Generalized Scaling Factor for Estimating the Activity Concentrations of Difficult-to-Measure Nuclides

2002 Mathematics Subject Classification: 62P35, 62P30.

Environmental effects of thermal and radioactive discharges from nuclear power plants in the boreal brackish-water conditions of the northern Baltic Sea

During recent decades, thermal and radioactive discharges from nuclear power plants into the aquatic environment have become the subject of lively debate as an ecological concern. The target of this thesis was to summarize the large quantity of results obtained in extensive monitoring programmes and studies carried out in recipient sea areas off the Finnish nuclear power plants at Loviisa and Olkiluoto during more than four decades. The Loviisa NPP is located on the coast of the Gulf of Finland and Olkiluoto NPP on that of the Bothnian Sea. The state of the Gulf of Finland is clearly more eutrophic; the nutrient concentrations in the surface water are about 1½ 2 times higher at Loviisa than at Olkiluoto, and the total phosphorus concentrations still increased in both areas (even doubled at Loviisa) between the early 1970s and 2000. Thus, it is a challenge to distinguish the local effects of thermal discharges from the general eutrophication process of the Gulf of Finland. The salinity is generally low in the brackish-water conditions of the northern Baltic Sea, being however about 1 higher at Olkiluoto than at Loviisa (the salinity of surface water varying at the latter from near to 0 in early spring to 4 6 in late autumn). Thus, many marine and fresh-water organisms live in the Loviisa area close to their limit of existence, which makes the biota sensitive to any additional stress. The characteristics of the discharge areas of the two sites differ from each other in many respects: the discharge area at Loviisa is a semi-enclosed bay in the inner archipelago, where the exchange of water is limited, while the discharge area at Olkiluoto is more open, and the exchange of water with the open Bothnian Sea is more effective. The effects of the cooling water discharged from the power plants on the temperatures in the sea were most obvious in winter. The formation of a permanent ice cover in the discharge areas has been delayed in early winter, and the break-up of the ice occurs earlier in spring. The prolonging of the growing season and the disturbance of the overwintering time, in conditions where the biota has adjusted to a distinct rest period in winter, have been the most significant biological effects of the thermal pollution. The soft-bottom macrofauna at Loviisa has deteriorated to the point of almost total extinction at many sampling stations during the past 40 years. A similar decline has been reported for the whole eastern Gulf of Finland. However, the local eutrophication process seems to have contributed into the decline of the zoobenthos in the discharge area at Loviisa. Thermal discharges have increased the production of organic matter, which again has led to more organic bottom deposits. These have in turn increased the tendency of the isolated deeps to a depletion of oxygen, and this has further caused strong remobilization of phosphorus from the bottom sediments. Phytoplankton primary production and primary production capacity doubled in the whole area between the late 1960s and the late 1990s, but started to decrease a little at the beginning of this century. The focus of the production shifted from spring to mid- and late summer. The general rise in the level of primary production was mainly due to the increase in nutrient concentrations over the whole Gulf of Finland, but the thermal discharge contributed to a stronger increase of production in the discharge area compared to that in the intake area. The eutrophication of littoral vegetation in the discharge area has been the most obvious, unambiguous and significant biological effect of the heated water. Myriophyllum spicatum, Potamogeton perfoliatus and Potamogeton pectinatus, and vigorous growths of numerous filamentous algae as their epiphytes have strongly increased in the vicinity of the cooling water outlet, where they have formed dense populations in the littoral zone in late summer. However, the strongest increase of phytobenthos has extended only to a distance of about 1 km from the outlet, i.e., the changes in vegetation have been largest in those areas that remain ice-free in winter. Similar trends were also discernible at Olkiluoto, but to a clearly smaller extent, which was due to the definitely weaker level of background eutrophy and nutrient concentrations in the Bothnian Sea, and the differing local hydrographical and biological factors prevailing in the Olkiluoto area. The level of primary production has also increased at Olkiluoto, but has remained at a clearly lower level than at Loviisa. In spite of the analogous changes observed in the macrozoobenthos, the benthic fauna has remained strong and diversified in the Olkiluoto area. Small amounts of local discharge nuclides were regularly detected in environmental samples taken from the discharge areas: tritium in seawater samples, and activation products, such as 60Co, 58Co, 54Mn, 110mAg, 51Cr, in suspended particulate matter, bottom sediments and in several indicator organisms (e.g., periphyton and Fucus vesiculosus) that effectively accumulate radioactive substances from the medium. The tritium discharges and the consequent detection frequency and concentrations of tritium in seawater were higher at Loviisa, but the concentrations of the activation products were higher at Olkiluoto, where traces of local discharge nuclides were also observed over a clearly wider area, due to the better exchange of water than at Loviisa, where local discharge nuclides were only detected outside Hästholmsfjärden Bay quite rarely and in smaller amounts. At the farthest, an insignificant trace amount (0.2 Bq kg-1 d.w.) of 60Co originating from Olkiluoto was detected in Fucus at a distance of 137 km from the power plant. Discharge nuclides from the local nuclear power plants were almost exclusively detected at the lower trophic levels of the ecosystems. Traces of local discharge nuclides were very seldom detected in fish, and even then only in very low quantities. As a consequence of the reduced discharges, the concentrations of local discharge nuclides in the environment have decreased noticeably in recent years at both Loviisa and Olkiluoto. Although the concentrations in environmental samples, and above all, the discharge data, are presented as seemingly large numbers, the radiation doses caused by them to the population and to the biota are very low, practically insignificant. The effects of the thermal discharges have been more significant, at least to the wildlife in the discharge areas of the cooling water, although the area of impact has been relatively small. The results show that the nutrient level and the exchange of water in the discharge area of a nuclear power plant are of crucial importance.

