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Concentrations and biosphere–atmosphere fluxes of inorganic trace gases and associated ionic aerosol counterparts over the Amazon rainforest

机译:无机痕量气体的浓度和生物圈 - 大气助气和亚马逊雨林上的相关离子气溶胶对应物

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The Amazon rainforest presents a unique, natural laboratory for the study of surface–atmosphere interactions. Its alternation between a near-pristine marine-influenced atmosphere during the wet season and a vulnerable system affected by periodic intrusions of anthropogenic pollution during the dry season provides an opportunity to investigate some fundamental aspects of boundary-layer chemical processes. This study presents the first simultaneous hourly measurements of concentrations, fluxes, and deposition velocities of the inorganic trace gases NH 3 , HCl , HONO , HNO 3 , and SO 2 as well as their water-soluble aerosol counterparts NH 4 + , Cl ? , NO 2 - , NO 3 - and SO 4 2 - over the Amazon. Species concentrations were measured in the dry season (from 6?October to 5?November 2017), at the Amazon Tall Tower Observatory (ATTO) in Brazil, using a two-point gradient wet-chemistry instrument (GRadient of AErosols and Gases Online Registration, GRAEGOR) sampling at 42 and 60? m . Fluxes and deposition velocities were derived from the concentration gradients using a modified form of the aerodynamic gradient method corrected for measurement within the roughness sub-layer. Findings from this campaign include observations of elevated concentrations of NH 3 and SO 2 partially driven by long-range transport (LRT) episodes of pollution and the substantial influence of coarse Cl ? and NO 3 - particulate on overall aerosol mass burdens. From the flux measurements, the dry season budget of total reactive nitrogen dry deposition at the ATTO site was estimated as ?2.9 ? kg N? ha - 1 a - 1 . HNO 3 and HCl were deposited continuously at a rate close to the aerodynamic limit. SO 2 was deposited with an average daytime surface resistance ( R c ) of 28? s?m ?1 , whilst aerosol components showed average surface deposition velocities of 2.8 and 2.7? mm?s ?1 for SO 4 2 - and NH 4 + , respectively. Deposition rates of NO 3 - and Cl ? were higher at 7.1 and 7.8? mm?s ?1 , respectively, reflecting their larger average size. The exchange of NH 3 and HONO was bidirectional, with NH 3 showing emission episodes in the afternoon and HONO in the early morning hours. This work provides a unique dataset to test and improve dry deposition schemes for these compounds for tropical rainforest, which have typically been developed by interpolation from conditions in temperate environments. A future campaign should focus on making similar measurements in the wet season in order to provide a complete view of the annual pattern of inorganic trace gas and coarse aerosol biosphere–atmosphere exchange over tropical rainforest.
机译:亚马逊雨林呈现出一种独特的自然实验室,用于研究地表 - 大气相互作用。它在湿季期间近乎原始海洋影响的气氛之间的交替以及受干燥季节期间人为污染的周期性侵入影响的脆弱系统提供了调查边界层化学过程的一些基本方面的机会。本研究介绍了无机痕量气体NH 3,HCl,Hono,HNO 3和SO 2以及它们的水溶性气溶胶对应物NH 4 +,CL的浓度,助熔剂和沉积速度的第一次同时测量的第一次同时测量。在亚马逊,没有2 - ,第3 - 等等4 2 - 物种浓度在干燥的季节测量(从6月到5月到2017年11月),在巴西的亚马逊高塔观测所(Atto),使用两点梯度湿化学仪器(在线登记的气溶胶和气体梯度,格劳格)在42和60时抽样? m。使用用于在粗糙度子层内测量的校正的空气动力学梯度方法的改性形式,从浓度梯度衍生通量和沉积速度。来自该运动的调查结果包括观察由远程运输(LRT)污染的远程运输(LRT)发作的升高浓度的NH 3和SO 2以及粗克的大量影响?没有3-颗粒在整体气溶胶质量负担上。从磁通量测量,估计ATTO部位的总反应性氮气干燥沉积的干燥季预算估计为?2.9? kg n? HA - 1 A - 1。 HNO 3和HCl以靠近空气动力学极限的速率连续沉积。所以2沉积了平均白天表面电阻(R C)为28? s?m?1,虽然气溶胶组分显示平均表面沉积速度为2.8和2.7? mm?s?1分别为SO 4 2 - 和NH 4 +。沉积率为3 - 和cl? 7.1和7.8较高? MM?S?1,分别反映其较大的平均尺寸。 NH 3和Hono的交换是双向的,NH 3在清晨的时间内显示了下午和霍诺的排放集。这项工作提供了独特的数据集来测试和改善热带雨林的这些化合物的干燥沉积方案,这通常是由温带环境中的条件的插值而开发的。未来的竞选活动应该专注于在潮湿的季节进行类似的测量,以便在热带雨林上提供完整的无机痕量气体和粗气溶胶生物圈 - 氛围的年度模式。

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