Overview
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- Table 1. Hg Isotope Enrichment Factors of Odd-MIF and Even-MIF in Physical and Chemical Processes Contained in the
- and Sun et al.43 cEnrichment factors for atmospheric HgII photoreduction process are assumed from Song et al.,25 which is the mean enrichment
- measurement37,38 has reported E199Hg of about 3.5‰ between snow and air during the Arctic AMDE. We speculate that 60% of deposited
- tion of stable Hg isotopes for marine source attribution. Flux down = K w × CHg a/H (2)
- studies.18,35,36,38,52−56,59−80 (b-c) Comparison of observed and modeled mean Δ199Hg and Δ200Hg signatures for atmospheric Hg0, HgII(g),
- are listed in Table 1, adapted from Song et al.25 Specifically,
- emissions are summarized in Table S1. The model is initialized
- residual Hg II (p) and depletion in the reduced Hg 0 . inherent uncertainties (Table 1), which may influence the
- mechanisms remain incompletely understood. In our recent simulated values. As shown in Table S2, doubling the
- reproduces observed global Δ200Hg values across different variability ranges from 0.02‰ to 0.05‰ for Hg0 deposition,
- atmospheric Hg species (Table 1). In this study, seasonal approximately 0.1‰ to 0.2‰ for HgII dry deposition, and
- et al.25,44 (Table S1), with natural emissions derived from field Δ199Hg variability of approximately 0.1‰ to 0.2‰ for dry
- in Table S1, the Δ199Hg and Δ200Hg of Hg0 emissions has model aligns with most available observations, the limited
- anthropogenic emission sources, are synthesized to validate 1c). The model results show −0.07 ± 0.01‰ (n = 52) for Hg0,
- our model results (Figure 1a). The model successfully 0.16 ± 0.01‰ (n = 2) for HgII(g), 0.07 ± 0.05‰ (n = 4) for
- atmosphere. As shown in Figure 1b, the modeled annual (n = 4) for HgII(p) in remote mountain sites, and 0.15 ±
- mean Δ199Hg values for Hg0 (−0.20 ± 0.02‰, n = 53), 0.03‰ (n = 14) for HgII(pre), which are in close agreement
- HgII(g) (0.33 ± 0.12‰, n = 2), HgII(p) in near-shore and with observed values of −0.06 ± 0.03‰ (n = 52) (R2 = 0.18,
- MBL environment (0.26 ± 0.06‰, n = 5), HgII(p) in remote RMSE = 0.02), 0.17 ± 0.02‰ (n = 2), 0.08 ± 0.05‰ (n = 4)
- mountain sites (0.46 ± 0.33‰, n = 4), and HgII(pre) (0.39 ± (R2 = 0.82, RMSE = 0.02), 0.10 ± 0.03‰ (n = 4), and 0.16 ±
- 0.14‰, n = 15) are comparable to the observed values of 0.03‰ (n = 14) (R2 = 0.50, RMSE = 0.03), respectively. This
- −0.19 ± 0.06‰ (n = 53) (R2 = 0.15, RMSE = 0.05), 0.40 ± reflects the feasibility of even-MIF modeling in this study.
- 0.05‰ (n = 2), 0.25 ± 0.32‰ (n = 5), 0.43 ± 0.14‰ (n = 4), We further validated the model results in the MBL by using
- and 0.33 ± 0.28‰ (n = 15), respectively. This indicates that available marine and coastal atmospheric Hg isotope data.
- feasibility. Similarly, the modeled annual mean Δ200Hg values compositions of Hg0 from island52−54 and MBL sites,55 the
- mean of Δ199HgII(p) signatures. (b) The background color represents modeled annual mean of Δ200HgII(p) signatures. (c)−(f) Comparison of
- 0.07‰, n = 4) and Δ200Hg (−0.06 ± 0.01‰, n = 4) favorably with the measurements of 0.35 ± 0.16‰ and 0.18 ±
- signatures, yielding modeled values of −0.18 ± 0.03‰ (n = 4) 0.04‰, respectively. In addition, the simulated isotope
- and − 0.06 ± 0.01‰ (n = 4), respectively. The model also signatures are consistent with vessel-based observations in
- mean simulation results. Specifically, the observed and S5). This pattern indicates that chemical fractionation
- 0.02 ± 0.27‰ (n = 109), respectively, while the Δ200Hg values while the isotopic composition of Hg0 remains stable due to its
- are 0.11 ± 0.12‰ and 0.09 ± 0.13‰ (n = 109), respectively. dominance in the atmospheric Hg pool (>90%) and the
- Figure 4. Association between monthly mean values of important factors and MIF signals of atmospheric Hg over: (a) Indian ocean, (b) North
- ments. The model also reveals pronounced seasonal trends and (Figure S7); annual zonal mean (Figure S8); annual
- variations among different atmospheric Hg species, under- mean chemistry rates (Figure S9); monthly mean of Br
- oxidized Hg and dry deposition. Such advancements are emission sources (Table S1); min and max monthly
- transformation of atmospheric Hg in marine environments. (Table S2) (PDF)
- indicate a maximum monthly mean difference of 0.30‰ for China; Frontiers Science Center for Critical Earth Material
- implications for the global mercury budget. Atmos. Chem. Phys. 2017, (23) Jiskra, M.; Heimbürger-Boavida, L.-E.; Desgranges, M.-M.;
- (6) UN-Environment, Global Mercury Assessment 2018; UN Environ- J.; Thyssen, M.; Point, D.; Sonke, J. E. Mercury stable isotopes
- (8) Tsui, M.-K.; Blum, J. D.; Kwon, S. Y. Review of stable mercury Isotope Data Constrains Redox Chemistry of Atmospheric Mercury.
- Choi, J. W. Mercury stable isotopes for monitoring the effectiveness of No. 119588.
Methods (brief)
- factor of photoreduction for aqueous Hg collected in Sun et al.39 Even-MIF in the HgII(p) photoreduction process is speculated in Song et al.44
- samples, including gaseous, particulate, and precipitation
- samples, as shown in Figure 1. Hg0 observations are primarily successfully reproduces most observed Δ200Hg values in the
- remote mountain sites. Marine aerosol data were collected lightning activity, which has been suggested as a contributor
- collecting 52 HgII(p) samples from the western North Pacific, Peterborough, Ontario, Canada.45,50 In addition, the limited
- Pacific between 2018 and 2019. Qiu et al.48 collected and constrains model validation and introduces uncertainties into
- samples in the marginal seas of South and Southeast Asia in and their seasonal variations over the Indian Ocean, South
- aerosol samples collected along a cruise track from Shanghai, absence of corresponding observational data, which may
- precipitations samples are also primarily located in East Asia on the MBL environment. Nevertheless, despite these
- precipitation samples exhibit the highest levels of odd-MIF established Hg isotope fractionation mechanisms, providing
- minimal impact on the analysis of the modeling results. isotopes, primarily collected from regions distant from major
- respectively. Observations are represented points, which are collected from three studies.47−49.
- captures the Δ199Hg (0.22 ± 0.1‰) and Δ200Hg (0.16 ± the MBL (Figure 1a). These field measurements, collected at
- Ocean, central-eastern Pacific, and the Southern Ocean. Given All the collected data for validating the modeling results
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