Variations and controls of iron oxides and isotope compositions during paddy soil evolution over a millennial time scale

摘要

AbstractA paddy soil chronosequence consisting of five profiles derived from calcareous marine sediments with cultivation history from 0 to 1000years was studied to understand the underlying mechanisms and processes controlling the millennial scale Fe evolution. We evaluated the chronosequencial changes in depth distribution of Fe oxide contents and Fe isotopic compositions. Results showed that paddy soil evolution under the influence of periodic flooding and groundwater fluctuation resulted with time in variations of soil moisture regime and redox condition that control Fe mobilization, translocation and redistribution, leading to enhanced profile differentiation of Fe oxides and measurable Fe isotope fractionation. Total Fe and oxide bound Fe as well as their differentiation between surface and subsurface horizons increased as paddy soils age, leading to the formation of diagnostic horizons and features characterizing Fe distribution and redistribution. Selective extractions showed that the weakly-bound, oxide-bound and silicate bound Fe corresponded to 1–16%, 8–46%, and 52–91% of the total Fe, respectively, and these proportions varied with both time and depth due to the redox-related Fe transformation and translocation. δ56Fe values in the studied paddy soil chronosequence ranged from ?0.01‰ to 0.18‰ and exhibited a strong negative correlation with the logarithm of total Fe concentrations, suggesting mass-dependent Fe isotope fractionation occurred as a result of the preferential removal of lighter Fe isotopes during long-term paddy soil evolution under the predominant reducing conditions. However, the Fe isotopic ratio of a specific paddy