Surface water was collected from the Jiulong Estuary for determination of activity concentrations of uranium isotopes in different size fractions, namely, greater than 53, 10 -53, 2 - 10, 0.4 -2 μm, 10 000 u -0.4 μm...Surface water was collected from the Jiulong Estuary for determination of activity concentrations of uranium isotopes in different size fractions, namely, greater than 53, 10 -53, 2 - 10, 0.4 -2 μm, 10 000 u -0.4 μm and less than 10 000 u fractions by microfihration and cross-flow uhrafiltration technologies. Results indicated that most of the dissolved uranium ( 〈 0.4 μm) exis- ted in the low molecular mass fraction ( 〈 10 000 u), and the colloidal uranium-238 (10 000 u -0.4 μm) only contributed less than 1% of the dissolved uranium-238. The fractions of colloidal uranium in the dissolved phases decreased with the increasing sa- linity. A positive linear relationship between uranium-238 activities and salinities was observed for the dissolved, colloidal and low molecular mass fractions, indicating a conservative behavior of uranium in the Jiulong Estuary. In the particulate phases ( 〉 0.4 μm), the partitioning of uranium isotopes among different size fractions was controlled by the partitioning of particle concentrations. In the regions with salinities below 20, the partitioning of uranium-238 among different size fractions was as follows: 10 - 53 μm 〉 2 - 10 μm 〉 0.4 - 2 μm greater than above 53 μm. However, the order at the offshore station with salinities above 30 changed as follows : 0.4 - 2 μm 〉 10 - 53 μm 〉 2 - 10 μm greater than above 53 μm. The fraction of the 0.4 - 2 μm particles increased at the offshore station, suggesting the increased contribution of the authigenic uranium. The activity ratio of uranium-234 to uranium-238 in the dissolved phases, including the low molecular mass fraction and the colloidal fraction, was larger than unity, showing the occurrence of excess uranium-234. In contrast, the activity ratio of uranium-234 to uranium-238 in all size fractions of the particulate phase was close to the equilibrium value (1.0). The observed different values of the activity ratio of uranium-234 to uranium-238 in the dissolved phase and the particulate phase were ascribed to the preferential leaching of uranium-234 and the small amount of the leaching particulate uranium. The mass ratio of thorium-232 to uranium-238 also showed different values between the dissolved phase and the particulate phase. Mass ratio of thorium-232 to uranium-238 in the dissolved, colloidal and low molecular mass fractions was less than unity, while those in the different size fractions of particulate phases were larger than unity, reflecting a different behavior between uranium and thorium during their transport into the ocean.展开更多
Seawater samples are collected in the spring of 2013 from the Taiwan Strait for the analysis of uranium(U)concentrations and isotopic compositions using MC-ICP-MS, and the geochemical behavior patterns of U in the T...Seawater samples are collected in the spring of 2013 from the Taiwan Strait for the analysis of uranium(U)concentrations and isotopic compositions using MC-ICP-MS, and the geochemical behavior patterns of U in the Taiwan Strait are then investigated. Average concentrations of individual U isotopes are(3.23±0.14) μg/kg for 238 U,(2.34±0.09)×10^(–2) μg/kg for ^(235)U and(2.05±0.07)×10^(–4) μg/kg for 234 U. Correspondingly, the U isotopic compositions are 155±18 for δ234U and 138±2 for 238U:235U. The U concentrations and isotopic ratios in the Taiwan Strait are similar to those of open ocean seawater, suggesting the dominance of the open ocean input to the strait's U pool.However, river input, as suggested by the slightly lower salinity than that of the open ocean, also affected the U concentrations and isotopic compositions in the strait. From a compilation of U concentrations in the Taiwan Strait and adjacent areas, including the Jiulong Estuary and Zhujiang Estuary, the Xiamen Bay and the northern South China Sea, a strong and significant relationship between U concentration and salinity [U:S; U=(0.093 4±0.002 4)S+(0.092 0±0.061 5)] is revealed, suggesting conservative mixing of U in the Taiwan Strait. To better understand the U geochemistry in the Taiwan Strait, a multiple endmembers mixing model is applied to estimate the contributions of potential sources. The open ocean seawater contributed 69%–95% of U in the Taiwan Strait, with river water approximately 2%, and dust deposition only around 0.13%. Therefore, the model results supported the open ocean input source and the conservative mixing behavior of U derived from the observation of U concentrations and isotopic ratios and U:S ratios. The sediment interstitial water may be an important source of U to the Taiwan Strait with a possible contribution of 3%–29%, consistent with previous investigations based on radium isotopes.However, further investigations are warranted to examine the U concentration in the sediment interstitial water and its input to the overlying seawater in the Taiwan Strait.展开更多
基金The National Key Basic Research Special Foundation Programof China under contract No.2005CB422305the China Ocean Mineral Resources Research and Development Association Foundation under contract Nos DY105-02-04 and DY105-02-01.
