Continuous southwestward spread of Fukushima-derived 137Cs in the subtropical western North Pacific and its intrusion flux into the South China Sea.

We provide transect profiles of 137Cs and 90Sr along 146.5°E, 136°E and 21°N in the subtropical western North Pacific (WNP) during May 2018. Exploiting the constant global fallout 137Cs/90Sr ratio, we separated Fukushima-derived 137Cs (137CsF) from background 137Cs. At most stations, 137CsF exhibited only one subsurface peak at 300 m depth, corresponding to subtropical mode water (STMW); however, at 25-28°N along 146.5°E and 25-26°N along 136°E, 137CsF exhibited two subsurface peaks, with another peak occurring at 500 m depth, corresponding to lighter central mode water (L-CMW). Temporal changes in 137CsF vertical profiles showed that 137CsF entrained by STMW has recirculated within the western subtropical gyre, while 137CsF entrained by L-CMW has turned southwestward and arrived the western basin in 2018. In the Luzon Strait, the entrance to the South China Sea (SCS), subsurface 137Cs increased since 2013 and peaked in approximately 2018. The estimated amount of 137CsF entering the SCS during 2013-2019 was 0.33 ± 0.10 PBq, equivalent to 1.7-2.2% of total leakage of 137CsF into the ocean. These results enhance our understanding of the protracted spread and fate of 137CsF in the subtropical WNP.

Fresh Groundwater Discharge as a Major Source of 90Sr into the Coastal Ocean.

The behavior and source of 90Sr in the coastal ocean remain uncertain. Here, we investigated the distributions of 90Sr in coastal fresh groundwater, river water, pore water, and seawater in three bays along the southeastern coast of China between 2019 and 2021 and evaluated the potential of submarine groundwater discharge (SGD) as a source of coastal 90Sr. The 90Sr activity in coastal fresh groundwater was higher than that in river water and seawater, while the 90Sr activity in pore water was comparable to that in adjacent seawater. In addition, nonconservative mixing behavior of 90Sr along the salinity gradient between river water and seawater was observed. These observations indicated that fresh SGD may serve as an additional source of 90Sr in coastal seawater. Combining our groundwater 90Sr data with the reported fresh SGD flux data, the estimated fresh SGD-derived 90Sr fluxes into the three bays were comparable to or even higher than those supplied by riverine sources. These results revealed that fresh SGD is a major but overlooked source of 90Sr in the coastal ocean. This subterranean pathway for transport of 90Sr to the coastal ocean should be considered in the monitoring and risk assessment of coastal areas, especially those near nuclear facilities.

Study of Ra desorption processes in an estuary system with high-turbidity at the Southeast China.

Radium (Ra) isotopes are extensively used as geochemical tracers for studying water mass mixing and submarine groundwater discharge in marginal and coastal seas. However, river-borne particles and seafloor sediments are an important source of Ra in marine systems due to Ra desorption. Therefore, it is necessary to study the desorption behaviors of Ra isotopes in river sediment or suspended particles. Here, the desorption behaviors of four Ra isotopes (223Ra, 224Ra, 226Ra, and 228Ra) in the Zhangjiang River sediments were investigated by a series of designed variable-controlling experiments in the laboratory. Within the designed salinity range, desorption amounts of Ra isotopes increased with increasing salinity, and when the salinity was greater than 15 ppt, Ra desorption reached an equilibrium state. Overall, desorption of Ra isotopes increased with the decrease of particle grain size, however, the desorption fractions of 224Ra and 228Ra decreased with decreasing particle size due to the increase of original Ra activities in smaller sediment particles. In the experiments, we found that two sediment samples with similar mean grain size (3.8 µm and 3.3 µm) and similar grain size distributions had significantly different Ra desorption under the same conditions. The results of mineral composition analysis based on X-ray diffraction showed that these two samples had different percentages of kaolinite, quartz, and plagioclase, which indicated that the mineral composition of particles had an important effect on Ra isotope desorption. In conclusion, salinity, particle grain size, and mineral composition all had significant effects on Ra desorption behaviors of sediment particles. Based on the above desorption experiments, the desorbed fluxes of four Ra isotopes from river-borne sediments to the Dongshan Bay were estimated to be (5.95 ± 1.47) × 107 Bq yr-1 for 223Ra, (1.95 ± 0.27) × 109 Bq yr-1 for 224Ra, (2.73 ± 0.47) × 108 Bq yr-1 for 226Ra, and (1.26 ± 0.20) × 109 Bq yr-1 for 228Ra, respectively.

