Uranium series disequilibrium in a young surficial uranium deposit, northeastern Washington, U.S.A.

Abstract

A recently discovered ore-grade accumulation of U in organic-rich sediments of late Quaternary age provides an opportunity for studying the early association of U, U-daughters, and organic matter in a natural setting. The U occurs in valley-fill sediments of peat, peaty clay, silt, and sand along the north fork of Flodelle Creek, Stevens County, Washington. Radiometric techniques (delayed neutron, high-resolution gamma-ray spectrometry, thin-source alpha spectrometry) were employed to determine the abundance and distribution of U-series nuclides, the extent of secular equilibrium within the U decay series, and the apparent U-series ages of U incorporation. Sixteen lithologically distinct intervals were sampled from a 292 cm core. Uranium contents range from 140 to 2790 ppm and are positively correlated with organic contents. Measured alpha activity ratios of 234U/ 238U (1.31–1.38) are very similar to those reported in coexisting waters, suggesting a rather constant isotopic composition of introduced U. Much lower Th contents of <10–40 ppm are controlled by the type and abundance of silicate detritus. The youth of the host sediments (<15 000 a) and the paucity of associated radioactivity suggested large excesses of U relative to radioactive daughters and such excesses were observed, particularly in the shallowest intervals. Apparent ages of U emplacement determined by the (alpha) activity ratio of 230Th daughter to 234U parent show a general increase with depth and fair agreement with estimated depositional ages. This observation suggests dominantly syndepositional or early post depositional emplacement of U followed by decay-generated buildup of 230Th daughter with time. However, interval by interval comparisons of the relative abundances of other daughters, particularly 226Ra and 210Pb, indicate variability caused by processes other than closed-system growth and decay, probably because chemically diverse daughters that are decay-generated in situ have differing mobilities and because upwelling ground water continuously adds more U and minor amounts of daughters. If 230Th is considered the least susceptible to these modifications, the data suggest some addition of 234U in the deepest intervals and some loss of 226Ra and/or gain of 222Rn throughout the studied core.