Stable (Cu, Mg) and radiogenic (Sr, Nd) isotope fractionation in colloidsof boreal organic-rich watersстатья
Статья опубликована в высокорейтинговом журнале
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Дата последнего поиска статьи во внешних источниках: 19 июля 2013 г.
Аннотация:Stable (Cu and Mg) and radiogenic (Sr and Nd) isotopic compositions in filtrates and ultrafiltrates of various size
fractions have been measured in waters of subarctic watersheds (NWRussia) and in temperate rivers and lakes
of the south boreal zone. A large volume of samples were filtered in the field using cascade filtration and ultrafiltration
employing progressively decreasing pore sizes (100, 20, 10, 5, 0.8, 0.4, 0.22, and 0.1 μm; 100, 10 and
1 kDa) followed by element isotopic analysis using thermal ionization mass spectrometers and a Neptune
multicollector ICP-MS. In the boreal watershed underlain by Archean and Proterozoic rocks, the 87Sr/86Sr ratio
decreased in the 1–100 kDa ultrafiltrates and dialysates by 0.0001–0.0004 units compared to the 0.45 μm filtrates.
Despite the dominance of colloids in the Nd speciation in surface waters, the isotopic value of Nd in the
filtrates and ultrafiltrates remained constant within the uncertainty of the measurements. We hypothesize the
absence of an atmospheric input of silicate dust for Nd but the presence of marine aerosols for Sr. It follows
that the Sr in the investigated surface waters has a short residence time compared to the time required for
achieving isotopic equilibrium between the colloidal (1 kDa–0.22 μm) and truly dissolved (b1 kDa) pools. For
Nd, the residence time is long enough to achieve this equilibrium. The stable isotope composition of Cu in the
streams remained constant within ±0.1‰ during filtration through 100 μm to 1 kDa membranes, despite the
fact that 40–60% of Cu was colloidal. This result suggests that the homogeneity of the Cu isotopic composition
within the colloidal and truly dissolved pools is likely associated with the similarity of the structure and stability
of Cu(II) complexes with fulvic acids of different molecular weights. The stable isotope composition of dissolved
Mg in soil solution and bog surface water demonstrates similar,within the analytical uncertainty, isotopic signatures
between truly dissolved and colloidal fractions.
Despite the dramatically different structures of the metal–dissolved organic matter (DOM) complexes for
Cu2+ and Mg2+, the results of the present work reveal a high homogeneity of stable isotope compositions
between colloidal (1 kDa–0.22 μm) and ultrafiltered (b1 kDa) fractions, which is presumably due to the
high rate of isotopic exchange between the colloidal and ionic forms of the metals. Variation of radiogenic
isotopic composition of Sr among ultrafiltered, colloidal and particulate fractions suggests that there is a contribution
of atmospheric input to the chemical composition of surface waters and provides certain constraints
on the isotopic composition of Sr carried by small organic-rich boreal rivers to the Arctic Ocean.