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Impact of Crop Residue Burning on PM2.5 Inorganic Components in Beijing-Tianjin-Hebei and Surrounding Areas
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摘要: 华北平原是我国主要农作物产区，田间秸秆焚烧现象普遍存在，选取秋收季节（2014年10月）分析了秸秆燃烧的排放特征，利用区域化学传输模型WRF-Chem模拟研究了燃烧排放对气态前体物及其氧化产物的影响，以及最终导致的PM2.5中硫酸盐、硝酸盐和铵盐的变化。研究表明：2014年秋收季节，河南和山东等省份的秸秆燃烧排放会在东南风的输送作用下影响京津冀地区；秸秆燃烧排放大量挥发性有机物（VOCs），导致火点源及周边地区大气中主要氧化剂浓度上升，提升了区域大气氧化能力；当携带大量VOCs的秸秆燃烧烟羽与以化石燃料排放为主的城市气团相混合时，大气氧化性增强会加速城市地区人为源排放的NOx和SO2等气态前体物的氧化过程，提高硫酸盐和硝酸盐的形成速率、促进二次无机气溶胶的生成。Abstract: Tremendous advances in atmospheric aerosol particle research have taken place in the last decade in the context of climate and global change science. Biomass burning, one of the largest sources of accumulation mode particles globally, is closely studied for its radiative, geochemical, and dynamic impacts. In addition to primary aerosols such as organic carbon (OC) and black carbon (BC), straw burning emits a large amount of gaseous precursor of aerosols. The transformation of these gaseous precursors to secondary aerosols is one of the important ways to the formation of heavy pollution episodes. Due to rapid economic growth and urbanization in China, crop residues are often burnt in a couple of days post harvests to prepare for planting the next season's crops. The North China Plain is a major agricultural base in China with straw burning widely in the field. Remote sensing data, ground monitoring data, meteorological data are used for analyzing effects on the haze pollution from autumn crop residue burning over Beijing-Tianjin-Hebei area. Results indicate that lots of heavy pollution processes are related to the pollutant transmission from the crop residue burning in surrounding regions. Emission characteristics of straw burning during the autumn harvest season (October 2014) are analyzed, using the regional chemical transport model WRF-Chem. Effects of straw burning on gaseous precursors of inorganic aerosols and their oxidation products as well as resulting changes of sulfate, nitrate and ammonium in PM2.5 are studied. It's found that during the autumn harvest season of 2014, the straw burning emissions in Henan and Shandong provinces tend to affect Beijing-Tianjin-Hebei urban areas under the influence of the southeast wind. A large number of VOCs emitted by straw burning lead to an increase in the concentration of major oxidants in the atmosphere which enhances the regional atmospheric oxidation capacity. When the straw burning plume carrying a large number of VOCs is mixed with the urban air mass mainly composed of fossil fuel emissions, the increase of atmospheric oxidation accelerates the oxidation process of gaseous precursors such as NO2 and SO2 emitted by anthropogenic sources and increases the conversion rate of sulfate and nitrate. Ammonia-rich state in Beijing-Tianjin-Hebei area are favorable for the formation of secondary inorganic aerosols, and straw burning intensifies the development of this process, and then results in a significant increase in the concentration of nitrate, sulfate and ammonium.
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图 1 模拟区域(蓝框为内层区域)及2014年10月MODIS火点分布(红点)(a), 秸秆燃烧源CO格点平均月排放量区域分布(b)
Fig. 1 Modeling area(the blue frame) and spatial distributions of MODIS fire counts(red dots)(a), regional distribution of monthly mean CO emission load for each grid of straw burning(b) in Oct 2014
图 3 2014年10月秸秆燃烧排放导致日间(07:00—18:00)地面RO2和HO2月平均浓度变化量区域分布
Fig. 3 Regional distributions of monthly-averaged changes of surface RO2 and HO2 during the daytime(0700 BT-1800 BT) due to the straw burning in Oct 2014
图 4 2014年10月秸秆燃烧排放导致NOx和SO2月平均浓度变化量区域分布
Fig. 4 Regional distributions of monthly-averaged changes of surface NOx and SO2 due to the straw burning in Oct 2014
图 5 2014年10月秸秆燃烧排放导致HNO3和S(Ⅵ)月平均浓度变化量区域分布
Fig. 5 Regional distributions of monthly-averaged changes of surface HNO3 and hexavalent sulfur due to the straw burning in Oct 2014
图 6 2014年10月秸秆燃烧排放导致SOR及NOR变化量月平均值的区域分布
Fig. 6 Regional distributions of monthly-averaged changes of surface SOR and NOR due to the straw burning in Oct 2014
图 7 2014年10月秸秆燃烧排放导致SNA月平均变化的区域分布
Fig. 7 Regional distributions of monthly-averaged SNA changes due to the straw burning in Oct 2014
表 1 模式内层区域主要污染物月排放量对比统计
Table 1 Monthly emission statistics of major pollutants in the inner layer of the model
污染物 人为排放 秸秆燃烧排放 秸秆燃烧排放占人为排放比例/% CO 4.9×106 t 1.2×105 t 2.4 SO2 9.2×105 t 0.4×103 t 0.1 NOx 1.03×106 t 6×103 t 0.6 VOCs 8.1×109 mol 1.1×109 mol 14.0 NH3 2.52×105 t 2.4×103 t 0.9 OC 7.2×104 t 3.6×103 t 5.0 BC 5.1×104 t 0.7×103 t 1.4 PM2.5 3.6×105 t 6.3×103 t 1.8 
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表 2 气象要素模拟与观测小时平均值对比
Table 2 Comparison of hourly mean values of meteorological elements between simulation and observation
统计量 温度 相对湿度 风速 有效数据对 46573 46428 42157 观测平均值 287.6 K 64.1% 2.0 m·s-1 模拟平均值 287.2 K 67.7% 3.6 m·s-1 平均偏差 -0.48 K 3.6% 1.5 m·s-1 归一化平均偏差 -0.002 0.057 0.7 相关系数 0.9 0.6 0.6
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表 3 地面NO2, SO2, PM2.5浓度模拟值与观测值对比
Table 3 Comparison of NO2, SO2, PM2.5 between simulation and observation
统计量 NO2 SO2 PM2.5 有效数据对 3244 3180 3180 观测平均值/(μg·m-3) 46.01 34.2 75.36 模拟平均值/(μg·m-3) 44.99 46.71 77.21 平均偏差/(μg·m-3) -1.02 12.51 1.86 归一化平均偏差 -0.07 0.37 0.02 相关系数 0.61 0.35 0.70
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