共查询到20条相似文献，搜索用时 38 毫秒
1.
2.
This paper highlights an analytical method based on mass measurement that can be used to directly quantify 129I in groundwater samples at concentrations below the maximum contaminant level (MCL) without the need for sample pre-concentration or extraction. Samples were analyzed on a Perkin Elmer ELAN DRC II ICP-MS after minimal dilution using O2 as the reaction gas. Analysis of continuing calibration verification standards indicated that the dynamic reaction cell (DRC) mode could be used for quantitative analysis of 129I in samples below the MCL (0.0057 ng/mL or 1 pCi/L). The low analytical detection limit of 129I analysis in the DRC mode coupled with minimal sample dilution (1.02x) resulted in a final estimated quantification limit of 0.0051 ng/mL. Subsequent analysis of three groundwater samples containing 129I resulted in fully quantitative results in the DRC mode, and spike recovery analyses performed on all three samples confirmed that the groundwater matrix did not adversely impact the analysis of 129I in the DRC mode. This analytical approach has been proven to be a cost-effective, high-throughput technique for the direct, quantitative analysis of 129I in groundwater samples at environmentally relevant concentrations that reach below the current MCL. 相似文献
3.
Iodine enrichment in the Atacama Desert of northern Chile is widespread and varies significantly between reservoirs, including nitrate-rich “caliche” soils, supergene Cu deposits and marine sedimentary rocks. Recent studies have suggested that groundwater has played a key role in the remobilization, transport and deposition of iodine in Atacama over scales of millions-of-years. However, and considering that natural waters are also anomalously enriched in iodine in the region, the relative source contributions of iodine in the waters and its extent of mixing remain unconstrained. In this study we provide new halogen data and isotopic ratios of iodine (129I/I) in shallow seawater, rivers, salt lakes, cold and thermal spring water, rainwater and groundwater that help to constrain the relative influence of meteoric, marine and crustal sources in the Atacama waters. Iodine concentrations in surface and ground waters range between 0.35 μM and 26 μM in the Tarapacá region and between 0.25 μM and 48 μM in the Antofagasta region, and show strong enrichment when compared with seawater concentrations (I = ∼0.4 μM). In contrast, no bromine enrichment is detected (1.3–45.7 μM for Tarapacá and 1.7–87.4 μM for Antofagasta) relative to seawater (Br = ∼600 μM). These data, coupled to the high I/Cl and low Br/Cl ratios are indicative of an organic-rich sedimentary source (related with an “initial” fluid) that interacted with meteoric water to produce a mixed fluid, and preclude an exclusively seawater origin for iodine in Atacama natural waters. Iodine isotopic ratios (129I/I) are consistent with halogen chemistry and confirm that most of the iodine present in natural waters derives from a deep initial fluid source (i.e., groundwater which has interacted with Jurassic marine basement), with variable influence of at least one atmospheric or meteoric source. Samples with the lowest isotopic ratios (129I/I from ∼215 to ∼1000 × 10−15) strongly suggest mixing between the groundwater and iodine storage in organic-rich rocks (with variable influence of volcanic fluids) and pre-anthropogenic meteoric water, while samples with higher values (∼2000–93,700 × 10−15) indicate the input of anthropogenic meteoric fluid. Taking into account the geological, hydrologic and climatic features of the Atacama region, we propose that the mean contribution of anthropogenic 129I is associated with 129I releases during nuclear weapon tests carried out in the central Pacific Ocean until the mid 1990's (129I/I = ∼12,000 × 10−15). This source reflects rapid redistribution of this radioisotope on a global scale. Our results support the notion of a long-lived continental iodine cycle in the hyperarid margin of western South America, which is driven by local hydrological and climate conditions, and confirm that groundwater was a key agent for iodine remobilization and formation of the extensive iodine-rich soils of Atacama. 相似文献
4.
Data are presented here on the anthropogenic 129I inventory in regions that have been strongly affected by releases from European reprocessing facilities which, to the authors’ knowledge, presently account for >90% of the global isotope source in the Earth’s surface environment. The results show that >90% of the isotope inventory occurs in marine waters with the Nordic Seas and Eurasian basin of the Arctic Ocean containing most of the 129I. Within the terrestrial environment of Europe, soils contain the largest part of the isotope inventory. However, the inventory of the terrestrial system did not provide clues on the most plausible atmospheric source of 129I to Europe, thus supply from both gaseous and marine releases is proposed. The sum of the total inventory in both the marine and terrestrial environments did not match the estimated releases. This imbalance is likely to relate to unconstrained inventory estimates for marine basins (Irish Sea, English Channel and North Sea) close to the facilities, but also to the occurrence of 129I in the biosphere, and possible overestimated releases from the nuclear reprocessing facilities. There is no doubt that the available data on 129I distribution in the environment are far from representative and further research is urgently needed to construct a comprehensive picture. 相似文献
5.
