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The contemporary mercury (Hg) cycle in the world's oceans has been greatly affected by human activities. However, we are still lacking reliable, long-term, and continuous records of Hg in seawater. Here, we report for the first time on using annually banded Porites coral skeletons from the northern South China Sea (SCS) as an archive for recording changes of seawater dissolved Hg spanning the past two centuries. We developed a combustion-trapping method to preconcentrate ultratrace Hg concentrations from coral aragonitic skeletons for highly accurate total Hg measurements. Results show that Hg in the coral skeletons ranges from 0.3 to 5.1 pmol/g and is discriminated against Ca during coral skeletal calcification. Preindustrial (1798-1832) Hg levels in coral skeletons were found to be approximately 0.5 pmol/g. The highest Hg concentrations (3-5 pmol/g) were observed during the WWII period (1933-1942). Other distinct Hg maxima (-3 pmol/g) are observed for the periods 1833-1847, 1858-1862, 1918-1927, 1978-1982, and 1988-1992, with the first four coinciding with contemporary Chinese wars. Our study suggests that the production and use of ammunitions in those wars likely account for the primary Hg emission sources in the northern SCS before 1950, and coral is potentially a robust indicator of historical, regional Hg contamination events. [ABSTRACT FROM AUTHOR]

Gaseous elemental mercury (GEM) is the dominant form of mercury in the atmosphere. Its conversion into oxidized gaseous and particulate forms is thought to drive atmospheric mercury wet deposition to terrestrial and aquatic ecosystems, where it can be subsequently transformed into toxic methylmercury. The contribution of mercury dry deposition is however largely unconstrained. Here we examine mercury mass balance and mercury stable isotope composition in a peat bog ecosystem. We find that isotope signatures of living sphagnum moss (Δ(199)Hg = -0.11 ± 0.09‰, Δ(200)Hg = 0.03 ± 0.02‰, 1σ) and recently accumulated peat (Δ(199)Hg = -0.22 ± 0.06‰, Δ(200)Hg = 0.00 ± 0.04‰, 1σ) are characteristic of GEM (Δ(199)Hg = -0.17 ± 0.07‰, Δ(200)Hg = -0.05 ± 0.02‰, 1σ), and differs from wet deposition (Δ(199)Hg = 0.73 ± 0.15‰, Δ(200)Hg = 0.21 ± 0.04‰, 1σ). Sphagnum covered during three years by transparent and opaque surfaces, which eliminate wet deposition, continue to accumulate Hg. Sphagnum Hg isotope signatures indicate accumulation to take place by GEM dry deposition, and indicate little photochemical re-emission. We estimate that atmospheric mercury deposition to the peat bog surface is dominated by GEM dry deposition (79%) rather than wet deposition (21%). Consequently, peat deposits are potential records of past atmospheric GEM concentrations and isotopic composition.

Mercury (Hg) emissions from coal combustion contribute approximately half of anthropogenic Hg emissions to the atmosphere. With the implementation of the first legally binding UNEP treaty aimed at reducing anthropogenic Hg emissions, the identification and traceability of Hg emissions from different countries/regions are critically important. Here, we present a comprehensive world coal Hg stable isotope database including 108 new coal samples from major coal-producing deposits in South Africa, China, Europe, India, Indonesia, Mongolia, former USSR, and the U.S. A 4.7‰ range in δ(202)Hg (-3.9 to 0.8‰) and a 1‰ range in Δ(199)Hg (-0.6 to 0.4‰) are observed. Fourteen (p < 0.05) to 17 (p < 0.1) of the 28 pairwise comparisons between eight global regions are statistically distinguishable on the basis of δ(202)Hg, Δ(199)Hg or both, highlighting the potential application of Hg isotope signatures to coal Hg emissions tracing. A revised coal combustion Hg isotope fractionation model is presented, and suggests that gaseous elemental coal Hg emissions are enriched in the heavier Hg isotopes relative to oxidized forms of emitted Hg. The model explains to first order the published δ(202)Hg observations on near-field Hg deposition from a power plant and global scale atmospheric gaseous Hg. Yet, model uncertainties appear too large at present to permit straightforward Hg isotope source identification of atmospheric forms of Hg. Finally, global historical (1850-2008) coal Hg isotope emission curves were modeled and indicate modern-day mean δ(202)Hg and Δ(199)Hg values for bulk coal emissions of -1.2 ± 0.5‰ (1SD) and 0.05 ± 0.06‰ (1SD).