Uncertainties in the preparation of Ra Mn fiber standards

Delayed coincidence counters (RaDeCC), used for measuring ²²³Ra and ²²⁴Ra preconcentrated from water onto MnO₂-impregnated acrylic fiber (“Mn-fiber”), require a standard Mn-fiber column that has a precisely known activity of ²²⁴Ra for calibration. This may be done by adding an aged ²²⁸Th standard solution to adsorb both ²²⁸Th and its daughter ²²⁴Ra quantitatively onto a Mn fiber. We used both seawater and deionized water (DIW) for testing the adsorption efficiency of Th and Ra onto Mn fibers. Our experimental results show that more than 50% of thorium (²³²Th and ²²⁸Th) breaks through the Mn-fiber column when DIW is used as a medium. However, near quantitative recoveries are obtained if filtered (0.45 μm) seawater is used to prepare the standard. In the case of pure DIW, the pH (initial pH  5.3) rises to > 10 after passing through the column while seawater (initial pH  7.8) changes to  7.2. Thus, the lack of thorium adsorption in DIW may be attributed to this huge increase of pH and the consequent formation of Th(OH)₄ and polyhydroxyl colloids. Based on these observations, we recommend that one should use either artificial seawater or natural seawater (which has negligible ²²⁴Ra and ²²⁸Th) as a loading solution after 0.45 μm filtration. In addition, the thorium adsorption efficiency should be confirmed either by thorium analysis of the effluent solution or long-term monitoring of the supported ²²⁴Ra on the Mn fiber using the RaDeCC. Similar cautions are likely necessary for making ²²³Ra standards by adsorption of ²²⁷Ac onto Mn fibers.     

TIMS measurements of Ra and Ra in the Gulf of Lion, an attempt to quantify submarine groundwater discharge

Submarine groundwater discharge (SGD) is now recognized as an important pathway for water and chemical species fluxes to the coastal ocean. In order to determinate SGD to the Gulf of Lion (France), we measured the activities of ²²⁶Ra and ²²⁸Ra by thermal ionization mass spectrometry (TIMS) in coastal waters and in the deep aquifer waters of the Rhone deltaic plain after pre-concentration of radium by MnO₂. Compared to conventional counting techniques, TIMS requires lower quantities of water for the analyses, and leads to higher analytical precision. Radium isotopes were thus measured on 0.25–2 L water samples containing as little as 20 fg of ²²⁶Ra and 0.2–0.4 fg of ²²⁸Ra with precision equal to 2%. We demonstrate that coastal surface waters samples are enriched in ²²⁶Ra and ²²⁸Ra compared to the samples further offshore. The high precision radium measurements display a small but significant ²²⁶Ra and ²²⁸Ra enrichment within a strip of circa 30 km from the coast. Radium activities decrease beyond this region, entrained in the northern current along the shelf break or controlled by eddy diffusion. The radium excess in the first 30 km cannot be accounted for by the river nor by the early diagenesis. The primary source of the radium enrichment must therefore be ascribed to the discharge of submarine groundwater. Using a mass-balance model, we estimated the advective fluxes of ²²⁶Ra and ²²⁸Ra through SGD to be 5.2 × 10¹⁰ and 21 × 10¹⁰ dpm/d respectively. The ²²⁶Ra activities measured in the groundwater from the Rhone deltaic plain aquifer are comparable to those from other coastal groundwater studies throughout the world. By contrast, ²²⁸Ra activities are higher by up to one order of magnitude. Taking those groundwater radium activities as typical of the submarine groundwater end-member, a minimum volume of 0.24–4.5 × 10¹⁰ l/d is required to support the excess radium isotopes on the inner shelf. This has to be compared with the average rivers water runoff of 15.4 × 10¹⁰ l/d during the study period (1.6 to 29% of the river flow).     

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.     

Uncertainties associated with Ra and Ra measurements in water via a Delayed Coincidence Counter (RaDeCC)

The short-lived radium isotopes, ²²³Ra (T_1/2 = 11.4 days) and ²²⁴Ra (T_1/2 = 3.66 days), have been successfully used as tracers of several environmental processes, e.g., submarine groundwater discharge, coastal mixing processes, and water residence times. In this paper, the uncertainties associated with ²²³Ra and ²²⁴Ra measurements using a Radium Delayed Coincidence Counter are determined on a detailed error propagation basis with a confidence interval of 1σ. From the data analyses of several groups of coastal water samples, the calculated relative uncertainties averaged 12% for the ²²³Ra and 7% for the ²²⁴Ra. These uncertainties can decrease for radium-enriched groundwater samples although asymptotic limits have been found at 7% relative uncertainty for ²²³Ra and 4% for ²²⁴Ra. In this paper, the influence of sampling and measurement parameters on the final radium uncertainties is evaluated in order to provide guidance to optimize these factors and obtain more reliable results.     

