Improving Simulation of Gas‐Particle Partitioning of Atmospheric Mercury Using CMAQ‐newHg‐Br v2.

Mercury (Hg) is a global pollutant whose atmospheric deposition is a major input to the terrestrial and oceanic ecosystems. Gas‐particle partitioning (GPP) of gaseous oxidized mercury (GOM) redistributes speciated Hg between gas and particulate phase and can subsequently alter Hg deposition flux. Most 3‐dimensional chemical transport models either neglected the Hg GPP process or parameterized it with measurement data limited in time and space. In this study, CMAQ‐newHg‐Br (Ye et al., 2018, https://doi.org/10.1002/2017ms001161) was updated to CMAQ‐newHg‐Br v2 by implementing a new GPP scheme and the most up‐to‐date Hg redox chemistry and was run for the northeastern United States over January‐November 2010. CMAQ‐newHg‐Br v2 reproduced the measured spatiotemporal distributions of gaseous elemental mercury (GEM) and particulate bound mercury (PBM) concentrations and Hg wet deposition flux within reasonable ranges and simulated dry deposition flux in agreement with previous studies. The GPP scheme improved the simulation of PBM via increasing winter‐, spring‐ and fall‐time PBM concentrations by threefold. It also improved simulated Hg wet deposition flux with an increase of 2.1 ± 0.7 μgm2 in the 11‐month accumulated amount, offsetting half of the decreasing effect of the updated chemistry (−4.2 ± 1.8 μgm2). Further, the GPP scheme captured the observed Kp‐T relationship as reported in previous studies without using measurement data and showed advantages at night and in rural/remote areas where existing empirical parameterizations failed. Our study demonstrated CMAQ‐newHg‐Br v2 a promising assessment tool to quantify impacts of climate change and emission reduction policy on Hg cycling. Plain Language Summary: Mercury is a toxic global pollutant and can enter the food chain through atmospheric deposition to ecosystems. Atmospheric mercury was defined operationally in the forms of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM) and particulate bound mercury (PBM). GEM is relatively inert, but GOM and PBM are highly soluble and readily removed from the air via deposition. GEM gets oxidized to GOM and GOM can be transformed to PBM through gas particle partitioning (GPP). CMAQ‐newHg‐Br v2 was updated from its predecessor via implementing the most up‐to‐date Hg redox chemistry and a new GPP scheme. The model improved the simulation of GEM, PBM, and Hg wet deposition. Most notably the model reproduced the observed partitioning coefficient and temperature relationship (Kp‐T) and improved nighttime and less polluted PBM simulations. CMAQ‐newHg‐Br v2 can be used to assess how climate change and emission reduction policy impact environmental Hg cycling. Key Points: CMAQ‐newHg‐Br was updated to version 2 with a new gas‐particle partitioning (GPP) scheme and the most up‐to‐date Hg redox chemistryCMAQ‐newHg‐Br v2 better simulated gaseous elemental mercury (GEM), particulate bound mercury (PBM) and Hg wet depositionThe new GPP scheme captured the observed Kp‐T relation not using measurement data and improved nighttime and less polluted simulations [ABSTRACT FROM AUTHOR]