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无机盐热力学平衡模式的简化及其应用
Simplification of an Inorganic Salt Thermodynamic Equilibrium Model and Its Application
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摘要: 利用查表法简化无机盐热力学平衡模式ISORROPIA，对温度、相对湿度、总氨（NH3+NH4+）、总氮（HNO3+NO3-）和总硫（H2SO4+SO42-）等5个影响因子进行分档，建立不同组合情况下硫酸盐、硝酸盐、铵盐等物种平衡浓度的查算表。在区域气候化学模式系统（RegCCMS）中，分别用查算表检索法和直接耦合热力学平衡模式的方法模拟我国2003年1月和7月硝酸盐气溶胶的浓度分布。结果表明：查表法既能显著提高计算效率，在无机盐模拟性能方面又与直接耦合法保持较好的一致性，在气溶胶气候效应研究方面具有良好的应用前景。Abstract:
In order to simulate the spatial distribution and temporal variation of volatile nitrate aerosols, it is necessary to introduce a thermodynamic equilibrium model and calculate the concentration under the state of equilibrium from the viewpoint of chemical thermodynamics. However, it costs much time to carry out a large scale and long term simulation because the thermodynamic equilibrium model contains a lot of species and reactions. The inorganic salt thermodynamic equilibrium model ISORROPIA is simplified using look up table method. A look up table for concentrations of 5 species (sulfate, nitrate, ammonium, nitric acid and ammonia) under the state of equilibrium is constructed according to various conditions of effecting factors (temperature, relative humidity, NH3+NH4+, HNO3+NO3- and HH2SO4+SO42-). The regional climate chemistry modeling system (RegCCMS) is an on line coupled modeling system which contains the regional climate model (RegCM3) and the tropospheric atmosphere chemistry model (TACM). The look up table scheme and the thermodynamic equilibrium model are introduced into TACM to treat nitrate, sulfate and ammonium. These two schemes are respectively adopted in RegCCMS to investigate spatial distribution of nitrate aerosol over China in January and July of 2003. Nitrate aerosol is mainly distributed in Sichuan, Yunnan, Guizhou, Hebei, Henan, Shandong in January and Henan, Hebei, Shandong, Jiangsu in July, which is roughly consistent with the distribution of the industry development. Influenced by temperature on thermodynamic equilibrium, wet scavenging of precipitation and the monsoon climate, the nitrate concentration is high in winter, and is very low in summer. The results of monthly average surface concentration show that look up table method has a good agreement with the thermodynamic equilibrium model in both quantity and distribution. The effect of look up table method is better on land than on ocean. Look up table method can save about 80% of the computing time compared with the thermodynamic equilibrium model, greatly improving the computational efficiency. The surface concentrations every 6 hours in several cities got from the look up table method and the thermodynamic equilibrium model are compared. The correlation coefficients of these two schemes in Chongqing, Xi'an and Xiamen are 0.99, 0.99, 0.97 in January and 0.75, 0.81, 0.86 in July. The results show that look up table method is able to simulate the characteristic of temporal variation. Due to higher temperature and humidity, differences between these two schemes are more obvious in July than those in January. As a whole, the look up table method can deal with the thermodynamic equilibrium processes successfully and reduce time for calculation significantly, therefore it has broad application prospect in research of climate effects of aerosols.
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图 1 直接耦合法 (a) 与查表法 (b) 得到的2003年1月硝酸盐气溶胶地面浓度分布 (单位:μg/ m3)
Fig. 1 Monthly average surface concentration of nitrate aerosol in January 2003(a) coupling method, (b) look-up table method (unit:μg/m3)
图 2 直接耦合法 (a) 与查表法 (b) 得到的2003年7月硝酸盐气溶胶地面浓度分布 (单位:μg/m3)
Fig. 2 Monthly average surface concentration of nitrate aerosol in July 2003(a) coupling method, (b) look-up table method (unit:μg/m3)
图 3 卫星观测、模拟得到的2003年1月和7月NO2柱含量 (单位:mg/m2)
Fig. 3 Monthly average NO2 column burden from satellite measurement andsimulation in January and July 2003 (unit:mg/m2)
图 4 部分城市2003年1月和7月雨水中NO3-浓度 (单位:μmol/ L)
Fig. 4 Concentr ation of NO3- in rainwater in January and July 2003(unit :μmol/L)
图 5 2003年1月和7月重庆、西安、厦门硝酸盐气溶胶每6 h地面浓度的变化
Fig. 5 Surface concent ration of nitrate aero solevery 6 hours of Chong qing, Xi' an, Xiamen in January and July 2003
表 1 查表法考虑的因子及分档
Table 1 Factors and their spectral bins for look-up table method
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