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DOI10.1029/2023MS003823
Improving Simulation of Gas-Particle Partitioning of Atmospheric Mercury Using CMAQ-newHg-Br v2
发表日期2024
EISSN1942-2466
起始页码16
结束页码3
卷号16期号:3
英文摘要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, ) 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 mu gm2 in the 11-month accumulated amount, offsetting half of the decreasing effect of the updated chemistry (-4.2 +/- 1.8 mu gm2). 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. 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. CMAQ-newHg-Br was updated to version 2 with a new gas-particle partitioning (GPP) scheme and the most up-to-date Hg redox chemistry CMAQ-newHg-Br v2 better simulated gaseous elemental mercury (GEM), particulate bound mercury (PBM) and Hg wet deposition The new GPP scheme captured the observed Kp-T relation not using measurement data and improved nighttime and less polluted simulations
英文关键词gas-particle partitioning; atmospheric mercury; CMAQ
语种英语
WOS研究方向Meteorology & Atmospheric Sciences
WOS类目Meteorology & Atmospheric Sciences
WOS记录号WOS:001181528800001
来源期刊JOURNAL OF ADVANCES IN MODELING EARTH SYSTEMS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/294957
作者单位State University of New York (SUNY) System; State University of New York (SUNY) College of Environmental Science & Forestry; Aarhus University; Aarhus University; Consejo Superior de Investigaciones Cientificas (CSIC); CSIC - Instituto de Quimica Fisica Rocasolano (IQFR); Nanjing University
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GB/T 7714
. Improving Simulation of Gas-Particle Partitioning of Atmospheric Mercury Using CMAQ-newHg-Br v2[J],2024,16(3).
APA (2024).Improving Simulation of Gas-Particle Partitioning of Atmospheric Mercury Using CMAQ-newHg-Br v2.JOURNAL OF ADVANCES IN MODELING EARTH SYSTEMS,16(3).
MLA "Improving Simulation of Gas-Particle Partitioning of Atmospheric Mercury Using CMAQ-newHg-Br v2".JOURNAL OF ADVANCES IN MODELING EARTH SYSTEMS 16.3(2024).
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