Silicon is the second most abundant element on Earth. It is an important nutrient for phytoplankton and is readily absorbed by terrestrial vegetation; it also assists the removal of carbon dioxide from the atmosphere through the weathering of silicates. But the continental cycle of silicon is not well known, and only a few studies have attempted to use silicon stable isotopes (28Si, 29Si and 30Si) to quantify the continental silicon reservoirs. Dissolved silicon in sea and river waters forms a reservoir of mean isotopic value +1.1 per thousand (refs 7, 10). It is enriched in 30Si with respect to the igneous rocks reservoir, which has a mean isotopic value of -0.3 per thousand (refs 4, 9). This enrichment can only be produced by a major fractionation during weathering, and should result in the formation of a continental 30Si-depleted reservoir. Such a reservoir, however, has not been identified to date. Here we analyse silicon isotopes of in situ quartz from a sandstone series in France, using a new-generation secondary ion mass spectrometry apparatus. We show that quartz that precipitates as siliceous cements forms a strongly 30Si-depleted reservoir with isotopic values down to -5.7 per thousand, a more negative value than any previously published for terrestrial samples. Our findings suggest that quartz re-precipitation plays an important role in the biogeochemical cycle of silicon.
The laser fluorination technique reported here for analyzing the oxygen isotope composition (d 18 O) of fine quartz size fractions 50-20, 20-10, 10-5, 5-2, 2-1 and <1 lm has been validated by comparison with the ion microprobe technique. It yields accurate d 18 O data with an external precision better than 0.15&. This is a significant methodological improvement for isotopic studies dealing with materials such as soil or biogenic oxides and silicates: particles are often too small and recovered in insufficient amount to be easily handled for ion microprobe analysis. Both techniques were used to investigate d 18 O composition of a Cretaceous quartzite and silcrete sequence from the South-East of France. Quartzite cements average 31.04 ± 1.93&. They formed from Mid-Cretaceous seawater. Higher in the series, silcretes cements average 26.66 ± 1.36&. They formed from Upper-or post-Upper-Cretaceous soil water and groundwater. Oxygen isotope data show that the silicification steps from one mineralogical phase to another and from one layer to another (including from an upper pedogenic silcrete to a lower groundwater silcrete) occurred in a closed or weakly evaporating hydrological system.
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