Technetium isotopes 97Tc, 98Tc and 99Tc decay to 97Mo, 98Ru and 99Ru, with half-lives of 2.6 My, 4.1 My, and 0.21 My respectively. If there were early solar system processes that resulted in significant fractionation of Tc from the daughter elements, decay of extant Tc could have led to the creation of Mo and Ru isotopic heterogeneities. To assess the potential of metallic core crystallization to fractionate these elements, we examine the partitioning behavior of Tc relative to Re, Mo and Ru in the Fe-Ni-S system between solid metal and liquid metal alloy. The experimental evidence shows that Tc behaves more like the modestly compatible siderophile element Ru than the more highly compatible siderophile element Re, and that Tc is substantially more compatible than Mo. We also demonstrate a pressure effect in the partitioning of Mo during the crystallization of Fe-Ni-S melts. For a sulfur concentration in the liquid fraction of the core of 10 wt% (16.3 at%), the Jones and Malvin (1990) parameter is −ln(1-2 × 1.09 × 0.163) ≅ 0.44, which yields: D(Re) ≅ 4.1; D(Ru) ≅ 2.3; D(Tc) ≅ 1.7; D(Mo)Lo-P ≅ 1.0;.and D(Mo)Hi-P ≅ 0.5. Our results suggest that detectable Tc-induced isotopic anomalies (≥0.1 ε unit) in Ru and Mo could only be produced by unrealistically extreme degrees of crystallization of metal during asteroidal core fractionation, regardless of the time scales and initial Tc abundances involved. 相似文献
6.
Previous studies have shown that brines in an Ordovician paleokarst reservoir of the Lunnan oilfield in the Tarim Basin, China, are the product of mixing of paleo-evaporated seawater in the east with paleometeoric waters in the west. In order to put time constraints on the brine and related hydrocarbons in this field, 10 brine samples were collected, for which the iodine concentrations and 129I/I ratios were measured and discussed. The iodine concentration (3.70–31.2 mg/L) and the 129I/I ratio (189–897 × 10−15) show that the iodine in the paleoseawater and meteoric water (MW) had different origins and 129I characteristics. The paleoseawater has a high iodine content (∼31 mg/L), indicating that iodine was introduced into the reservoir along with thermally generated hydrocarbons, possibly in the Cretaceous, from the Caohu Sag in the eastern area. Based on consideration of all possible origins of iodine and 129I in the brines, it is suggested that the meteoric water maintained its initial iodine content (0.01 mg/L) and 129I/I ratio (1500 × 10−15), whereas the iodine-enriched paloseawater (IPSW) exhibited a secular 129I equilibrium (Nsq = 39 atom/μL) as a result of fissiogenic 129I input in the reservoir over a long period of time. The model of brine evolution developed on that basis confirmed that meteoric water entered the reservoir in the Miocene at about 10 Ma, and partially mixed with the iodine-enriched paleoseawater. The movement of meteoric water was facilitated by faults created during the Himalayan orogeny, then became more dense after dissolving Paleogene halite and infiltrated into the reservoir at high pressure. The iodine and 129I concentration in the brine contains information about the path and history of the fluid in the reservoir. This may be useful in oil exploration, since the movement of water was, to some extent, related to hydrocarbon migration. 相似文献
7.
Sediments are an excellent archive for evaluation of time-series environmental contamination of water systems. Measurements of ultra-trace radioactive species, such as 129I, provide information for both chronologic calibration and anthropogenic emissions during the nuclear era. Here data are presented on 129I and other chemical parameters from two sediment cores collected in the Baltic Sea during 1997. The sediment sections have a relatively uniform grain size (clay–mud) and cover a period of about 50 a. Distribution of 129I in the sediment strongly relates to the liquid release records from the nuclear reprocessing facilities at Sellafield and La Hague. However, syn- and post-depositional alteration of organic matter at the sediment–water interface and within the sediment column may have contributed to slightly obliterating the anthropogenic 129I signals. Indication of Chernobyl-derived 129I occurs in the sediment profile, but is apparently overridden by the overwhelming flux from the nuclear reprocessing facilities. Although the record did not cover the pre-nuclear era (before 1945) sections, the ultra sensitive 129I profile provides a potential tool for relative dating and monitoring sources of water and sediment to the region. 相似文献
8.
