Methylmercury (MeHg)
contamination in rice via paddy soils is an
emerging global environmental issue. An understanding of mercury (Hg)
transformation processes in paddy soils is urgently needed in order
to control Hg contamination of human food and related health impacts.
Sulfur (S)-regulated Hg transformation is one important process that
controls Hg cycling in agricultural fields. In this study, Hg transformation
processes, such as methylation, demethylation, oxidation, and reduction,
and their responses to S input (sulfate and thiosulfate) in paddy
soils with a Hg contamination gradient were elucidated simultaneously
using a multi-compound-specific isotope labeling technique (200HgII, Me198Hg, and 202Hg0). In addition to HgII methylation and MeHg demethylation,
this study revealed that microbially mediated reduction of HgII, methylation of Hg0, and oxidative demethylation–reduction
of MeHg occurred under dark conditions; these processes served to
transform Hg between different species (Hg0, HgII, and MeHg) in flooded paddy soils. Rapid redox recycling of Hg species
contributed to Hg speciation resetting, which promoted the transformation
between Hg0 and MeHg by generating bioavailable HgII for fuel methylation. Sulfur input also likely affected
the microbial community structure and functional profile of HgII methylators and, therefore, influenced HgII methylation.
The findings of this study contribute to our understanding of Hg transformation
processes in paddy soils and provide much-needed knowledge for assessing
Hg risks in hydrological fluctuation-regulated ecosystems.