Fate and Transport of Mercury through Waterflows in a Tropical Rainforest.

Knowledge gaps of mercury (Hg) biogeochemical processes in the tropical rainforest limit our understanding of the global Hg mass budget. In this study, we applied Hg stable isotope tracing techniques to quantitatively understand the Hg fate and transport during the waterflows in a tropical rainforest including open-field precipitation, throughfall, and runoff. Hg concentrations in throughfall are 1.5-2 times of the levels in open-field rainfall. However, Hg deposition contributed by throughfall and open-field rainfall is comparable due to the water interception by vegetative biomasses. Runoff from the forest shows nearly one order of magnitude lower Hg concentration than those in throughfall. In contrast to the positive Δ199Hg and Δ200Hg signatures in open-field rainfall, throughfall water exhibits nearly zero signals of Δ199Hg and Δ200Hg, while runoff shows negative Δ199Hg and Δ200Hg signals. Using a binary mixing model, Hg in throughfall and runoff is primarily derived from atmospheric Hg0 inputs, with average contributions of 65 ± 18 and 91 ± 6%, respectively. The combination of flux and isotopic modeling suggests that two-thirds of atmospheric Hg2+ input is intercepted by vegetative biomass, with the remaining atmospheric Hg2+ input captured by the forest floor. Overall, these findings shed light on simulation of Hg cycle in tropical forests.

Elevated Mercury Deposition, Accumulation, and Migration in a Karst Forest.

The karst forest is one of the extremely sensitive and fragile ecosystems in southwest China, where the biogeochemical cycling of mercury (Hg) is largely unknown. In this study, we investigated the litterfall deposition, accumulation, and soil migration of Hg in an evergreen-deciduous broadleaf karst forest using high-resolution sampling and stable isotope techniques. Results show that elevated litterfall Hg concentrations and fluxes in spring are due to the longer lifespan of evergreen tree foliage exposed to atmospheric Hg0. The hillslope has 1-2 times higher litterfall Hg concentration compared to the low-lying land due to the elevated atmospheric Hg levels induced by topographical and physiological factors. The Hg isotopic model suggests that litterfall Hg depositions account for ∼80% of the Hg source contribution in surface soil. The spatial trend of litterfall Hg deposition cannot solely explain the trend of Hg accumulation in the surface soil. Indeed, soil erosion enhances Hg accumulation in soil of low-lying land, with soil Hg concentration up to 5-times greater than the concentration on the hillslope. The high level of soil Hg migration in the karst forest poses significant ecological risks to groundwater and downstream aquatic ecosystems.

Deposition and Re-Emission of Atmospheric Elemental Mercury over the Tropical Forest Floor.

Significant knowledge gaps exist regarding the emission of elemental mercury (Hg0) from the tropical forest floor, which limit our understanding of the Hg mass budget in forest ecosystems. In this study, biogeochemical processes of Hg0 deposition to and evasion from soil in a Chinese tropical rainforest were investigated using Hg stable isotopic techniques. Our results showed a mean air-soil flux as deposition of -4.5 ± 2.1 ng m-2 h-1 in the dry season and as emission of +7.4 ± 1.2 ng m-2 h-1 in the rainy season. Hg re-emission, i.e., soil legacy Hg evasion, induces negative transitions of Δ199Hg and δ202Hg in the evaded Hg0 vapor, while direct atmospheric Hg0 deposition does not exhibit isotopic fractionation. Using an isotopic mass balance model, direct atmospheric Hg0 deposition to soil was estimated to be 48.6 ± 13.0 µg m-2 year-1. Soil Hg0 re-emission was estimated to be 69.5 ± 10.6 µg m-2 year-1, of which 63.0 ± 9.3 µg m-2 year-1 is from surface soil evasion and 6.5 ± 5.0 µg m-2 year-1 from soil pore gas diffusion. Combined with litterfall Hg deposition (∼34 µg m-2 year-1), we estimated a ∼12.6 µg m-2 year-1 net Hg0 sink in the tropical forest. The fast nutrient cycles in the tropical rainforests lead to a strong Hg0 re-emission and therefore a relatively weaker atmospheric Hg0 sink.

Quantifying Mercury Distribution and Source Contribution in Surface Soil of Qinghai-Tibetan Plateau Using Mercury Isotopes.