The analysis of excess 129Xe in meteoritic nanodiamonds and the kinetics of its release during stepwise pyrolysis allow to suggest that (1) in the solar nebula 129I atoms were adsorbed onto nanodiamond grains and (or) chemisorbed by forming covalent bonds with carbon atoms. Most 129I atoms existed in a surface connected state, but a minor amount of them was in nanopores of the grains. At radioactive decay of 129I the formed 129Xe (129Xe∗) was trapped by diamond grains due to nuclear recoil. (2) During thermal metamorphism or aqueous alteration, the surface-sited 129I atoms were basically lost. On the basis of these assumptions and calculated concentrations of 129Xe∗ in meteoritic nanodiamonds it is shown that the minimum closing time of the I-Xe system for meteorites of different chemical classes and low petrologic types may be about one million years relative to the minimally thermally metamorphized CO3 meteorite ALHA 77307. With increasing metamorphic grade the closing time of the I-Xe system increases and can range up to several ten millions years. This tendency is in agreement with an onion-shell model of structure and cooling history of meteorite parent bodies where the temperature increases in the direction from surface to center of the asteroids. 相似文献
9.
《Chemical Geology》2007,236(3-4):350-366
A gas hydrate field with highly active venting of methane was recently found near Sado Island in the eastern Japan Sea. Piston cores were collected from active venting sites and nearby locations in the Umitaka Spur–Joetsu Knoll area during two cruises in 2004 (UT04) and 2005 (KY05-08). We report here halogen concentrations and 129I/I ratios in pore waters associated with gas hydrates from these expeditions. The strongly biophilic behavior of I and, to a lesser degree, of Br together with the presence of the long-lived iodine radioisotope (129I) allow evaluation of potential source materials for methane in gas hydrate systems. Depth profiles of all three halogens, particularly the very rapid downward increases of Br and I concentrations, strongly suggest input of deep fluids enriched in Br and I, but the profiles also display the effects of gas hydrate formation and dissociation. Although the 129I/I ratios are modified by 129I from seawater and sediments at shallow depth, likely ratios of the deep fluids are estimated to be between 400 × 10− 15 and 600 × 10− 15, equivalent to a Late Oligocene to Early Miocene age. Ages in the active methane venting sites typically are closer to the old end of this range than those in the reference sites. This age range suggests that the methane associated with venting and gas hydrate formation in this area is derived from organic materials accumulated during the initial opening of the Japan Sea. The Umitaka Spur–Joetsu Knoll gas hydrate field demonstrates the movement of deep fluids associated with the release of significant amounts of methane from the seafloor, processes which might be important components of mass transfer and carbon cycle in the shallow geosphere. 相似文献
10.
Homogeneous 129I / 127I ratios from 6.51 ± 1.36 × 10− 14 to 12.6 ± 1.49 × 10− 14 were measured in formation brine at the Pol-Chuc, Abkatún, Taratunich–Batab off-shore oil reservoirs, Bay of Campeche in S-Mexico. Cosmogenic production could account for a homogeneous, Late Cretaceous/Paleocene time period (71.3 ± 5.3 to 56.3 ± 2.9 Ma) for the sedimentation and burial of organic material in the source formation. As the actual reservoir column is formed by Paleocene to Kimmeridgian sediments, the lower part of the lithological column must have received hydrocarbons that migrated downward from an initial source rock (Upper Cretaceous?) during a post-Paleocene event, probably during Miocene. Cosmogenic production from Tithonian shales can be excluded, as 129I would have been decayed. As an alternative or complementary process, the subsurface, radiogenic production of 129I / 127I by 238U-fission in Uranium-enriched sediments should also be considered to explain the present, low 129I / 127I ratios. 相似文献
11.
