Transport and transformation of sulfur compounds over East Asia during the TRACE-P and ACE-Asia campaigns

Transport and transformation of sulfur compounds over East Asia during the TRACE-P and ACE-Asia campaigns
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DOI:
10.1016/j.atmosenv.2004.02.073
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发表时间:
2004-12
影响因子:
5
通讯作者:
Meigen Zhang;I. Uno;Y. Yoshida;Yongfu Xu;Zifa Wang;H. Akimoto;T. Bates;Trish Quinn;A. Bandy;B. Blomquist
Meigen Zhang;I. Uno;Y. Yoshida;Yongfu Xu;Zifa Wang;H. Akimoto;T. Bates;Trish Quinn;A. Bandy;B. Blomquist
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Meigen Zhang;I. Uno;Y. Yoshida;Yongfu Xu;Zifa Wang;H. Akimoto;T. Bates;Trish Quinn;A. Bandy;B. Blomquist

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以最近估算的东亚地区排放物清单(1×1°)为基础,利用mods -3社区多尺度空气质量(CMAQ)模拟系统和区域大气模拟系统(RAMS)计算的气象场,研究了2001年2月22日至5月4日东亚地区硫化合物的运输和化学转化。为了评估模型的性能,将模拟的二氧化硫(SO2)和气溶胶硫酸盐(SO42−)浓度与日本四个偏远站点的地面观测数据以及太平洋和亚太地区气溶胶表征实验场运动期间的飞机和船舶观测数据进行了比较,发现该模型再现了观测数据中的许多重要特征。包括水平和垂直梯度。so2和SO42 -浓度在时间和空间上表现出明显的变化,由于化学转化、去除和运输过程的相互作用,so2和SO42 -表现不同。模型结果分析表明,排放是调节so2空间分布的主导因素,而so2在气相和水相转化为SO42−和湿法去除是控制SO42−量的主要因素。气相和水相在氧化SO2中具有同样的重要性,在研究期间,模型域中排放的约42%的硫化合物(SO2中约25%)被输送出去,而约57%(湿法去除过程约35%)沉积在该区域。
On the basis of the recently estimated emission inventory for East Asia with a resolution of 1×1°, the transport and chemical transformation of sulfur compounds over East Asia during the period of 22 February through 4 May 2001 was investigated by using the Models-3 Community Multi-scale Air Quality (CMAQ) modeling system with meteorological fields calculated by the regional atmospheric modeling system (RAMS). For evaluating the model performance simulated concentrations of sulfur dioxide (SO2) and aerosol sulfate (SO42−) were compared with the observations on the ground level at four remote sites in Japan and on board aircraft and vessel during the transport and chemical evolution over the Pacific and Asian Pacific regional aerosol characterization experiment field campaigns, and it was found that the model reproduces many of the important features in the observations, including horizontal and vertical gradients. The SO2and SO42−concentrations show pronounced variations in time and space, with SO2and SO42−behaving differently due to the interplay of chemical conversion, removal and transport processes. Analysis of model results shows that emission was the dominant term in regulating the SO2spatial distribution, while conversion of SO2to SO42−in the gas phase and the aqueous phase and wet removal were the primary factors that controlled SO42−amounts. The gas phase and the aqueous phase have the same importance in oxidizing SO2, and about 42% sulfur compounds (∼25% in SO2) emitted in the model domain was transported out, while about 57% (∼35% by wet removal processes) was deposited in the domain during the study period.