Molecular level characterization of the biolability of rainwater dissolved organic matter.

The atmospheric wet deposition has been recognized as a significant allochthonous source of dissolved organic carbon (DOC) to the ocean. However, few studies have examined the biolability of rainwater dissolved organic matter (DOM) at the molecular level. Rainwater samples were collected and incubated with ambient microbes. DOC, UV-vis spectroscopy, formic acid (FA), acetic acid (AA), and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS) were applied. Approximately 50 ± 16 % of rainwater DOC and ~90 % of FA and AA were bioconsumed within 28 days. The contribution of FA and AA to the total BDOC was ~30 %, which was the largest known biolabile fraction in rainwater DOC. In contrast, only approximately 15 % of formulae identified by FT-ICRMS were consumed, which were characterized by higher saturation, higher heteroatom content and lower modified aromaticity. Among the major high molecular weight secondary organic carbon (HWW-SOC)-like compounds, organosulfate contained the largest fraction of consumed formulae, while biogenic volatile organic-derived CHO compounds had the lowest. Our study for the first time provided both quantitative and qualitative understanding of the bioavailability of rainwater DOM, which is essential for understanding their effects on the biogeochemical cycles and the environmental health in the receiving waters.

Multiproxy probing of anthropogenic influences on the different components of dissolved organic matter in coastal rainwater.

In an environment that is tightly linked to humankind, how anthropogenic activity affects the quality and quantity of dissolved organic matter (DOM) in atmospheric depositions is not well understood. In this study, dissolved organic carbon (DOC), UV-vis spectra combined with molecular markers, including formic acid (FA), acetic acid (AA) and dissolved black carbon (DBC), were applied to track the temporal variation and influential factors of rainwater DOM at a coastal site. The ranges of DOC, light absorption at 254 nm (a254), FA, AA and DBC were 23.2-471 µmol L-1, 0.16-10.6 m-1, 0.12-23.5 µmol L-1, 0.44-37.8 µmol L-1 and 0.02-4.8 µmol L-1, respectively. The negative correlations between DOC, a254, AA and precipitation amount revealed a dilution effect. The concentrations of all measured DOM components were statistically different among different seasons with the highest value in spring. Higher DOM concentrations also occurred in the rain with backward trajectories influenced by the land. Compared to the nearby riverine DOM, the DOC-specific UV absorbance (SUVA254) of rainwater was lower, suggesting lower aromaticity of rainwater DOM. Significant correlations among different DOM components suggest that they shared similar sources or were affected by the same processes, while the significant correlations with anions (SO42-, F- and NO3-) and the ratio of FA to AA all suggested that the direct emission and secondary production from anthropogenic emissions (fossil fuel burning, biomass and biofuel burning) played important roles in regulating the level of DOM concentration in rainwater. Correlations with environmental variables (PM2.5, CO and NO2) further confirmed the input from anthropogenic activities. Furthermore, the monthly wet atmospheric deposition fluxes of DOM components (except DBC) can be successfully simulated by monthly precipitation and monthly average values of PM2.5 and NO2. Future studies should examine how atmospheric deposition affects the biogeochemical cycles in coastal regions.

Comprehensive risk assessment of marine radioactivity in the Beibu Gulf of Guangxi.

In this paper, a marine environmental sensitivity index system was constructed based on three factors: the marine biological species sensitivity, the marine ecological value sensitivity and the social and economic sensitivity. Combined with numerical simulations of 137Cs in the Beibu Gulf under the condition of a level-7 nuclear accident, a comprehensive risk assessment of marine radioactivity under the simulated accident in the Beibu Gulf was carried out. The results show that the areas at high risk and medium-to-high risk to marine radioactivity are mainly concentrated within 30 km of the Fangchenggang Nuclear Power Plant. The medium-risk areas are mainly distributed in sea areas within 30-50 km of the nuclear power plant, and the other sea areas are low-risk areas. The distribution of the risk sources and the characteristics of the regional tidal currents are the main factors affecting the magnitude and distribution of the comprehensive risk of regional marine radioactivity.

An effective method for the determination of 106Ru in seawater by γ-spectrometry.