《Geochimica et cosmochimica acta》1999,63(13-14):1927-1938
Large quantities of iodine-129 have been released during nuclear weapons testing, and from nuclear power and fuel reprocessing plants. The distribution of this isotope was investigated in 110 surface water and soil samples from western New York (where several potential point sources are located) and other areas of North America, to evaluate its sources, transport pathways, and reservoirs. Elevated 129I concentrations associated with a former reprocessing facility at West Valley, NY, can be tracked to Lakes Erie and Ontario via site drainage, and for over 200 km via atmospheric transport, while only a negligible signal is associated with active power plants in the area. The results point to local reprocessing as the major source of 129I in western New York, while bomb fallout constitutes less than 0.5% of the signal. Surface soil is the dominant reservoir for anthropogenic 129I in this region. Across North America, 129I concentrations are lower than in western New York, although still significantly higher than expected weapons fallout. Reprocessing releases are currently seen to be the major source for elevated 129I concentrations on a global scale, in contrast to previous suggestions that most anthropogenic 129I was still derived from weapons fallout. Concentrations of 129I and iodine in surface reservoirs are generally found to be uncorrelated, implying that natural iodine and anthropogenic 129I are not yet in equilibrium. The results suggest that anthropogenic 129I is cycled between the atmosphere-soil-vegetation systems more rapidly than natural, pre-anthropogenic iodine. 相似文献
12.
Chen Xu Saijin Zhang Eric J. Miller Hsiu-Ping Li Shigeyoshi Otosaka Robin Brinkmeyer Peter H. Santschi 《Geochimica et cosmochimica acta》2011,75(19):5716-9983
129I is one of the three major radiation risk contributors to the public as a consequence of past nuclear processing activities at Department of Energy (DOE) facilities. Elevated levels of 129I are present in the surface soils of F-Area of Savannah River Site, which used to be an isotope separation facility for the production of nuclear weapons components. The 129I in soils is thought to be bound predominantly to soil organic matter (SOM). Measurements of stable 127I and radioactive 129I in humic acids (HAs) and fulvic acids (FAs) obtained by five successive alkaline, two glycerol and one citric acid-alkaline extraction, demonstrated that these extractable humic substances (HS) together account for 54-56% and 46% of the total 127I and 129I in the soil, respectively. The remainder was likely bound to residual SOM. The iodine content (μg-I/g-C) generally decreased with each subsequent extract, while 129I/127I increased concurrently. The coincident variations in chemical compositions, aromaticity (estimated by UV spectroscopy), functional groups (e.g., aliphatic), degree of humification, relative migration in the hydrophobic interaction column, and molecular weight indicated that: (1) iodine in different HAs was bound to a small-size aromatic subunit (∼10 kDa); (2) the large-size subunit (∼90 kDa), which likely linked the small-size unit through some weak chemical forces (hydrogen bonds, hydrophobic or electrostatic interactions), determined the relative mobility of iodine bound to organic matter; (3) from the strong correlation between iodine content and aromaticity in the HAs, we suggested that iodine incorporation into the SOM via covalent aromatic C-I bond is the key mechanism controlling iodine behavior in this system. However, this relationship is not universal for all fractions of organic matter as evidenced from the different slopes of this relationship at the two sampling sites, as well as from the different relationships for HAs and FAs, respectively. These differences in iodination are due to different SOM molecular sizes, compositions, and availability of preferred iodination sites. 129I in the soil downstream from the contaminated site and near a wetland abruptly dropped below our detection limit (0.5 pCi-129I/g-soil), which suggests that the high SOM in the plume soil around the 129I-contaminated F-Area might be a natural barrier to scavenge radioiodine released from the nuclear waste repository by forming organo-iodine compounds. Soil resuspension experiments showed that mobile 129I was mostly associated with a low average molecular weight amphiphilic organic carrier (13.5-15 kDa). SOM clearly behaves as a sink for iodine at the Savannah River Site F-Area. However, this work demonstrates that a small fraction of the SOM can also behave as a source, namely that a small fraction that may be readily dispersible under some environmental conditions and presumably release iodine in the organic-colloidal form. This radioiodinated organo-colloid likely can get into the groundwater through infiltration or surface runoff where it might migrate further into the wetlands. Results from this study provide the geochemical basis for future 129I migration controls, remediation, and/or land-groundwater management strategies. 相似文献
13.
