Source Apportionment of Speciated Mercury in Chinese Rice Grain Using a High-Resolution Model

[Image: see text] Rice grain consumption is a primary pathway of human mercury exposure. To trace the source of rice grain mercury in China, we developed a rice paddy mercury transport and transformation model with a grid resolution of 1 km × 1 km by using the unit cell mass conservation method. The simulated total mercury (THg) and methylmercury (MeHg) concentrations in Chinese rice grain ranged from 0.08 to 243.6 and 0.03 to 238.6 μg/kg, respectively, in 2017. Approximately, 81.3% of the national average rice grain THg concentration was due to atmospheric mercury deposition. However, soil heterogeneity, especially the variation in soil mercury, led to the wide rice grain THg distribution across grids. Approximately, 64.8% of the national average rice grain MeHg concentration was due to soil mercury. In situ methylation was the main pathway via which the rice grain MeHg concentration was increased. The coupled impact of high mercury input and methylation potential led to extremely high rice grain MeHg in partial grids among Guizhou province and junctions with surrounding provinces. The spatial variation in soil organic matter significantly impacted the methylation potential among grids, especially in Northeast China. Based on the high-resolution rice grain THg concentration, we identified 0.72% of grids as heavily polluted THg grids (rice grain THg > 20 μg/kg). These grids mainly corresponded to areas in which the human activities of nonferrous metal smelting, cement clinker production, and mercury and other metal mining were conducted. Thus, we recommended measures that are targeted at the control of heavy pollution of rice grain by THg according to the pollution sources. In addition, we observed a wide spatial variation range of MeHg to THg ratios not only in China but also in other regions of the world, which highlights the potential risk of rice intake.