文摘Surface water was collected from the Jiulong Estuary for determination of activity concentrations of uranium isotopes in different size fractions, namely, greater than 53, 10 -53, 2 - 10, 0.4 -2 μm, 10 000 u -0.4 μm and less than 10 000 u fractions by microfihration and cross-flow uhrafiltration technologies. Results indicated that most of the dissolved uranium ( 〈 0.4 μm) exis- ted in the low molecular mass fraction ( 〈 10 000 u), and the colloidal uranium-238 (10 000 u -0.4 μm) only contributed less than 1% of the dissolved uranium-238. The fractions of colloidal uranium in the dissolved phases decreased with the increasing sa- linity. A positive linear relationship between uranium-238 activities and salinities was observed for the dissolved, colloidal and low molecular mass fractions, indicating a conservative behavior of uranium in the Jiulong Estuary. In the particulate phases ( 〉 0.4 μm), the partitioning of uranium isotopes among different size fractions was controlled by the partitioning of particle concentrations. In the regions with salinities below 20, the partitioning of uranium-238 among different size fractions was as follows: 10 - 53 μm 〉 2 - 10 μm 〉 0.4 - 2 μm greater than above 53 μm. However, the order at the offshore station with salinities above 30 changed as follows : 0.4 - 2 μm 〉 10 - 53 μm 〉 2 - 10 μm greater than above 53 μm. The fraction of the 0.4 - 2 μm particles increased at the offshore station, suggesting the increased contribution of the authigenic uranium. The activity ratio of uranium-234 to uranium-238 in the dissolved phases, including the low molecular mass fraction and the colloidal fraction, was larger than unity, showing the occurrence of excess uranium-234. In contrast, the activity ratio of uranium-234 to uranium-238 in all size fractions of the particulate phase was close to the equilibrium value (1.0). The observed different values of the activity ratio of uranium-234 to uranium-238 in the dissolved phase and the particulate phase were ascribed to the preferential leaching of uranium-234 and the small amount of the leaching particulate uranium. The mass ratio of thorium-232 to uranium-238 also showed different values between the dissolved phase and the particulate phase. Mass ratio of thorium-232 to uranium-238 in the dissolved, colloidal and low molecular mass fractions was less than unity, while those in the different size fractions of particulate phases were larger than unity, reflecting a different behavior between uranium and thorium during their transport into the ocean.
基金The National Basic Research Program(973 Program)of China under contract Nos 2014CB953700 and 2014CB953702the National Natural Science Foundation of China under contract Nos 40906040 and 41276063+2 种基金the Natural Science Foundation of Fujian Province under contract No.2015Y0040the Public Science and Technology Research Fund of the State Oceanic Administration of China under contract No.201505034the Fundamental Research Funds for the Central Universities of China and the Scientific Research Foundation for Returned Overseas Chinese Scholars of the Ministry of Education of China
文摘Seawater samples are collected in the spring of 2013 from the Taiwan Strait for the analysis of uranium(U)concentrations and isotopic compositions using MC-ICP-MS, and the geochemical behavior patterns of U in the Taiwan Strait are then investigated. Average concentrations of individual U isotopes are(3.23±0.14) μg/kg for 238 U,(2.34±0.09)×10^(–2) μg/kg for ^(235)U and(2.05±0.07)×10^(–4) μg/kg for 234 U. Correspondingly, the U isotopic compositions are 155±18 for δ234U and 138±2 for 238U:235U. The U concentrations and isotopic ratios in the Taiwan Strait are similar to those of open ocean seawater, suggesting the dominance of the open ocean input to the strait's U pool.However, river input, as suggested by the slightly lower salinity than that of the open ocean, also affected the U concentrations and isotopic compositions in the strait. From a compilation of U concentrations in the Taiwan Strait and adjacent areas, including the Jiulong Estuary and Zhujiang Estuary, the Xiamen Bay and the northern South China Sea, a strong and significant relationship between U concentration and salinity [U:S; U=(0.093 4±0.002 4)S+(0.092 0±0.061 5)] is revealed, suggesting conservative mixing of U in the Taiwan Strait. To better understand the U geochemistry in the Taiwan Strait, a multiple endmembers mixing model is applied to estimate the contributions of potential sources. The open ocean seawater contributed 69%–95% of U in the Taiwan Strait, with river water approximately 2%, and dust deposition only around 0.13%. Therefore, the model results supported the open ocean input source and the conservative mixing behavior of U derived from the observation of U concentrations and isotopic ratios and U:S ratios. The sediment interstitial water may be an important source of U to the Taiwan Strait with a possible contribution of 3%–29%, consistent with previous investigations based on radium isotopes.However, further investigations are warranted to examine the U concentration in the sediment interstitial water and its input to the overlying seawater in the Taiwan Strait.