R. N. Nair Faby Sunny Manish Chopra L. K. Sharma V. D. Puranik A. K. Ghosh 《Environmental Earth Sciences》2014,71(3):1007-1019
High concentrations of several radionuclides were reported in the sea near the Fukushima Daiichi Nuclear Power Station (FDNPS) in Japan due to the nuclear accident that occurred on 11 March 2011. The main source of these concentrations was leakage of highly radioactive liquid effluent from a pit in the turbine building near the intake canal of Unit-2 of FDNPS through a crack in the concrete wall. In the immediate vicinity of the plant, seawater concentrations reached 68 MBq m?3 for 134Cs and 137Cs, and exceeded 100 MBq m?3 for 131I in early April 2011. These concentrations began to fall as of 11 April 2011 and, at the end of April, had reached a value close to 0.1 MBq m?3 for 137Cs. Following the nuclear accident, the Tokyo Electric Power Company (TEPCO) had initiated intense monitoring of the environment including the Pacific Ocean. Seawater samples were collected and the concentrations of few radionuclides were measured on a wide spatial and temporal scale. In this study, the measured concentrations of different radionuclides near the south discharge canal of the FDNPS were used to estimate their leakages into the Pacific Ocean. The method is based on estimating the release rates that reproduce the concentration of radionuclides in seawater at a chosen location using a two-dimensional advection–dispersion model in an iterative manner. The radioactive leakages were estimated as 5.68 PBq for 131I, 2.24 PBq for 134Cs and 2.25 PBq for 137Cs. Leakages were also estimated for 99mTc, 136Cs, 140Ba and 140La and they range between 0.02 PBq (99mTc) and 0.53 PBq (140Ba). It was estimated that about 11.28 PBq of radioactivity in total was leaked into the Pacific Ocean from the damaged FDNPS. Out of this, 131I constitutes 50.3 %; 134Cs 20 %; 137Cs 20 %; 140Ba 4.6 %; 136Cs 2.6 %; 140La 2.3 % and 99mTc 0.2 % of the total radioactive leakage. Such quantitative estimates of radioactive leakages are essential prerequisites for short-term and local-scale as well as long-term and large-scale radiological impact assessment of the nuclear accident. 相似文献
14.
Use of Hydrofluoric Acid Desilicification in the Determination of Highly Siderophile Element Abundances and Re‐Pt‐Os Isotope Systematics in Mafic‐Ultramafic Rocks 
下载免费PDF全文
下载免费PDF全文 James M.D. Day Christopher L. Waters Bruce F. Schaefer Richard J. Walker Simon Turner 《Geostandards and Geoanalytical Research》2016,40(1):49-65
Properly combining highly siderophile element (HSE: Re, Pd, Pt, Ru, Ir, Os) abundance data, obtained by isotope dilution, with corresponding 187Os/188Os and 186Os/188Os measurements of rocks requires efficient digestion of finely‐ground powders and complete spike‐sample equilibration. Yet, because of the nature of commonly used methods for separating Os from a rock matrix, hydrofluoric acid (HF) is typically not used in such digestions. Consequently, some silicates are not completely dissolved, and HSE residing within these silicates may not be fully accessed. Consistent with this, some recent studies of basaltic reference materials (RMs) have concluded that an HF‐desilicification procedure is required to fully access the HSE (Ishikawa et al. (2014) Chemical Geology, 384, 27–46; Li et al. (2015) Geostandards and Geoanalytical Research, 39, 17–30). Highly siderophile element abundance and Os isotope studies of intraplate basalts typically target samples with a range of MgO contents (< 8 to > 18% m/m, or as mass fractions, < 8 to > 18 g per 100 g), in contrast to the lower MgO mass fractions (< 10 g per 100 g) of basalt and diabase RMs (i.e., BIR‐1, BHVO‐2, TDB‐1). To investigate the effect of HF‐desilicification on intraplate basalts, experiments were performed on finely ground Azores basalts (8.1–17 g per 100 g MgO) using a ‘standard acid digestion’ (2:1 mixture of concentrated HNO3 and HCl), and a standard acid digestion, followed by HF‐desilicification. No systematic trends in HSE abundances were observed between data obtained by standard acid digestion and HF‐desilicification. Desilicification procedures using HF do not improve liberation of the HSE from Azores basalts, or some RMs (e.g., WPR‐1). We conclude that HF‐desilicification procedures are useful for obtaining total HSE contents of some young lavas, but this type of procedure is not recommended for studies where Re‐Pt‐Os chronological information is desired. The collateral effect of a standard acid digestion to liberate Os, followed by HF‐desilicification to obtain Re and Pt abundances in samples, is that the measured Re/Os and Pt/Os may not correspond with measured 187Os/188Os or 186Os/188Os. 相似文献
15.