Long-range transport and atmospheric deposition of gaseous mercury (Hg0) result in significant accumulation of Hg in the Qinghai-Tibetan Plateau (QTP). However, there are significant knowledge gaps in understanding the spatial distribution and source contribution of Hg in the surface soil of the QTP and factors influencing Hg accumulation. In this study, we comprehensively investigated Hg concentrations and isotopic signatures in the QTP to address these knowledge gaps. Results show that the average Hg concentration in the surface soil ranks as follows: forest (53.9 ± 36.9 ng g-1) > meadow (30.7 ± 14.3 ng g-1) > steppe (24.5 ± 16.1 ng g-1) > shrub (21.0 ± 11.6 ng g-1). Hg isotopic mass mixing and structural equation models demonstrate that vegetation-mediated atmospheric Hg0 deposition dominates the Hg source in the surface soil, with an average contribution of 62 ± 12% in forests, followed by 51 ± 10% in shrub, 50 ± 13% in steppe, and 45 ± 11% in meadow. Additionally, geogenic sources contribute 28-37% of surface soil Hg accumulation, and atmospheric Hg2+ inputs contribute 10-18% among the four types of biomes. The Hg pool in 0-10 cm surface soil over the QTP is estimated as 8200 ± 3292 Mg. Global warming, permafrost degradation, and anthropogenic influences have likely perturbed Hg accumulation in the soil of QTP.

[Mercury Speciation, Distribution, and Potential Sources in Surface Waters of the Yangtze and Yellow River Source Basins of Tibetan Plateau During Wet Season].

To understand the mercury (Hg) biogeochemical cycle in alpine regions under global warming, it is critical to identify the distribution and sources of Hg in aquatic ecosystems of the Tibet Plateau. The spatial distribution pattern and potential sources of Hg species including total mercury (THg), particulate mercury (PHg), and dissolved mercury (DHg) were investigated in surface waters of the Yangtze and Yellow River source basins during the wet season. The results showed that average ρ(DHg) in surface water of the Yangtze and Yellow River source basins were comparable[(2.96±1.26) ng·L-1 and (2.47±0.83) ng·L-1, respectively], whereas the average ρ(THg)[(10.69±11.14) ng·L-1] and ρ(PHg)[(8.46±11.41) ng·L-1] in the source basin of the Yangtze River were significantly higher than that in surface water of the Yellow River source basin[(3.37±2.03) ng·L-1 and (1.13±1.02) ng·L-1, respectively]. It is worth noting that the ecological risk of Hg in the study area was limited because of low Hg concentration and methylation level. In addition, the correlation analysis illustrated that the THg was mainly concentrated by PHg in the source basin of the Yangtze River. Specifically, the concentration variations in Hg were mainly affected by the input of glacier meltwater, soil erosion, and precipitation. By contrast, the main species of Hg in the source basin of the Yellow River was DHg, the distribution pattern of which was mainly controlled by DOC. Spatially, a significant negative correlation was found between ρ(PHg) and longitude in the source basin of the Yangtze River (R2=0.46, P<0.01). The spatial distribution differences of river slope and soil erosion intensity were identified as the key factors leading to the decreasing trend of ρ(PHg) and ρ(THg) along the river flow in the source basin of the Yangtze River. The results of the PMF model further demonstrated that in the surface waters of the source regions of the Yangtze and Yellow Rivers, 51.4% of Hg derived from long-distance atmospheric deposition, 38.8% from erosion of soil rock or sediment via stream flow, and 9.7% from soil runoff or seepage input.

Understanding heavy metal accumulation in roadside soils along major roads in the Tibet Plateau.

The heavy metal accumulation in the Tibet Plateau (TP) poses a serious ecologic risk to the health of human and the other biota. Given the TP far away from the large anthropogenic emission sources, the rapid development of traffic activities during last several decades possibly leads to the elevated heavy metal concentration in the roadside soils. Therefore, we comprehensively assessed the heavy metal distribution in the 0-5 cm and 15-20 cm depth soils located at 5 m, 50 m, and 100 m distance to the edge of two major roads among the different vegetation covers and climatic conditions in the TP to verify this hypothesis. Results show that most of heavy metal concentrations in soils of different distance to the major road display an insignificant difference. The Nemero Synthesis indexes which represent the risk of pollution for these regions almost range 1 to 2 (low pollution risk), except 12.7 (extreme pollution risk) at one site. These indicate the limited impacts from the traffic activities for the whole region, but at some specific sites with the elevated traffic pollution. The forest cover at the altitude of 3700-4100 m has the highest mercury accumulation due to the vegetation and climatic factors induced the higher atmospheric depositions and stronger complexation with the organic matters. The statistical analysis finally suggests the geogenic weathering processes, climate, terrain and vegetation play an important role in shaping heavy metal distribution along the roadside of the TP.