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. The marine boundary layer (MBL) is the largest transport place andreaction vessel of atmospheric mercury (Hg). The transformations ofatmospheric Hg in the MBL are crucial for the global transport and deposition ofHg. Herein, Hg isotopic compositions of total gaseous mercury (TGM) andparticle-bound Hg (PBM) collected during three cruises to Chinese seas insummer and winter were measured to reveal the transformation processes ofatmospheric Hg in the MBL. Unlike the observation results at inland sites,isotopic compositions of TGM in the MBL were affected not only by mixingcontinental emissions but also largely by the oxidation of Hg0primarily derived by Br atoms. Δ199Hg values of TGM weresignificantly positively correlated with air temperature in summer,indicating that processes inducing positive mass-independent fractionationof odd isotopes in TGM could be more active at low temperatures, while therelative processes might be weak in winter. In contrast, the positiveΔ199Hg and high ratios of Δ199Hg∕Δ201Hg in PBM indicated that alternative oxidants other than Br or Clatoms played a major role in the formation of Hg(II) in PBM, likelyfollowing the nuclear volume effect. Our results suggest the importance oflocal Hg environmental behaviors caused by an abundance of highly reactivespecies and provide new evidence for understanding the complicatedtransformations of atmospheric Hg in the MBL.

New evidence for atmospheric mercury transformations in the marine boundary layer from stable mercury isotopes