensional model with applications

The distribution of trace metals in sediments and their exchange between sediments and overlying water is governed by multiple processes including molecular diffusion, bioturbation (porewater advection, porewater mixing, and particle mixing), chemical reactions and adsorption–desorption. To understand these processes and their relative contributions, a one-dimensional model was built, which includes bioturbation and adsorption–desorption processes, to describe the transport of ²²⁴Ra. Because ²²⁴Ra is adsorbed on MnO₂, ²²⁴Ra may serve as a proxy for trace metal transport. Three sites were sampled and both dissolved and adsorbed ²²⁴Ra were analyzed and modeled to understand the transport and exchange processes. It was found that particle transport of adsorbed ²²⁴Ra followed by desorption at the sediment/water interface typically represents the dominant flux. We have further been able to define conditions where the porewater transport for adsorption reactive metals like ²²⁴Ra (and other metals) may be out of the sediments whereas the active scavenging of ²²⁴Ra from the water column at the sediment water interface via adsorption reactions can result in a flux of ²²⁴Ra into the sediment. These processes are both predicted by the model and observed in sediment samples.     

Characterizing sources of groundwater to a tropical coastal lagoon in a karstic area using radium isotopes and water chemistry

Radium isotopes (²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and water chemistry were used to identify two chemically distinct sources of submarine groundwater discharge (SGD) in Celestún Lagoon, Yucatán, Mexico. Low salinity groundwater discharging from springs within the lagoon has previously been identified and extensively sampled for nutrient concentrations. However, a second type of groundwater discharging into the lagoon was detected during this study using radium isotope activity measurements. This second type of groundwater is characterized by moderate salinities (within the range of lagoon salinities) and very elevated radium activities in comparison to the low salinity groundwater, mixed lagoon water, and seawater. Further analysis showed that the two types of groundwater also have distinct chloride, strontium, and sulfate ratios, along with slightly different nutrient concentrations. Groundwater discharge occurs through large and small springs scattered throughout the lagoon, and both types of groundwater were detected discharging from one of the larger springs. The relative proportions of low salinity groundwater and brackish high radium groundwater varied over the tidal cycle. In order to better understand the relative contributions of each type of groundwater to the lagoon, a three end-member mixing model based on the distinct chemical and isotopic compositions of both types of groundwater and of seawater was used to estimate the distribution of each water type throughout the lagoon in different seasons. This study suggests that substantial groundwater discharge to the lagoon can occur during both dry and rainy seasons. The presence of two groundwater sources has implications for monitoring and protection of the Celestún Lagoon Biosphere Reserve, since the two sources may have different susceptibilities to anthropogenic contamination depending on their respective recharge area and recharge rates.     

Estimating submarine groundwater discharge around Isola La Cura, northern Venice Lagoon (Italy), by using the radium quartet

The four naturally-occurring radium isotopes (²²³Ra, ²²⁴Ra, ²²⁶Ra and ²²⁸Ra) were used to estimate the submarine groundwater discharge (SGD) in the Isola La Cura marsh area in the northern Venice Lagoon (Italy). By determining the radium contributors to the study area (river, coastal ocean and sediments) the radium excess in the lagoon water was quantified through a mass balance model. This radium excess is attributed to a submarine groundwater discharge source and represents the most important input of radium. Possible endmembers were considered from analysis of groundwater samples (subtidal and marsh piezometers, marsh wells and seepage meters) that were enriched in Ra by one to two orders of magnitude relative to surface waters. In particular, a permeable layer at 80 cm depth in the surrounding marsh is considered to be representative of the most likely SGD source, although similar radium activities were measured in other subtidal porewater samples collected in the Isola La Cura area. The estimated SGD flux to the study area ranged from 1 · 10⁹ to 6 · 10⁹ L·d^− 1, the same order of magnitude as the overall riverine input to the lagoon (3 · 10⁹ L·d^− 1). A major fraction of this SGD flux is likely recirculated seawater, as evidenced by the endmember salinity. The water residence time of 2 days was estimated by both using the shortest-lived radium isotope and estimating the volume of water exchanged between the lagoon and the open sea during a tidal cycle (tidal prism approach). This SGD flux could be used to estimate the input of other chemical species (metals, nutrients, etc.) via SGD which might affect the Venice Lagoon ecosystem.     