224,223Ra和137Cs在吕宋海峡及周边海域的分布以及其对“彩虹”台风的响应

本文报道2015年9月和2016年5月期间天然放射性核素²²⁴Ra和²²³Ra在吕宋海峡及周边海域表层和垂向水体的分布特征。为理解日本福岛核事故的影响,本文亦分析研究区域内人工放射性核素¹³⁷Cs的分布特征。结果表明,^224,223Ra和¹³⁷Cs比活度水平均处于我国南海海洋天然放射性本底变化范围之内。²²⁴Ra在吕宋海峡以西南海北部海域比活度较高,在吕宋海峡以东菲律宾海域比活度较低。¹³⁷Cs没有明显的分布趋势。基于三站位（LS3,LS5和LS8）²²⁴Ra、¹³⁷Cs以及温盐的垂向分布特征,本文揭示²²⁴Ra和¹³⁷Cs在热带表层水、次表层水和中-深层水中比活度水平和梯度变化的差异特征。彩虹台风事件扭转了整个吕宋海峡及周边海域的海流循环过程。大量以低水平²²⁴Ra为特征的西太平洋海水涌入南海,降低水体²²⁴Ra比活度水平。但是,西太平洋和南海北部海域水体¹³⁷Cs比活度水平没有明显差异,台风导致的海流变化对水体¹³⁷Cs比活度没有明显影响。     

Water mass ages of coastal ponds estimated using Ra and Ra as tracers

Measurements of the naturally occurring radioisotopes ²²³Ra (t_1/2 = 11.4 days) and ²²⁴Ra (t_1/2 = 3.66 days) in southern Rhode Island salt ponds were combined with a simple model to obtain independent estimates of the age of these coastal waters. Surface water and porewater samples were collected quarterly in Winnapaug, Quonochontaug, Ninigret, Green Hill, and Pt. Judith-Potter Ponds, as well as nearly monthly in the surface water of Rhode Island Sound, beginning January 2002 through August 2003. Surface water activities ranged from 1–78 dpm 100 L^− 1 and 5–885 dpm 100 L^− 1 for ²²³Ra and ²²⁴Ra, respectively. Porewater radium activities ranged from 3 to 715 dpm 100 L^− 1 for ²²³Ra, and 57–4926 dpm 100 L^− 1 for ²²⁴Ra. Results indicate seasonally varying water mass ages for Ninigret (5–12 days), Winnapaug (2–6 days) and Pt. Judith-Potter Ponds (1–9 days) and, in contrast, relatively constant ages for Green Hill (5–7 days) and Quonochontaug Ponds (3–6 days).     

Analysis of Ac in seawater by delayed coincidence counting

The activity of ²²⁷Ac in seawater was determined using a delayed coincidence counting technique based on the measurement of the short-lived daughter ²²³Ra (half-life of 11 days). Two 180-l aliquots of Ac free seawater from surface waters of the California borderlands were spiked with Harwell Uraninite standard and the added Ac and Ra were extracted on Mn-fibers. The measured activities on the fibers agreed to within 5% of the equilibrium Ac activity of the spike addition, well within the 2σ counting error of 7% for the measurements. Thus, any recovery error was indistinguishable from counting error. Large volume samples were collected from the water column of the Eastern North Pacific in December of 1998 and processed through Mn-fiber columns. The ²²³Ra activities on the fibers were measured four or more times over a period of 2 months by the technique of [J. Geophys. Res. 101 (1996) 1321] to determine if the activity of ²²³Ra was wholly supported by ²²⁷Ac. In most cases, no significant differences in ²²³Ra activity were observed during repeated counting of the same sample, again implying that ²²³Ra was supported wholly by ²²⁷Ac. In samples where unsupported ²²³Ra were present, samples were counted beyond five half live of the ²²³Ra (>60 days). Two depth profiles of ²²⁷Ac in the Eastern North Pacific showed similar shape and activity to profiles in the Western and Central Pacific measured with alpha-spectrometry by [Nature 310 (1984) 486). Surface waters of the Southern Ocean were relatively enriched in ²²⁷Ac compared to Eastern North Pacific waters, possibly indicating export of the parent ²³¹Pa from Atlantic surface waters or upwelling.     