Christoph Schnabel Valérie Olive Mariko Atarashi-Andoh Andrew Dougans Robert M. Ellam Stewart Freeman Colin Maden Martin Stocker Hans-Arno Synal Lukas Wacker Sheng Xu 《Applied Geochemistry》2007
This work constitutes the first survey of I isotope ratios for Scottish sea water including the first data for the west of Scotland. These data are of importance because of the proximity to the world’s second largest emission source of 129I to the sea, the Sellafield nuclear reprocessing plant, because of the increasing importance of the sea to land transfer of 129I and also as input data for dose estimates based on this pathway of 129I. 129I/127I ratios in SW Scotland reached 3 × 10−6 in 2004. No strong variation of I isotope ratios was found from 2003 to 2005 in Scottish sea waters. Iodine isotope ratios increased by about a factor of 6 from 1992 to 2003 in NE Scotland, in agreement with the increase of liquid 129I emissions from Sellafield over that time period. It is demonstrated that 129I/127I ratios agree better than 129I concentrations for samples from similar locations taken in very close temporal proximity, indicating that this ratio is more appropriate to interpret than the radionuclide concentration. 相似文献
16.
A. Ya. Bolsunovskii Yu. V. Aleksandrova A. G. Degermendzhi 《Doklady Earth Sciences》2010,434(1):1219-1221
The content of a long-lived technogenic radionuclide 99Tc in the Yenisei within the territory of radioactive effluents of the Rosatom mining chemical combine (MCC) has been studied.
In 2008–2009 the maximal 99Tc content in water was registered near the dumping site of the MCC and came to 33 mBq/l. According to analysis of filtered
water samples, technetium in the Yenisei water is presented as pertechnetate ion (TcO4). When moving away from the MCC downstream, the 99Tc content in water is decreased, which is caused both by dilution of waste water and by 99Tc accumulation by aquatic plants. The 99Tc content in the biomass of the aquatic plant Potamogeton lucens came to 8215 Bq/kg, and the concentration factor (CF) to 8200, which is three times more than the maximal values of the CF of 99Tc by the plants in laboratory conditions (2700). 相似文献
17.
半封闭硝酸溶解体系ICP-MS快速测定辉钼矿的Re-Os年龄及Re含量 总被引：4，自引：4，他引：0
Re-Os法能够直接厘定内生金属矿床成矿时代,但是封闭Carius管法化学流程复杂,且有一定的危险性。本文建立了一种简便快速测定辉钼矿Re-Os年龄及其Re含量的方法。用3 mL浓硝酸在10 mL比色管中溶解5~15 mg辉钼矿样品,将溶液中的钼酸沉淀分离后稀释定容,直接采用质谱测量187和185质量数比值(M187/M185)。利用辉钼矿Re-Os年龄标准物质JDC和HLP的M187/M185值与其年龄的正相关线性关系计算未知辉钼矿样品的Re-Os年龄,并通过185Re计数利用相对法计算Re含量。本方法应用于测量13.26~2130 Ma的辉钼矿,Re-Os年龄的测定值与推荐值的相对偏差多数在0.36%~7.42%之间,由于放射性积累较多,长年龄样品测量的准确度较高。与传统Carius管法相比,该方法不需要加入稀释剂,省去了封闭和打开Carius管环节以及Re-Os分离纯化流程,适合于辉钼矿Re-Os年龄的初步分析。 相似文献
18.
