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Mercury is a potent neurotoxin that poses significant health risks to humans, primarily through seafood consumption. Atmospheric deposition is the largest source of oceanic mercury, in either oxidized (Hg ) or elemental (Hg ) form. Understanding the relative contributions of atmospheric Hg and Hg to the ocean is essential for accurately assessing global mercury budgets. Earlier even mercury isotope (Δ Hg) analyses suggested equivalent Hg /Hg contributions but neglected spatial variations in atmospheric Δ Hg signatures. Here, we developed a 3D atmospheric model incorporating mercury chemistry and isotopic fractionation to address this limitation. Our simulations reveal distinct atmospheric Δ Hg patterns and quantify their deposition to the ocean. Constrained by observed Δ Hg data in the ocean, we propose an updated deposition ratio of atmospheric Hg to Hg to the ocean, which may exceed 2:1, higher than the previously reported 1:1. Our findings are crucial for assessing atmospheric mercury dispersal and predicting the recovery of marine ecosystems.

The Carnian Pluvial Episode (CPE; 234–232 million years ago) is an iconic but poorly understood hyperthermal event. Here, we present an integrated high-resolution (~2–10 kyr) multi-proxy record from a Carnian lacustrine succession of the Junggar Basin of northwestern China. We find that the rapid CPE onset (~15.8 kyr) could have been the result of volcanism and subsequent surface carbon-cycle feedbacks. The CPE terrestrial carbon cycling, at a scale of ± 1‰ (δ 13 C org ), displays an in-phase relationship with the 405-kyr-long-eccentricity parameter, paralleling the warmhouse climate–carbon-cycle interactions throughout the Oligo–Miocene. The CPE hydrological cycle was typified by increased aridification in continental interiors and multiple precipitation centres at low-latitude eastern regions of Pangea and at the poles. The carbon and hydrological cycle changes of the CPE include features reminiscent of other warm events, suggesting they may share key characteristics and hold important clues to Earth system functioning. Understanding past warming events is essential to project the consequences of anthropogenic carbon emissions. Here, carbon and hydrological cycle changes of the Carnian Pluvial Episode are revealed, offering insights into Earth System functioning.

Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.

There exists observational evidence that gaseous elemental mercury (GEM) can be readily removed from the atmosphere via chemical oxidation followed by deposition in the polar and sub-polar regions, free troposphere, lower stratosphere, and marine boundary layer under specific environmental conditions. Here we report GEM depletions in a temperate mixed forest at Mt. Changbai, Northeast China. The strong depletions occurred predominantly at night during the leaf-growing season and in the absence of gaseous oxidized mercury (GOM) enrichment (GOM  <  3 pg m−3). Vertical gradients of decreasing GEM concentrations from layers above to under forest canopy suggest in situ loss of GEM to forest canopy at Mt. Changbai. Foliar GEM flux measurements showed that the foliage of two predominant tree species is a net sink of GEM at night, with a mean flux of −1.8 ± 0.3 ng m2 h−1 over Fraxinus mandshurica (deciduous tree species) and −0.1 ± 0.2 ng m2 h−1 over Pinus Koraiensis (evergreen tree species). Daily integrated GEM δ202Hg, Δ199Hg, and Δ200Hg at Mt. Changbai during 8–18 July 2013 ranged from −0.34 to 0.91 ‰, from −0.11 to −0.04 ‰ and from −0.06 to 0.01 ‰, respectively. A large positive shift in GEM δ202Hg occurred during the strong GEM depletion events, whereas Δ199Hg and Δ200Hg remained essentially unchanged. The observational findings and box model results show that uptake of GEM by forest canopy plays a predominant role in the GEM depletion at Mt. Changbai forest. Such depletion events of GEM are likely to be a widespread phenomenon, suggesting that the forest ecosystem represents one of the largest sinks ( ∼ 1930 Mg) of atmospheric Hg on a global scale.

To understand the ambient levels and sources of atmospheric mercury (Hg) in the Tibetan Plateau, a full-year continuous measurement of speciated atmospheric mercury was conducted at the Waliguan (WLG) Baseline Observatory (3816 m a.s.l.) from May 2012 to April 2013. Mean concentrations (± 1 SD) of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) during the whole study period were 1.90±0.80 ng m−3, 12.0±10.6 and 65.4±63.2 pg m−3, respectively. Seasonal variations of GEM were very small, while those of PBM were quite large with mean values being 4 times higher in the cold (102.3±66.7 pg m−3) than warm (22.8±14.6 pg m−3) season. Anthropogenic emissions to the east of the Tibetan Plateau contributed significantly to GEM pollution at WLG, while dust particles originating from desert and Gobi regions in Xinjiang province and the Tibetan Plateau to the west of WLG were responsible for PBM pollution at WLG. This finding is also supported by the significant positive correlation between daily PBM concentration and daily cumulative absorbing aerosol index (AAI) in air masses transported during the preceding 2 d.