Radium and radon radioisotopes in regional groundwater, intertidal groundwater, and seawater in the Adelaide Coastal Waters Study area: Implications for the evaluation of submarine groundwater discharge

The input of groundwater-borne nutrients to Adelaide's (South Australia) coastal zone is not well known but could contribute to the ongoing decline of seagrass in the area. As a component of the Adelaide Coastal Waters Study (ACWS), the potential for using the radium quartet (²²³Ra, ²²⁴Ra, ²²⁶Ra and ²²⁸Ra) and ²²²Rn to evaluate submarine groundwater discharge (SGD) was evaluated. Potential isotopic signatures for SGD were assessed by sampling groundwater from three regional aquifers potentially contributing SGD to the ACWS area. In addition, intertidal groundwater was sampled at two sand beach sites. In general, the regional groundwaters were enriched in long-lived Ra isotopes (²²⁶Ra and ²²⁸Ra) and in ²²²Rn relative to intertidal groundwater. Radium activity (but not ²²²Rn activity) was positively correlated to salinity in groundwater from one of the regional aquifers and in intertidal groundwater. Radium isotope ratios (²²³Ra/²²⁶Ra, ²²⁴Ra/²²⁶Ra and ²²⁸Ra/²²⁶Ra) were less variable than individual Ra isotope activities within potential SGD sources. Recirculated seawater (estimated from the intertidal groundwater samples with seawater-like salinities) also had distinctly higher Ra isotope ratios than the regional groundwaters. The activities for all radioisotopes were relatively low in seawater. The activity of the short-lived ²²³Ra and ²²⁴Ra were highest at the shoreline and declined exponentially with distance offshore. In contrast, ²²⁸Ra and ²²⁶Ra activities had a weak linear declining trend with distance offshore. Rn-222 activity was at or near background in all seawater samples. The pattern of enrichment in short-lived Ra isotopes and the lack of ²²²Rn in seawater suggest that seawater recirculation is the main contributor to SGD in the ACWS area. Preliminary modeling of the offshore flux of ²²⁸Ra and ²²⁶Ra suggest that the SGD flux to the ACWS area ranges between 0.2 and 3 · 10^− 3 m³ (m of shoreline)^− 1 s^− 1.     

Comparison of techniques for pre-concentrating radium from seawater

In the framework of the KEOPS project (KErguelen: compared study of the Ocean and the Plateau in Surface water), we aimed to provide information on the water mass pathways and vertical mixing on the Kerguelen Plateau, Southern Ocean, based on ²²⁸Ra profiles. Because ²²⁸Ra activities are extremely low in this area (~ 0.1 dpm/100 kg or ~ 2.10^− 18 g kg^− 1), the filtration of large volumes of seawater was required in order to be able to detect it with minimal uncertainty. This challenging study was an opportunity for us to test and compare methods aimed at removing efficiently radium isotopes from seawater. We used Mn-fiber that retains radium and that allows the measurement of all four radium isotopes (²²⁶Ra, ²²⁸Ra, ²²³Ra, ²²⁴Ra). First, we used Niskin bottles or the ship's seawater intake to collect large volumes of seawater that were passed onto Mn-fiber in the laboratory. Second, we filled cartridges with Mn-fiber that we placed in tandem on in situ pumps. Finally, we fixed nylon nets filled with Mn-fiber on the frame of in situ pumps to allow the passive filtration of seawater during the pump deployment.Yields of radium fixation on the cartridges filled with Mn-fiber and placed on in situ pumps are ca. 30% when combining the two cartridges. Because large volumes of seawater can be filtered with these pumps, this yields to effective volumes of 177–280 kg (that is, higher than that recovered from fourteen 12-l Niskin bottles). Finally, the effective volume of seawater that passed through Mn-fiber placed in nylon nets and deployed during 4 h ranged between 125 and 364 kg. Consequently, the two techniques that separate Ra isotopes in situ are good alternatives for pre-concentrating radium from seawater. They can save ship-time by avoiding repeated CTD casts to obtain the large volumes of seawater. This is especially true when in situ pumps are deployed to collect suspended particles. However, both methods only provide ²²⁸Ra/²²⁶Ra ratios. The determination of the ²²⁸Ra specific activity is obtained by multiplying this ratio by the ²²⁶Ra activity measured in a discrete sample collected at the same water depth.     

