Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.

As a globally transported pollutant, mercury (Hg) released from human activity and methylmercury (MeHg) in the food web are global concerns due to their increasing presence in the environment. In this study, we found that Hg released from municipal sewage into the environment in China is a substantial anthropogenic source based on mass sampling throughout China. In total, 160 Mg (140-190 Mg, from the 20th percentile to the 80th percentile) of Hg (THg) and 280 kg (240-330 kg) of MeHg were released from municipal sewage in China in 2015. The quantities of released THg and MeHg were the most concentrated in the coastal regions, especially in the East, North and South China regions. However, the per capita release of THg and MeHg was the highest in the Tibetan region, which is recognized as the cleanest region in China. THg released into aquatic environments was mitigated from 2001 to 2015 in China, but the amounts released into other sinks increased. This study provides the first picture of the release of Hg from municipal sewage into various sinks in China, and policy makers should pay more attention to the diversity and complexity of the sources and transport of Hg, which can lead to Hg accumulation in the food web and can threaten human health.

The global pollutant mercury (Hg), especially as methylmercury (MeHg), threatens human and ecosystem health. But major contributors of MeHg exposure to people in China remain highly debated. We developed the China Mercury Exposure Assessment (CMEA) model, which incorporates human exposure pathways for MeHg and total Hg (THg), the interregional, including international and interprovincial, food trading as well as human physiology to provide a comprehensive system that can evaluate the pathway of Hg forms to human consumers in China. Based on the CMEA model that employed the most comprehensive and recent data, we have found that the probable daily intake (PDI) of MeHg for the Chinese population was 0.057 (range: 0.036 – 0.091 as 60% confidence interval) μg·kg−1·day−1, while that of THg was 0.35 (range: 0.22 – 0.55) μg·kg−1·day−1. MeHg exposure was dominated by fish intake, especially by farm-raised freshwater fish due to higher consumption of these fish. In 2011, fish intake contributed to 56% to the total MeHg exposure, followed by rice (26%). Consumption of farm-raised fish reduced human exposure to MeHg by 33%. On the other hand, interregional food trading increased MeHg exposure of the Chinese population, as a whole, by 7.6%. The international and interprovincial food trades contributed to 5.1% and 22% of MeHg intake, respectively. For the whole China, fish intake related exposure to MeHg was highest for the Eastern and Northeastern populations, while Tibetans were chronically exposed to the highest MeHg from other sources. Our findings highlight the importance of farmed fish and food trade for MeHg exposure.