Characterization and iodide adsorption behaviour of HDPY+ modified bentonite

Owing to its favourable physical, chemical and rheological properties, densely compacted bentonite or bentonite-sand mix is considered as a suitable buffer material in deep geological repositories to store high level nuclear waste. Iodine-129 is one of the significant nuclides in the high level waste owing to its long half life and poor sorption onto most geologic media. Bentonite by virtue of negatively charged surface has negligible affinity to retain iodide ions. As organo-bentonites are known to retain iodide ions, the present study characterizes hexadecylpyridinium chloride (HDPyCl.H2O) treated bentonite from Barmer India (referred as HDPy+B) for physico-chemical properties, engineering properties and the iodide adsorption behavior of the organo clay. Batch experiments revealed that HDPy+ ions are largely retained (94 % retention) via cation exchange; the ion-exchange process neutralizes the negative surface charge and bridges clay particles leading to reduction in Atterberg limits, clay content and sediment volume. The organo clay retains iodide by Coulombic attraction (at primary sites) and anion exchange (at secondary sites). The free-energy change (Delta G (o) = -25.5 kJ/mol) value indicated that iodide retention by organo clay is favored physical adsorption process. Iodide adsorption capacity of organo clay decreased significantly (85-100 %) on dilution with 50-80 % bentonite. On the other hand, dilution of bentonite with 50 % organo clay caused 58 % reduction in swell potential and 21 % reduction in swell pressure.

Iodide Retention by Modified Kaolinite in the Context of Safe Disposal of High Level Nuclear Waste

Bentonite clay is identified as potential buffer in deep geological repositories (DGR) that store high level radioactive wastes (HLW) as the expansive clay satisfies the expected mechanical and physicochemical functions of the buffer material. In the deep geological disposal of HLW, iodine-129 is one of the significant nuclides, attributable to its long half-life (half life 1⁄4 1:7 × 107 years). However, the negative charge on the basal surface of bentonite particles precludes retention of iodide anions. To render the bentonite effective in retaining hazardous iodide species in DGR, improvement of the anion retention capacity of bentonite becomes imperative. The iodide retention capac-ity of bentonite is improved by admixing 10 and 20% Ag-kaolinite (Ag-K) with bentonite (B) on a dry mass basis. The present study produced Ag-kaolinite by heating silver nitrate-kaolinite mixes at 400°C. Marginal release of iodide retained by Ag-kaolinite occurred under extreme acidic (pH 1⁄4 2:5) and alkaline (pH 1⁄4 12:5) conditions. The swell pressure and iodide etention results of the B-Ag-K specimens bring out that mixing Ag-K with bentonite does not chemically modify the expansive clay; the mixing is physical in nature and Ag-K presence only contributes to iodide retention of the admixture. DOI: 10.1061/(ASCE)HZ.2153-5515.0000121. © 2012 American Society of Civil Engineers.

Bestimmung von künstlichen Radionukliden in Konsumfisch

The identification of artificial radionuclides in fish involves some diffculties, because the quantities of these nuclides are very low (10-16 to 10-10 g/kg). The procedures have to be done very carefully. The sample preparation, the radiochemical analyses and the final preparation of the samples for the detection of the radioactivity of strontium-90, plutonium-238, -239, -240 and americium-241 are briefly described. The levels of artificial radioactivity in some species of fish from the North Sea are shown. The additional exposure to radiation by artificial radionuc1ides by ingestion of fish amounts only to about 0,02 % of the mean exposure to natural radiation. Nevertheless further monitoring of radioactivity should be continued in order to ensure that changes can be detected in time.

