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.

Protecting the environment and enhancing food security are among the world’s greatest challenges. Fish consumption is widely considered to be the single significant dietary source of methylmercury. Nevertheless, by synthesizing data from the past six decades and using a variety of models, we find that rice could be a significant global dietary source of human methylmercury exposure, especially in South and Southeast Asia. In 2013, globalization caused 9.9% of human methylmercury exposure via the international rice trade and significantly aggravated rice-derived exposure in Africa (62%), Central Asia (98%) and Europe (42%). In 2016, 180 metric tons of mercury were generated in rice plants, 14-fold greater than that exported from oceans via global fisheries. We suggest that future research should consider both the joint ingestion of rice with fish and the food trade in methylmercury exposure assessments, and anthropogenic biovectors such as crops should be considered in the global mercury cycle.

Terrestrial mercury (Hg) transport, induced by water erosion and exacerbated by human activities, constitutes a major disturbance of the natural Hg cycle, but the processes are still not well understood. In this study, we modeled these processes using detailed information on erosion and Hg in soils and found that vast quantities of total Hg (THg) are being removed from land surfaces in China as a result of water erosion, which were estimated at 420 Mg/yr around 2010. This was significantly higher than the 240 Mg/yr mobilized around 1990. The erosion mechanism excavated substantial soil THg, which contributed to enhanced Hg(0) emissions to the atmosphere (4.9 Mg/yr around 2010) and its transport horizontally into streams (310 Mg/yr). Erosion-induced THg transport was driven by the extent of precipitation but was further enhanced or reduced by vegetation cover and land use changes in some regions. Surface air temperature may exacerbate the horizontal THg release into water. Our analyses quantified the processes of erosion-induced THg transport in terrestrial ecosystems, demonstrated its importance, and discussed how this transport is impacted by anthropogenic inputs and legacy THg in soils. We suggest that policy makers should pay more attention to legacy anthropogenic THg sources buried in soil.

Highly elevated concentrations of total mercury (THg) and methylmercury (MeHg) were found in the municipal sewage in Tibet. Material flow analysis supports the hypothesis that these elevated concentrations are related to regular ingestion of Hg-containing Traditional Tibetan Medicine (TTM). In Tibet in 2015, a total of 3,600 kg of THg was released from human body into the terrestrial environment as a result of TTM ingestion, amounting to 45% of the total THg release into the terrestrial environment in Tibet, hence substantially enhancing the environmental Hg burden. Regular ingestion of TTM leads to chronic exposure of Tibetans to inorganic Hg (IHg) and MeHg, which is 34 to 3,000-fold and 0 to 12-fold higher than from any other known dietary sources, respectively. Application of a human physiology model demonstrated that ingestion of TTM can induce high blood IHg and MeHg levels in the human body. Moreover, 180 days would be required for the MeHg to be cleared out of the human body and return to the initial concentration i.e. prior to the ingestion of 1 TTM pill. Our analysis suggests that high Hg level contained in TTM could be harmful to human health and elevate the environmental Hg burden in Tibet.

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