Determination of residence time and mixing processes of the Ubatuba,Brazil, inner shelf waters using natural Ra isotopes

Coastal waters contain elevated dissolved activities of short-lived radium isotopes, ²²³Ra and ²²⁴Ra, having half-lives of 11.4 and 3.66 days, respectively. The input of these isotopes near the coast must be balanced by decay and mixing into the open ocean, where excess activities are zero. Since the decay rate is known, in the ideal case the mixing rate may be determined from the offshore distribution of these isotopes. This study found that samples collected in June 2000 followed the expected exponential decrease with distance offshore. We assign a dispersion coefficient of 28–39 m² s⁻¹ for this study. During January 2002 and November 2003, there was not a consistent decrease of activity with distance offshore. This is likely due to the ruggedness of the coastline, where many bays and small islands interrupt simple mixing patterns. To estimate exchange rates during 2002 and 2003, we used a model based on the decrease in the ²²⁴Ra/²²³Ra activity ratio (AR) with time for samples isolated from fresh inputs of Ra. This model yielded residence times of 1–2 weeks for samples collected within 20 km of the coast. We used this residence time to calculate the flux of ²²⁸Ra (half-life = 5.7 years) to the study area necessary to maintain the enrichment relative to ocean water. This enrichment is a factor of ten greater than the flux of ²²⁸Ra expected from submarine groundwater discharge (SGD) occurring within 50 m of shore.     

Short-lived radium isotopes in the Hawaiian margin: Evidence for large fluid fluxes through the Puna Ridge

We measured significant activities of short-lived radium isotopes, ²²³Ra (half-life = 11 days) and ²²⁴Ra (half-life = 3.7 days), around the margins of the Hawaiian Islands to water depths of 3500 m. These measurements suggest fluid inputs from the basalt to the surrounding ocean. In general ²²³Ra activities were considerably greater than ²²⁴Ra in spite of the expected higher production rate of ²²⁴Ra activity in basalt. The ²²³Ra was not supported by dissolved ²²⁷Ac. The highest enrichments of ²²³Ra were measured over the Puna Ridge (2100 m depth) east of Hawaii. Here ²²³Ra activities reached 19 dpm/m³, similar to activities measured near sites of active submarine groundwater discharge in the South Atlantic Bight. To explain the high activities of ²²³Ra unaccompanied by ²²⁴Ra, we postulate that thermally-driven circulation of seawater through the Puna Ridge deposits ²³¹Pa on basalt surfaces. With time the ²³¹Pa produces ²²⁷Ac and ²²³Ra; and ²²³Ra desorbs into the circulating fluids. These fluids then transport ²²³Ra into the overlying ocean. Based on the inventory of ²²³Ra above the Puna Ridge, we estimate the flow of fluids through the ridge to be on the order of 20–60 cm³ cm^− 2 day^− 1. In less than 1000 years the incoming seawater could provide enough ²³¹Pa to basalt surfaces to balance the inventory of ²²³Ra above the ridge if only 8% of the ²²³Ra was transported to the overlying water. These observations on the flanks of a volcanically-active ocean island have significant implications for quantifying fluid fluxes from the flanks of the mid-ocean ridge system. By mapping ²²³Ra inventories in the ocean above ridge flanks and measuring the activity of ²²³Ra in the emerging fluids, the fluid flux can be obtained.     

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.     

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^224 Ra

用锰纤维富集-射气法测量了北黄海水体的^224 Ra,研究了该海域夏季和冬季2个季节^224 Ra比活度及其垂直分布,并对其进行了比较研究．北黄海夏季^224 Ra 比活度为0．24—3．48Bq／m2,平均值为1．14Bq／m2;冬季^224 Ra比活度为0．37～6．68Bq／m2,平均值为0．94Bq／m2．北黄海的表层水有3个^224 Ra 高值区,分别位于东北部海域、渤海海峡南部和北黄海中北部海区．30m水深将^224 Ra比活度的垂直分布分成上层和下层2层．在0～30m水层,夏季,随着水深增加^224 Ra比活度逐渐增加,比活度变化较小;冬季部分站位由表层向下^224 Ra比活度逐渐降低．30m水深以下,^224 Ra比活度随着水深的增加而增加,而且变化幅度较大．由^224 Ra比活度的垂直分布得出该海域的垂直涡动扩散系数为2．5～43．5cm2／s,夏季北黄海冷水团中心海域底层溶解态化学物质输运补给到上层所经历的时间为9～15d左右．     

Submarine groundwater discharge to Great South Bay, NY, estimated using Ra isotopes