106Ru is a product originating from the fission reactions of uranium (235U) and plutonium (239Pu). 106Ru represents a potential source of radioactive marine contamination since it makes up 70-90% of the total radioactivity of liquid effluents from fuel reprocessing plants; thus, it is important to effectively determine the quantity of 106Ru in the natural environment. In this study, a simple and effective method was developed for the determination of 106Ru in seawater by γ-spectrometry using NiS coprecipitation. In addition, the amounts of S2- and Ni2+ added, Ru3+ carrier addition, pH, salinity, and sample volume were tested, and accordingly, optimal conditions were proposed. With the optimized conditions, the recovery of 106Ru in seawater ranged from 85.3% to 92.3%, with an average of 88.1 ± 4.2%. The method proposed in the present study can also be applied to seawater samples with various salinities and volumes. For 20 L seawater and 24 h counting time on a γ-spectrometer, the limit of detection for 106Ru in seawater was 5.74 mBq/L. In contrast to the traditional CoS method, the usage of NiS does not require any heating process; thus, the pretreatment time is substantially reduced. In addition, by using our method, 106Ru can be determined in the presence of other radionuclides, further enhancing processing efficiency.

The detection of Fukushima-derived radiocesium in the Bering Sea and Arctic Ocean six years after the nuclear accident.

After the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, radionuclides released by this event were observed in the Pacific Ocean. Models predicted that these radionuclides would be transported to the Bering Sea; however, limited evidence currently reveals the transportation of these radionuclides to the Arctic Ocean. Here, we provide the first direct observation showing that FDNPP-derived 134Cs and 137Cs were present in subarctic regions and the Arctic Ocean (Chukchi Sea) in 2017. Furthermore, we conclude that these radionuclides were transported from the Pacific Ocean into the Bering and Chukchi Seas by ocean currents. Additionally, the 137Cs activity concentrations in the Bering Sea exceed those in all previous reports. Due to the continuous leaking of radionuclides from the FDNPP, we hypothesize that FDNPP-derived radionuclides will be continuously transported to the Arctic Ocean in the next several years. Our results suggest that though far away from Fukushima, the accident-derived anthropogenic radionuclides also influenced the Arctic Ocean by ocean currents.

Vertical profiles of 90Sr activities in seawater in the Greenland Sea, Chukchi Sea and Arctic Ocean.

The 90Sr activities of seawater were investigated in the high-latitude region of the Arctic Ocean from August-September 2017. The 90Sr activities in seawater in the Chukchi Sea, central Arctic Ocean and East Greenland Sea were 0.31-2.42, 0.12-1.86 and 0.13-1.20 Bq m-3, respectively. The average 90Sr activity (0.92 Bq m-3) below 500 m in the central Arctic Ocean was higher than those in previous reports. Our study provided high-resolution baseline 90Sr activity data for the whole water column in the high-latitude region of the Arctic Ocean (~85°N). The inventory of 90Sr in the central Arctic Ocean was higher than those in the Chukchi Sea and East Greenland Sea. The results of our study indicated that 90Sr could be transported to the deep seawater and remain in the Arctic Ocean for a long time.

A Nafion-coated bismuth film electrode for the determination of heavy metals in vegetable using differential pulse anodic stripping voltammetry: An alternative to mercury-based electrodes.

Mercury electrodes have been traditionally employed for achieving high reproducibility and sensitivity of the stripping technique. However, new alternative electrode materials are highly desired because of the toxicity of mercury. Bismuth is an electrode material characterized by its low toxicity and its ability to form alloys with some metals such as cadmium, lead and zinc, allowing their preconcentration at the electrode surface. In this work, we reported the simultaneous determination of Pb(II), Cd(II) and Zn(II) at the low µg/l concentration levels by differential pulse anodic stripping voltammetry (DPASV) on a Nafion-coated bismuth film electrode (NCBFE) plated in situ, and investigated the application of NCBFE to heavy metals analysis in vegetable samples. The analytical performance of NCBFE was evaluated for simultaneous determination of Pb(II), Cd(II) and Zn(II) in non-deaerated solution, with the limits of determination of 0.30µg/l for Zn, 0.17µg/l for Cd and Pb at a preconcentration time of 180s. High reproducibility for NCBFE was indicated from the relative standard deviations of 2.4% for Pb, 2.0% for Cd and 3.4% for Zn at the 15µg/l level (n=15). The NCBFE was successfully applied to determine Pb and Cd in vegetable samples, and the results were in agreement with those of graphite furnace atomic absorption spectrometry (GFAAS).