Uncovering geochemical fractionation of the newly deposited Hg in paddy soil using a stable isotope tracer.

The newly deposited mercury (Hg) is more readily methylated to methylmercury (MeHg) than native Hg in paddy soil. However, the biogeochemical processes of the newly deposited Hg in soil are still unknown. Here, a field experimental plot together with a stable Hg isotope tracing technique was used to demonstrate the geochemical fractionation (partitioning and redistribution) of the newly deposited Hg in paddy soils during the rice-growing period. We showed that the majority of Hg tracer (200Hg, 115.09 ± 0.36 μg kg-1) was partitioned as organic matter bound 200Hg (84.6-89.4%), followed by residual 200Hg (7.6-8.1%), Fe/Mn oxides bound 200Hg (2.8-7.2%), soluble and exchangeable 200Hg (0.05-0.2%), and carbonates bound 200Hg (0.04-0.07%) in paddy soils. Correlation analysis and partial least squares path modeling revealed that the coupling of autochthonous dissolved organic matter and poorly crystalline Fe (oxyhydr)oxides played a predominant role in controlling the redistribution of the newly deposited Hg among geochemical fractions (i.e., fraction changes). The expected aging processes of the newly deposited Hg were absent, potentially explaining the high bioavailability of these Hg in paddy soil. This study implies that other Hg pools (e.g., organic matter bound Hg) should be considered instead of merely soluble Hg pools when evaluating the environmental risks of Hg from atmospheric depositions.