There is increasing evidence that submarine groundwater discharge (SGD) in many areas represents a major source of dissolved chemical constituents to the coastal ocean. In Great South Bay, NY, previous studies have shown that the discharge of nutrients with SGD may cause harmful algal blooms. This study estimates SGD to Great South Bay during August 2006 by performing a mass balance for each of the dissolved Ra isotopes (²²⁴Ra, ²²³Ra, ²²⁸Ra, ²²⁶Ra). The budget indicates a major unknown source (between 30 and 60% of the total input) of Ra to the bay. This imbalance can be resolved by a flux of Ra-enriched groundwater on the order of 3.5–4.5 × 10⁹ L d^− 1, depending on the Ra isotope. The Ra-estimated SGD rates compare well with those previously estimated by models of flow that decreases exponentially away from shore. Compared to previous reports of fresh groundwater discharge to the bay, the Ra-estimated discharge must comprise approximately 90% recirculated seawater. The good agreement between Ra- and model-estimated flow rates indicates that the primary SGD endmember may be best sampled at shallow depths in the sediments a short distance bayward of the low tide line.     

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).     

Seasonal changes in submarine groundwater discharge to coastal salt ponds estimated using Ra and Ra as tracers

Submarine groundwater discharge (SGD) to coastal southern Rhode Island was estimated from measurements of the naturally-occurring radioisotopes ²²⁶Ra (t_1/2 = 1600 y) and ²²⁸Ra (t_1/2 = 5.75 y). Surface water and porewater samples were collected quarterly in Winnapaug, Quonochontaug, Ninigret, Green Hill, and Pt. Judith–Potter Ponds, as well as nearly monthly in the surface water of Rhode Island Sound, from January 2002 to August 2003; additional porewater samples were collected in August 2005. Surface water activities ranged from 12–83 dpm 100 L^− 1 (60 dpm = 1 Bq) and 21–256 dpm 100 L^− 1 for ²²⁶Ra and ²²⁸Ra, respectively. Porewater ²²⁶Ra activities ranged from 16–736 dpm 100 L^− 1 (2002–2003) and 95–815 dpm 100 L^− 1 (2005), while porewater ²²⁸Ra activities ranged from 23–1265 dpm 100 L^− 1. Combining these data with a simple box model provided average ²²⁶Ra-based submarine groundwater fluxes ranging from 11–159 L m^− 2 d^− 1 and average ²²⁸Ra-derived fluxes of 15–259 L m^− 2 d^− 1. Seasonal changes in Ra-derived SGD were apparent in all ponds as well as between ponds, with SGD values of 30–472 L m^− 2 d^− 1 (Winnapaug Pond), 6–20 L m^− 2 d^− 1 (Quonochontaug Pond), 36–273 L m^− 2 d^− 1 (Ninigret Pond), 29–76 L m^− 2 d^− 1 (Green Hill Pond), and 19–83 L m^− 2 d^− 1 (Pt. Judith–Potter Pond). These Ra-derived fluxes are up to two orders of magnitude higher than results predicted by a numerical model of groundwater flow, estimates of aquifer recharge for the study period, and values published in previous Ra-based SGD studies in Rhode Island. This disparity may result from differences in the type of flow (recirculated seawater versus fresh groundwater) determined using each technique, as well as variability in porewater Ra activity.     

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...     

Radium mass-balance in Jamaica Bay, NY: Evidence for a substantial flux of submarine groundwater

A mass balance for the naturally-occurring radium isotopes (²²⁴Ra, ²²³Ra, ²²⁸Ra, and ²²⁶Ra) in Jamaica Bay, NY, was conducted by directly estimating the individual Ra contributions of wastewater discharge, diffusion from fine-grained subtidal sediments, water percolation through marshes, desorption from resuspended particles, and water exchange at the inlet. The mass balance revealed a major unknown source term accounting for 19–71% of the total Ra input, which could only be resolved by invoking a source from submarine groundwater. Shallow (< 2 m depth) groundwater from permeable sediments in Jamaica Bay was brackish and enriched in Ra relative to surface bay waters by over two orders of magnitude. To balance Ra fluxes, a submarine groundwater input of 0.8 × 10⁹–9.0 × 10⁹ L d^− 1 was required. This flux was similar for all four isotopes, with individual estimates varying by less than a factor of 2. Our calculated groundwater flux was 6- to 70-fold higher than the fresh groundwater discharge to the bay estimated by hydrological methods, but closely matched direct flow rates measured with seepage meters. This suggests that a substantial portion of the discharge consisted of recirculated seawater. The magnitude of submarine groundwater discharge varied seasonally, in the order: summer > autumn > spring. Chemical analyses suggest that the recirculated seawater component of submarine groundwater delivers as much dissolved nitrogen to the bay as the fresh groundwater flux.     

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.