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Nitrate-dominated PM2.5 and elevation of particle pH observed in urban Beijing during the winter of 2017

机译:2017年冬季,北京市观察到硝酸硝酸盐的PM2.5和颗粒pH的升高

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The Chinese government has exerted strict emission controls to mitigate air pollution since 2013, which has resulted in significant decreases in the concentrations of air pollutants such as SO2. Strict pollution control actions also reduced the average PM2.5 concentration to the low level of 39.7μg?m?3 in urban Beijing during the winter of 2017. To investigate the impact of such changes on the physiochemical properties of atmospheric aerosols in China, we conducted a comprehensive observation focusing on PM2.5 in Beijing during the winter of 2017. Compared with the historical record (2014–2017), SO2 decreased to the low level of 3.2ppbv in the winter of 2017, but the NO2 level was still high (21.4ppbv in the winter of 2017). Accordingly, the contribution of nitrate (23.0μg?m?3) to PM2.5 far exceeded that of sulfate (13.1μg?m?3) during the pollution episodes, resulting in a significant increase in the nitrate-to-sulfate molar ratio. The thermodynamic model (ISORROPIA?II) calculation results showed that during the PM2.5 pollution episodes particle pH increased from 4.4 (moderate acidic) to 5.4 (more neutralized) when the molar ratio of nitrate to sulfate increased from 1 to 5, indicating that aerosols were more neutralized as the nitrate content elevated. Controlled variable tests showed that the pH elevation should be attributed to nitrate fraction increase other than crustal ion and ammonia concentration increases. Based on the results of sensitivity tests, future prediction for the particle acidity change was discussed. We found that nitrate-rich particles in Beijing at low and moderate humid conditions (RH: 20%–50%) can absorb twice the amount of water that sulfate-rich particles can, and the nitrate and ammonia with higher levels have synergetic effects, rapidly elevating particle pH to merely neutral (above 5.6). As moderate haze events might occur more frequently under abundant ammonia and nitrate-dominated PM2.5 conditions, the major chemical processes during haze events and the control target should be re-evaluated to obtain the most effective control strategy.
机译:自2013年以来,中国政府施加了严格的排放管制,以减轻空气污染,这导致了在SO2等空气污染物的浓度下显着降低。严格的污染控制行动也将平均PM2.5的浓度降低到2017年冬季城市北京中的低水平39.7μg?3。为了调查这种变化对中国大气气溶胶的生理化学特性的影响在2017年冬季进行了一项综合观察,重点关注北京的PM2.5。与历史记录(2014-2017)相比,SO2在2017年冬季减少到3.2ppbv的低水平,但No2水平仍然很高(21.4PPBV在2017年冬天)。因此,在污染发作期间,硝酸盐(23.0μg≤3)至pm2.5的贡献远远超过硫酸盐(13.1μg≤M≤3),导致硝酸盐 - 硫酸盐摩尔比例显着增加。热力学模型(Isorropia?II)计算结果表明,在PM2.5污染发作期间颗粒pH从4.4(中等酸性)增加到5.4(更浓度),当硝酸盐与硫酸盐增加到5时,表明随着硝酸盐含量升高,气溶胶更中和。受控变量试验表明,pH升高应归因于除菌离子和氨浓度的硝酸盐馏分增加。基于灵敏度试验的结果,讨论了对颗粒酸度变化的未来预测。我们发现北京富含硝酸盐的颗粒在北京(RH:20%-50%)可以吸收富含硫酸盐的颗粒的水两倍,硝酸盐和氨具有较高水平具有协同作用,快速升高颗粒pH以仅中性(5.6以上)。随着中度雾度事件可能在丰富的氨和硝酸盐支配的PM2.5条件下更频繁地发生,应重新评估雾度事件和对照目标期间的主要化学过程,以获得最有效的控制策略。

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