Land surface emissions are an important source of atmospheric total gaseous mercury (TGM); however, its role on the variations of TGM isotopic compositions and concentrations has not been properly evaluated. In this study, TGM isotope compositions, a powerful tracer for sources and transformation of Hg, were measured at 10 urban sites and one rural site in China. TGM concentrations were higher in summer than in winter in most cities except in Guiyang and Guangzhou in the low latitudes. The summertime high TGM concentrations coincided with prevailing low TGM δ202Hg and high TGM Δ199Hg signatures. These seasonal patterns were in contrast with those typically observed in rural areas in the Northern Hemisphere, suggesting that atmospheric oxidation chemistry, vegetation activity and residential coal combustion were likely not the dominant mechanisms contributing to the TGM concentration and isotopic composition seasonality in Chinese cities. The amplitudes of seasonal variations in TGM concentrations and Δ199Hg (or TGM δ202Hg) were significantly positively (or negatively) correlated with that of the simulated soil GEM emission flux. These results suggest that the seasonal variations in TGM isotopic compositions and concentrations in the 10 Chinese cities were likely controlled by land surface emissions that were observed or reported with highly negative δ202Hg signatures.

Atmospheric particulate-bound mercury (PBM) plays an important role in the geochemical cycling of mercury (Hg). This study reviewed research progress of the PBM, including the possible emission and deposition pathways, measurement methods and the global distribution. The primary PBM sources are anthropogenic sources, but natural sources could be also a considerable contributor, for instance, chemical transport and dust in the arid and desert area. Different filter methods, such as quartz fibre filters, have been applied to the PBM measurement, and PBM can also be real-time monitored automatically. Generally, the average PBM concentrations were higher in the Northern Hemisphere than in the Southern Hemisphere. However, the PBM level of Antarctica is quite high. PBM concentrations were higher in the urban areas than in the remote areas, and there was a high PBM level in the developing countries. Moreover, high PBM concentrations were observed in the range 20°–60° of northern latitude.

To better understand the influence of monsoonal climate and transport of atmospheric mercury (Hg) in southwestern China, measurements of total gaseous mercury (TGM, defined as the sum of gaseous elemental mercury, GEM, and gaseous oxidized mercury, GOM), particulate bound mercury (PBM) and GOM were carried out at Ailaoshan Station (ALS, 2450 m a.s.l.) in southwestern China from May 2011 to May 2012. The mean concentrations (± SD) for TGM, GOM and PBM were 2.09 ± 0.63, 2.2 ± 2.3 and 31.3 ± 28.4 pg m−3, respectively. TGM showed a monsoonal distribution pattern with relatively higher concentrations (2.22 ± 0.58 ng m−3, p  =  0.021) during the Indian summer monsoon (ISM, from May to September) and the east Asia summer monsoon (EASM, from May to September) periods than that (1.99 ± 0.66 ng m−3) in the non-ISM period. Similarly, GOM and PBM concentrations were higher during the ISM period than during the non-ISM period. This study suggests that the ISM and the EASM have a strong impact on long-range and transboundary transport of Hg between southwestern China and south and southeast Asia. Several high TGM events were accompanied by the occurrence of northern wind during the ISM period, indicating anthropogenic Hg emissions from inland China could rapidly increase TGM levels at ALS due to strengthening of the EASM. Most of the TGM and PBM events occurred at ALS during the non-ISM period. Meanwhile, high CO concentrations were also observed at ALS, indicating that a strong south tributary of westerlies could have transported Hg from south and southeast Asia to southwestern China during the non-ISM period. The biomass burning in southeast Asia and anthropogenic Hg emissions from south Asia are thought to be the source of atmospheric Hg in remote areas of southwestern China during the non-ISM period.

Mercury (Hg) concentrations and deposition fluxes in precipitation and litterfall were measured at multiple sites (six rural sites and an urban site) across a broad geographic area in China. The annual deposition fluxes of Hg in precipitation at rural sites and an urban site were 2.0 to 7.2 and 12.6 ± 6.5 µg m.sup.-2  yr.sup.-1, respectively. Wet deposition fluxes of Hg at rural sites showed a clear regional difference with elevated deposition fluxes in the subtropical zone, followed by the temporal zone and arid/semi-arid zone. Precipitation depth is the primary influencing factor causing the variation of wet deposition. Hg fluxes through litterfall ranged from 22.8 to 62.8 µg m.sup.-2  yr.sup.-1, higher than the wet deposition fluxes by a factor of 3.9 to 8.7 and representing approximately 75 % of the total Hg deposition at the forest sites in China. This suggests that uptake of atmospheric Hg by foliage is the dominant pathway to remove atmospheric Hg in forest ecosystems in China. Wet deposition fluxes of Hg at rural sites of China were generally lower compared to those in North America and Europe, possibly due to a combination of lower precipitation depth, lower GOM concentrations in the troposphere and the generally lower cloud base heights at most sites that wash out a smaller amount of GOM and PBM during precipitation events.