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Mercury (Hg) emission from natural surfaces plays an important role in globalHg cycling. The present estimate of global natural emission has largeuncertainty and remains unverified against field data, particularly forterrestrial surfaces. In this study, a mechanistic model is developed forestimating the emission of elemental mercury vapor (Hg0) from naturalsurfaces in China. The development implements recent advancements in theunderstanding of air–soil and air–foliage exchange of Hg0 and redoxchemistry in soil and on surfaces, incorporates the effects of soilcharacteristics and land use changes by agricultural activities, and isexamined through a systematic set of sensitivity simulations. Using themodel, the net exchange of Hg0 between the atmosphere and naturalsurfaces of mainland China is estimated to be 465.1 Mg yr−1, including565.5 Mg yr−1 from soil surfaces, 9.0 Mg yr−1 from waterbodies, and −100.4 Mg yr−1 from vegetation. The air–surfaceexchange is strongly dependent on the land use and meteorology, with 9 %of net emission from forest ecosystems; 50 % from shrubland, savanna, andgrassland; 33 % from cropland; and 8 % from other land uses. Giventhe large agricultural land area in China, farming activities play animportant role on the air–surface exchange over farmland. Particularly, ricefield shift from a net sink (3.3 Mg uptake) during April–October (riceplanting) to a net source when the farmland is not flooded (November–March).Summing up the emission from each landuse, more than half of the total emission occurs in summer (51 %),followed by spring (28 %), autumn (13 %), and winter (8 %). Modelverification is accomplished using observational data of air–soil/air–waterfluxes and Hg deposition through litterfall for forest ecosystems in Chinaand Monte Carlo simulations. In contrast to the earlier estimate by Shetty etal. (2008) that reported large emission from vegetative surfaces using anevapotranspiration approach, the estimate in this study shows naturalemissions are primarily from grassland and dry cropland. Such an emissionpattern may alter the current understanding of Hg emission outflow from Chinaas reported by Lin et al. (2010b) because a substantial natural Hg emissionoccurs in West China

Emission-dominated gas exchange of elemental mercury vapor over natural surfaces in China