HTGR fuel element depletion benchmark: Stage one results

In this paper, we reported the results of the first stage of HTGR fuel element depletion benchmark obtained with BGCore and HELIOS depletion codes. The results of the k-inf are generally in good agreement. However, significant deviation in concentrations of several nuclides between MCNP based and HELIOS codes was observed.

Implementation of multi-group cross-section methodology in BGCore MC-depletion code

BGCore is a software package for comprehensive computer simulation of nuclear reactor systems and their fuel cycles. The BGCore interfaces Monte Carlo particles transport code MCNP4C with a SARAF module - an independently developed code for calculating in-core fuel composition and spent fuel emissions following discharge. In BGCore system, depletion coupling methodology is based on the multi-group approach that significantly reduces computation time and allows tracking of large number of nuclides during calculations. In this study, burnup calculation capabilities of BGCore system were validated against well established and verified, computer codes for thermal and fast spectrum lattices. Very good agreement in k eigenvalue and nuclide densities prediction was observed for all cases under consideration. In addition, decay heat prediction capabilities of the BGCore system were benchmarked against the most recent edition of ANS Standard methodology for UO2 fuel decay power prediction in LWRs. It was found that the difference between ANS standard data and that predicted by the BGCore does not exceed 5%.

A combined nonfertile and UO2 PWR fuel assembly for actinide waste minimization

A new combined Non Fertile and Uranium (CONFU) fuel assembly is proposed to limit the actinides that need long-term high-level waste storage from the pressurized water reactor (PWR) fuel cycle. In the CONFU assembly concept, ∼20% of the UO2 fuel pins are replaced with fertile free fuel hosting the transuranic elements (TRUs) generated in the previous cycle. This leads to a fuel cycle sustainable with respect to net TRU generation, and the amount and radiotoxicity of the nuclear waste can be significantly reduced in comparison with the conventional once-through UO2 fuel cycle. It is shown that under the constraints of acceptable power peaking limits, the CONFU assembly exhibits negative reactivity feedback coefficients comparable in values to those of the reference UO2 fuel. Feasibility of the PWR core operation and control with complete TRU recycle has been shown based on full-core three-dimensional neutronic simulation. However, gradual buildup of small amounts of Cm and Cf challenges fuel reprocessing and fabrication due to the high spontaneous fission rates of these nuclides and heat generation by some Pu, Am, and Cm isotopes. Feasibility of the processing steps becomes more attainable if the time between discharge and reprocessing is 20 yr or longer.

A sustainable PWR fuel cycle with complete TRU recycling using fertile-free fuel

The feasibility of a conventional PWR fuel cycle with complete recycling of TRU elements in the same reactor is investigated. A new Combined Non-fertile and Uranium (CONFU) fuel assembly where about 20% of the uranium fuel pins are replaced with fertile free fuel (FFF) hosting TRU generated in the previous cycle is proposed. In this sustainable fuel cycle based on the CONFU fuel assembly concept, the amount and radiotoxicity of the nuclear waste can be significantly reduced in comparison with the conventional once-through UO 2 fuel cycle. It is shown that under the constraints of acceptable power peaking limits, the CONFU assembly exhibits negative reactivity feedback coefficients comparable in values to those of the reference UO2 fuel. Moreover, the effective delayed neutron fraction is about the same as for UO2-fueled cores. Therefore, feasibility of the PWR core operation and control with complete TRU recycle has been shown in principle. However, gradual build up of small amounts of Cm and Cf challenges fuel reprocessing and fabrication due to the high spontaneous fissions rates of these nuclides and heat generation by some Pu, Am, and Cm isotopes. Feasibility of the processing steps becomes more attainable if the time between discharge and reprocessing is 20 years or longer. The implications for the entire fuel cycle will have to be addressed in future studies.

Production of new superheavy Z=108-114 nuclei with U-238, Pu-244, and Cm-248,Cm-250 targets

Within the framework of the dinuclear system (DNS) model, production cross sections of new superheavy nuclei with charged numbers Z=108-114 are analyzed systematically. Possible combinations based on the actinide nuclides U-238, Pu-244, and Cm-248,Cm-250 with the optimal excitation energies and evaporation channels are pointed out to synthesize new isotopes that lie between the nuclides produced in the cold fusion reactions and the Ca-48-induced fusion reactions experimentally, which are feasible to be constructed experimentally. It is found that the production cross sections of superheavy nuclei decrease drastically with the charged numbers of compound nuclei. Larger mass asymmetries of the entrance channels enhance the cross sections in 2n-5n channels.