Measurement of nuclides of uranium and thorium series of disequilibrium using γ-spectroscopy

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基于223Ra和224Ra的桑沟湾海底地下水排放通量

海底地下水排放（SGD）是陆地向海洋输送水量和营养物质的重要通道之一,对沿海物质通量及其生物地球化学循环有重要的影响,对生态环境起着不可忽视的作用。本文运用天然放射性同位素223Ra和224Ra示踪估算了我国北方典型养殖基地桑沟湾的海底地下水排放通量。结果表明,海底地下水样尤其是间隙水中Ra活度[224Ra=（968±31）dpm/（100 L）,223Ra=（31.4±4.9）dpm/（100 L）,n=9]远高于表层海水[224Ra=（38.7±2.0）dpm/（100 L）,223Ra=（1.70±0.50）dpm/（100 L）, n=21]。假设稳态条件下,考虑Ra的各源、汇项,利用Ra平衡模型,估算出桑沟湾SGD排放通量为（0.23~1.03）×107 m3/d。潮周期内的观测结果显示,涨潮时,水力梯度较小,SGD排放变弱,落潮时,水力梯度较大,导致了相对较多的SGD排放。在一个潮周期间,基于223Ra和224Ra得到的SGD排放通量平均为0.39×107 m3/d。潮汐动力下的SGD排放平均占总SGD排放的61%,因此桑沟湾沿岸的地下水排放主要受潮汐动力的影响,并对海水组成及海陆间物质交换有显著贡献。     

228Ra, 226Ra, 224Ra and 223Ra in potential sources and sinks of land-derived material in the German Bight of the North Sea: implications for the use of radium as a tracer

Activities of the naturally occurring radium nuclides ²²⁸Ra, ²²⁶Ra, ²²⁴Ra and ²²³Ra were determined in waters of the open German Bight and adjacent nearshore areas in the North Sea, in order to explore the potential use of radium isotopes as natural tracers of land–ocean interaction in an environment characterised by extensive tidal flats, as well as riverine and groundwater influx. Data collected at various tidal phases from the Weser Estuary (²²⁸Ra: 46.3 ± 4.6; ²²⁶Ra: 17.1 ± 1.1; ²²⁴Ra: 26.1 ± 8.2 to 36.5 ± 6.1; ²²³Ra: 1.8 ± 0.1 to 4.0 ± 0.4), tidal flats near Sahlenburg (²²⁸Ra: 39.3 ± 3.8 to 46.0 ± 4.5; ²²⁶Ra: 15.5 ± 1.5 to 16.5 ± 1.7; ²²⁴Ra: 34.3 ± 2.2 to 85.3 ± 6.3; ²²³Ra: 3.6 ± 0.5 to 8.0 ± 1.2), freshwater seeps on tidal flats near Sahlenburg (²²⁸Ra: 42.1 ± 4.1; ²²⁶Ra: 21.3 ± 2.2; ²²⁴Ra: 5.1 ± 0.9; ²²³Ra: 2.6 ± 1.3) and also in permanently inundated parts of the North Sea (²²⁸Ra: 23.0 ± 2.3 to 28.2 ± 2.8; ²²⁶Ra: 8.2 ± 0.8 to 11.8 ± 1.2; ²²⁴Ra: 3.1 ± 1.0 to 10.1 ± 0.9; ²²³Ra: 0.1 ± 0.02 to 0.9 ± 0.05; units: disintegrations per minute per 100 kg water sample) reveal that, except for the fresh groundwater, the potential end-members of nearshore water mass mixing have quite similar radium signatures, excluding a simple discrimination between the sources. However, the decreasing activities of the short-lived ²²⁴Ra and ²²³Ra isotopes recorded towards the island of Helgoland in the central German Bight show a potential to constrain fluxes of land-derived material to the open North Sea. The largest source for all radium isotopes is generally found on the vast tidal flats and in the Weser Estuary. Future work could meaningfully combine this so-called radium quartet approach with investigations of radon activity. Indeed, preliminary data from a tidal flat site with fresh groundwater seepage reveal a ²²²Rn signal that is clearly lower in seawater.     

Distribution of radium-224 in the western Arctic Ocean

1Introduction ThephysicalcharacteristicsintheArcticOcean includewidecontinentalshelves,accountingfor36% oftheocean’ssurfacearea(MooreandSmith,1986) withseasonalicecover.Theprincipalwatersentering theArcticOceanarefromtheNorthAtlanticviathe FramStraitandtheBarentsSea,andtheNorthPacific viatheBeringStrait.Withinthearcticinterior,thewa- tersjoininthelarge-scalecirculationandaresubse- quentlymodifiedbyprocessesofair/sea/iceinterac- tion,riverinflow,andexchangewithsurrounding shelves.Howeve…