Understanding the effects of sulfur input on mercury methylation in rice paddy soils

Sulfur could be introduced into paddy soils via dry or wet deposition, irrigation, and fertilization, which subsequently impacts the production of methylmercury (MeHg), a bioaccumulative neurotoxicant. However, effects of sulfur input on MeHg production are variable, possibly due to the multiple effects of sulfur on Hg mobility and/or microbial Hg methylators, leading to uncertainties in predicting MeHg risk. To address that, we explored the effects of different types and amounts of sulfur as well as concentrations of ambient sulfate on Hg methylation in paddy soils, and elucidated the mechanisms by quantifying changes in (1) Hg mobility and (2) microbial Hg methylators (e.g., sulfate-reducing bacteria, SRB). Our results indicated that MeHg levels increased by 40-86% and 30-96% in soils under various types (i.e., 200 mg kg^-1 elemental sulfur, ammonium sulfate, sulfur-coated urea and potassium sulfate (K₂SO₄)) and different amounts (i.e., 100, 200 and 400 mg kg^-1 K₂SO₄) of sulfur input. The enhanced MeHg production could be explained by increased Hg mobility but not changes in microbial Hg methylators. Besides, sulfate input increased MeHg levels (89-240%) in soils with low ambient sulfate levels (<100 mg kg^-1) but had no effect on high-sulfate soils (>380 mg kg^-1). These could be explained by the diverse responses of Hg mobility and microbial Hg methylators to sulfate input at different ambient sulfate levels. Our study opens the "black box" of Hg methylation under sulfur input, which would help reduce uncertainties in predicting MeHg risk in soils.