DIRECT MASS MEASUREMENTS OF EXOTIC NUCLEI IN STORAGE RINGS

Mass measurements of exotic nuclei is a fast, developing field which is essential for basic nuclear physics and a wide range of applications. The method of storage ring mass spectrometry has many advantages: (1) a large amount of nuclides can be simultaneously measured; (2) very short-lived (T-1/2 greater than or similar to 50 mu s) and very rare species (yields down to single ions) can be accessed; (3) nuclides in several atomic charge states can be investigated, (4) half-life measurements can be performed with time-resolved mass spectrometry. In this contribution we concentrate on some recent achievements and future perspectives of the storage ring mass spectrometry.

Discovery of Highly Excited Long-Lived Isomers in Neutron-Rich Hafnium and Tantalum Isotopes through Direct Mass Measurements

A study of cooled Au-197 projectile-fragmentation products has been performed with a storage ring. This has enabled metastable nuclear excitations with energies up to 3 MeV, and half-lives extending to minutes or longer, to be identified in the neutron-rich nuclides Hf-183,Hf-184,Hf-186 and Ta-186,Ta-187. The results support the prediction of a strongly favored isomer region near neutron number 116.

Penning trap mass measurements on nobelium isotopes

The Penning trap mass spectrometer SHIPTRAP at GSI Darmstadt allows accurate mass measurements of radionuclides, produced in fusion-evaporation reactions and separated by the velocity filter SHIP from the primary beam. Recently, the masses of the three nobelium isotopes No252-254 were determined. These are the first direct mass measurements of transuranium elements, which provide new anchor points in this region. The heavy nuclides were produced in cold-fusion reactions by irradiating a PbS target with a Ca-48 beam, resulting in production rates of the nuclei of interest of about one atom per second. In combination with data from decay spectroscopy our results are used to perform a new atomic-mass evaluation in this region.

A high performance Time-of-Flight detector applied to isochronous mass measurement at CSRe

A high performance Time-of-Flight detector has been designed and constructed for isochronous mass spectrometry at the experimental Cooler Storage Ring (CSRe) The detector has been successfully used in an experiment to measure the masses of the N approximate to Z approximate to 33 nuclides near the proton drip-line Of particular interest is the mass of As-65 A maximum detection efficiency of 70% and a time resolution of 118 +/- 8 Ps (FWHM) have been achieved in the experiment The dependence of detection efficiency and signal average pulse height (APH) on atomic number Z has been studied The potential of APH for Z identification has been discussed (C) 2010 Elsevier B V All rights reserved

143Pm高自旋态和重丰中子新核素的合成及衰变性质研究

本论文从内容上可以分为两大部分：第一部分：对近球形核~(143)Pm高自旋态进行的在束γ研究。这一部分是本文的重点。利用能量为82和90 MeV的~(19)F束流，通过融合蒸发反应~(128)Te (~(19)F,4nγ) ~(143)Pm布局~(143)Pm的高自旋态。利用联合在束装置(JIBGE)的10套带BGO反康的HPGe探测器进行了标准在束γ谱学测量，包括γ射线的激发函数、γ单谱、γ-γ-t符合谱以及DCO测量。在已有工作的基础上，建立了~(143)Pm激发能高达10.5 MeV，自旋约为(61/2)h的高自旋态能级结构。观测到了28条新的跃迁能级和48条新的γ射线。对两个已知的同质异能态寿命进行了提取，并在8 MeV激发能附近进行了高自旋态同质异能态的搜索。以~(142)Nd，~(144)Sm为核实，用零级弱耦合模型对~(143)Pm的晕态能级结构进行了定量的解释。计算表明，直到激发能Ex = 6.77 MeV，自旋宇称J~π = (37/2~+)的晕态能级都可以用弱耦合模型进行很好的解释。但是，对于更高激发能的能级，组态情况要复杂的多，有出现N = 82中子闭壳打破的可能。同时，利用大基壳模型OXBASH程序对其能级结构进行了计算和讨论，其结果支持弱耦合模型的假设。第二部分：利用中能重离子的多核子转移反应，(~(186)W-2p + 2n)，(~(238)U-2p + 2n)对丰中子核~(186)Hf和~(238)Th进行了合成和鉴别。测量它们的半衰期分别为(2.6 ± 1.2) min和 (9.4 ± 2.0) min，与用质子一中子准粒子随机相近似方法的预言值是相符的。同时，对β延发裂变先驱核~(230)Ac进行了实验研究。观测到了它的两个裂变事件，得到~(230)Acβ延发裂变几率为(1.19 ± 0.85) * 10~(-8)。从而使~(230)Ac成为世界上第一种被确认了的基态β延发裂变先驱核。