Xenon isotopic data were acquired by high resolution step pyrolysis and combined step pyrolysis/combustion of aliquots of size separated nanodiamonds. 129Xe excess (129Xe*) from in situ decay of 129I is preferentially associated with the larger grain size separates. This observation rules out trapping by recoil from surrounding material. The releases of Xe-P3 and 129Xe occur in the same low temperature pyrolysis steps and exhibit similar distributions among the size separates. These observations imply a common site for the components and, in consequence, suggest a common incorporation event.Whether one component or two, our observations require that 129Xe* and Xe-P3 were incorporated into a subpopulation of nanodiamonds before nanodiamonds were mixed and incorporated into parent bodies. Their susceptibilities to loss during heating in the laboratory are similar, but the ratio of 129Xe* to Xe-P3 varies among nanodiamond separates from different meteorites (literature data). We conclude that the 129Xe* we observe today was present as 129I during parent body processing. Furthermore, the range of 129Xe*/132XeP3 ratios across all the separates requires that even nanodiamonds from CI chondrites were at least 5-10× more rich in Xe-P3 during 129I decay than they are today.We present a simple model involving one degassing event per parent body between incorporation of nanodiamonds and final decay of 129I. The observed variations among parent bodies require degassing events separated by several 129I half lives (∼50Ma), consistent with low-temperature processing on parent bodies but longer than expected for nebular processing. In this model, nanodiamonds from ALHA77307 degassed at an unusually early stage, suggesting they alone may retain the signature of processing in the nebula in their P3 and 129Xe* abundances.The isotopic signature associated with Xe-P6 is also found only in the larger size separates. Concentration of Xe-HL increases with increasing grain size, but its relative abundance with respect to Xe-P3 and P6 is higher in smaller grain-size fractions. We argue that Xe-P6 is best seen as a variant of Xe-HL, and that they are both mixtures of a “normal” component akin to solar xenon and a slightly variable exotic component. We show that both current models of Xe-H formation can account for the observed variability, and propose a scenario according to which Xe-HL and P6 were implanted into separate diamond populations before incorporation of Xe-P3 and 129I. 相似文献
19.
M. Atarashi-Andoh C. Schnabel G. Cook A.B. MacKenzie A. Dougans R.M. Ellam S. Freeman C. Maden V. Olive H.-A. Synal S. Xu 《Applied Geochemistry》2007
Accelerator Mass Spectrometry (AMS) was used to measure 129I/127I ratios in surface sea, lake, and river water samples collected in 2004 and 2005 from the English Lake District and from SW Scotland, areas which are in relatively close proximity to the Sellafield nuclear fuel reprocessing plant in NW England. The 129I/127I ratios in surface water collected from the shore of the Irish Sea were in the range 2.8 × 10−6 to 8.2 × 10−6. These ratios are one order of magnitude higher than that of seawater collected from the Irish Sea in 1992, correlating with the increase in 129I content of the Sellafield liquid effluent discharge over the last decade. The 129I/127I ratios in lakes in the Lake District were in the range 0.7 × 10−6 to 6.4 × 10−6 and decreased exponentially as a function of distance from Sellafield. Consideration of the relative variation of stable I concentrations and 129I/127I ratios suggests that Sellafield gaseous discharges may be the dominant source of 129I to the lakes. 相似文献
20.
A key component to closing the nuclear fuel cycle is the storage and disposition of nuclear waste in geologic systems. Multiphase ceramic waste forms have been studied extensively as a potential host matrix for nuclear waste. Understanding the speciation, partitioning, and release behavior of radionuclides immobilized in multiphase ceramic waste forms is a critical aspect of developing the scientific and technical basis for nuclear waste management. In this study, we evaluated a sodalite-bearing multiphase ceramic waste form (i.e., fluidized-bed steam reform sodium aluminosilicate [FBSR NAS] product) as a potential host matrix for long-lived radionuclides, such as technetium (99Tc). The FBSR NAS material consists primarily of nepheline (ideally NaAlSiO4), anion-bearing sodalites (ideally M8[Al6Si6O24]X2, where M refers to alkali and alkaline earth cations and X refers to monovalent anions), and nosean (ideally Na8[AlSiO4]6SO4). Bulk X-ray absorption fine structure analysis of the multiphase ceramic waste form, suggest rhenium (Re) is in the Re(VII) oxidation state and has partitioned to a Re-bearing sodalite phase (most likely a perrhenate sodalite Na8[Al6Si6O24](ReO4)2). Rhenium was added as a chemical surrogate for 99Tc during the FBSR NAS synthesis process. The weathering behavior of the FBSR NAS material was evaluated under hydraulically unsaturated conditions with deionized water at 90 °C. The steady-state Al, Na, and Si concentrations suggests the weathering mechanisms are consistent with what has been observed for other aluminosilicate minerals and include a combination of ion exchange, network hydrolysis, and the formation of an enriched-silica surface layer or phase. The steady-state S and Re concentrations are within an order of magnitude of the nosean and perrhenate sodalite solubility, respectively. The order of magnitude difference between the observed and predicted concentration for Re and S may be associated with the fact that the anion-bearing sodalites contained in the multiphase ceramic matrix are present as mixed-anion sodalite phases. These results suggest the multiphase FBSR NAS material may be a viable host matrix for long-lived, highly mobilie radionuclides which is a critical aspect in the management of nuclear waste. 相似文献