Heterogeneous uptake and reaction of nitrogen oxides and volatile organic compounds on the surface of atmospheric particles including oxides, carbonates, soot and mineral dust: Implications for the chemical balance of the troposphere
Heterogeneous uptake and reaction of nitrogen oxides and volatile organic compounds on the surface of atmospheric particles including oxides, carbonates, soot and mineral dust: Implications for the chemical balance of the troposphere
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DOI：
10.1080/01442350110051968
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发表时间：
2001-07
影响因子：
6.1
通讯作者：
V. Grassian
中科院分区：
文献类型：
--
作者：
V. Grassian
对流层中痕量大气气体在固体气溶胶表面上的非均相反应的作用还没有得到很好的理解。本文综述了氮氧化物和挥发性有机化合物在氧化物、烟尘、碳酸盐和矿物粉尘等大气相关颗粒物表面的非均相化学。解开分子水平的细节和这些反应的全球意义的方法是一个结合实验室调查和大气化学模型。实验室研究利用光谱测量来提供对气相中和颗粒表面上发生的化学细节的理解，以及动力学测量，以量化这些反应的速率。这些基本的测量为理解大气过程的详细分子水平物理化学提供了基础。动力学数据，连同光谱研究提供的细节，被纳入大气化学模型，以获得更好的理解的作用，多相化学在对流层的化学平衡中发挥。本文讨论了作者实验室的几个例子。这些例子包括：（i）氮氧化物的不均匀吸收和反应性（ii）水在氧化物、碳酸盐和灰尘颗粒上对硝酸的非均相吸收中的作用;（iii）二氧化硅和烟灰颗粒上亚硝酸的非均相产生;以及（iv）丙酮和其它羰基化合物对氧化物和矿物粉尘颗粒的非均相吸收和反应性。
The role of heterogeneous reactions of trace atmospheric gases on solid aerosol surfaces in the troposphere is not well understood. In this review, the heterogeneous chemistry of nitrogen oxides and volatile organic compounds on the surface of atmospherically relevant particles such as oxides, soot, carbonates and mineral dust is discussed. The approach to unravelling both the molecular level details and the global significance of these reactions is one that combines laboratory investigations and atmospheric chemistry models. The laboratory investigation utilizes spectroscopic measurements to provide an understanding of the details of the chemistry that occurs in the gas phase and on the surface of the particle together with kinetic measurements in order to quantify the rates of these reactions. These fundamental measurements provide a basis for understanding the detailed molecular level physical chemistry of atmospheric processes. The kinetic data, together with the details provided by the spectroscopic studies, are incorporated into atmospheric chemistry models in order to gain a greater understanding of the role that heterogeneous chemistry plays in the chemical balance of the troposphere. Several examples from the present author's laboratory are discussed in this review. These examples include: (i) the heterogeneous uptake and reactivity of nitrogen oxides (nitrogen dioxide and nitric acid) on oxide and dust particles; (ii) the role of water in the heterogeneous uptake of nitric acid on oxide, carbonate and dust particles; (iii) the heterogeneous production of nitrous acid on silica and soot particles; and (iv) the heterogeneous uptake and reactivity of acetone and other carbonyl compounds on oxide and mineral dust particles.