RESUMEN
The discovery of the existence of chain reactions at the Oklo natural reactors in Gabon, Central Africa in 1972 was a triumph for the accuracy of mass spectrometric measurements, in that a 0.5% anomaly in the (235)U/(238)U ratio of certain U ore samples indicated a depletion in (235)U. Mass spectrometric techniques thereafter played a dominant role in determining the nuclear parameters of the reactor zones themselves, and in deciphering the geochemical characteristics of various elements in the U-rich ore and in the surrounding rock strata. The variations in the isotopic composition of a large number of elements, caused by a combination of nuclear fission, neutron capture and radioactive decay, provide a powerful tool for investigating this unique geological environment. Mass spectrometry can be used to measure the present-day elemental and isotopic abundances of numerous elements, so as to decipher the past history of the reactors and examine the retentivity/mobility of these elements. Many of the fission products have a radioactive decay history that have been used to date the age and duration of the reactor zones, and to provide insight into their nuclear and geochemical behavior as a function of time. The Oklo fission reactors and their near neighbor at Bangombé, some 30 km to the south-east of Oklo, are unique in that not only did they become critical some 2 x 10(9) years ago, but also the deposits have been preserved over this period of geological time. The long-term geochemical behavior of actinides and fission products have been extensively studied by a variety of mass spectrometric techniques over the past 30 years to provide us with significant information on the mobility/retentivity of this material in a natural geological repository. The Oklo-Bangombé natural reactors are therefore geological analogs that can be evaluated in terms of possible radioactive waste containment sites. As more reactor zones were discovered, it was realized that they could be classified into two groups according to their burial depth in the Oklo mine-site. Reactor Zones 10, 13, and 16 were buried more deeply, and were therefore less weathered than the other zones. The less-weathered zones are of great importance in mobility/retentivity studies and therefore to the question of radioactive waste containment. Isotopic studies of these natural reactors are also of value in physics to examine possible variations in fundamental constants over the past 2 billion years.
RESUMEN
Even before the 20th century, a consistent set of internationally accepted atomic weights was an important objective of the scientific community because of the fundamental importance of these values to science, technology and trade. As the 20th century progressed, physicists, geoscientists, and metrologists collaborated with chemists to revolutionize the science of atomic weights. At the beginning of the century, atomic weights were determined from mass relationships between chemical reactants and products of known stoichiometry. They are now derived from the measured isotopic composition of elements and the atomic masses of the isotopes. Accuracy in measuring atomic weights has improved continually, leading to the revelation of small but significant variations in the isotope abundances of many elements in their normal terrestrial occurrences caused by radioactivity and a variety of physicochemical and biochemical fractionation mechanisms. This atomic-weight variability has now been recognized as providing new scientific insights into and knowledge of the history of materials. Atomic weights, except those of the monoisotopic elements, are thus no longer regarded as "constants of nature". At the beginning of the 20th century, two scales for atomic weights were in common use: that based on the atomic weight of hydrogen being 1 and that based on the atomic weight of oxygen being 16. Atomic weights are now scaled to (12)C, which has the value 12 exactly. Accurate atomic weights of silicon, silver, and argon, have enabled the values of the Avogadro, Faraday and Universal Gas constants, respectively, to be established, with consequent effects on other fundamental constants.
RESUMEN
Isotope dilution mass spectrometry is an ideal analytical technique to measure the elemental abundance of Mo in C1 carbonaceous chondrites and the metallic and troilite phases of iron meteorites. The mean abundance of Mo in two C1 meteorites is 0.909+/-0.040 microg/g which corresponds to a value of 2.55 atoms Mo with respect to Si equal to 10(6) atoms, which is identical to the currently accepted solar system abundance. The partitioning of Mo between the metallic and sulfide phases in the Mundrabilla iron meteorite was found to be 6.0+/-0.2 microg/g and 8.6+/-0.3 microg/g, respectively. A new, precise Mo concentration of 1.54+/-0.04 microg/g for the Geochemical Reference Standard BCR-1 is also reported.
RESUMEN
The role of mass spectrometry in nuclear fission has been invaluable since 1940, when A. O. C. Nier separated microgram quantities of (235) U from (238) U, using a gas source mass spectrometer. This experiment enabled the fissionable nature of (235) U to be established. During the Manhattan Project, the mass spectrometer was used to measure the isotope abundances of uranium after processing in various separation systems, in monitoring the composition of the gaseous products in the Oak Ridge Diffusion Plant, and as a helium leak detector. Following the construction of the first reactor at the University of Chicago, it was necessary to unravel the nuclear systematics of the various fission products produced in the fission process. Off-line mass spectrometry was able to identify stable and long-lived isotopes produced in fission, but more importantly, was used in numerous studies of the distribution of mass of the cumulative fission yields. Improvements in sensitivity enabled off-line mass spectrometric studies to identify fine structure in the mass-yield curve and, hence, demonstrate the importance of shell structure in nuclear fission. Solid-source mass spectrometry was also able to measure the cumulative fission yields in the valley of symmetry in the mass-yield curve, and enabled spontaneous fission yields to be quantified. Apart from the accurate measurement of abundances, the stable isotope mass spectrometric technique has been invaluable in establishing absolute cumulative fission yields for many isotopes making up the mass-yield distribution curve for a variety of fissile nuclides. Extensive mass spectrometric studies of noble gases in primitive meteorites revealed the presence of fission products from the now extinct nuclide (244) Pu, and have eliminated the possibility of fission products from a super-heavy nuclide contributing to isotopic anomalies in meteoritic material. Numerous mass spectrometric studies of the isotopic and elemental abundances of samples from the Oklo Natural Reactor have enabled the nuclear parameters of the various reactor zones to be calculated, and the mobility/retentivity of a number of elements to be established in the reactor zones and the surrounding rocks. These isotopic studies have given valuable information on the geochemical behavior of natural geological repositories for radioactive waste containment. © 1997 John Wiley & Sons, Inc.
RESUMEN
Procedures are described which permit mass spectrometric isotope-dilution analysis to be used to determine Ag, Te and Pd in rock samples at the ng g level. The concentrations (ng g ) of Ag, Te and Pd were found to be 25.7 +/- 0.7, 1.2 +/- 0.6 and 0.08 +/- 0.05 respectively in BCR-1 and 3.5 +/- 0.2, 4.2 +/- 0.7 and 2.9 +/- 1.7 respectively in PCC-1.
RESUMEN
The concentrations of Ag, Cd, Pb, Zn and Pd in sea-water have been determined by thermal-ionization isotope-dilution mass spectrometry. The concentrations found, in ng/kg, were 0.6 +/- 0.4 Ag, 1.9 +/- 0.4 Cd, 18 +/- 8 Pb, 30 +/- 8 Zn and < 4 Pd. These levels are lower than some reported previously. Determination of Pd in sea-water is reported for the first time.