Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol

Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol
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SO2 和 NO2 在矿物氧化物上的协同反应:硫酸盐气溶胶的潜在形成途径

DOI:
10.1039/c1cp22217a
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发表时间:
2012-01-01
影响因子:
3.3
通讯作者:
He, Hong
He, Hong
中科院分区:
化学2区
文献类型:
--
作者:
Liu, Chang;Ma, Qingxin;He, Hong

文献摘要

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硫酸盐是大气中最重要的气溶胶之一。提出了SO2和NO2在矿物氧化物上协同反应生成硫酸盐的新途径。采用原位漫反射红外光谱(in situ DRIFTS)研究了SO2和NO2在CaO、α-Fe 2 O3、ZnO、MgO、α-Al 2 O3、TiO 2和SiO2上的非均相反应。共存的NO2促进了SO2吸附生成硫酸盐,而表面N2 O 4是表面亚硫酸盐氧化的关键氧化剂。这一过程显着促进了O-2的存在。SO2和NO2之间的协同效应没有观察到其他矿物颗粒(如CaCO 3和CaSO 4)可能是由于缺乏表面活性氧位点。SO2和NO2在矿物氧化物上的协同反应导致形成硫酸盐、硝酸盐和矿物氧化物的内部混合物。混合状态的变化会影响大气颗粒物的物理化学性质,进而影响其环境和气候效应。
Sulfate is one of the most important aerosols in the atmosphere. A new sulfate formation pathway via synergistic reactions between SO2 and NO2 on mineral oxides was proposed. The heterogeneous reactions of SO2 and NO2 on CaO, alpha-Fe2O3, ZnO, MgO, alpha-Al2O3, TiO2, and SiO2 were investigated by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in situ DRIFTS) at ambient temperature. Formation of sulfate from adsorbed SO2 was promoted by the coexisting NO2, while surface N2O4 was observed as the crucial oxidant for the oxidation of surface sulfite. This process was significantly promoted by the presence of O-2. The synergistic effect between SO2 and NO2 was not observed on other mineral particles (such as CaCO3 and CaSO4) probably due to the lack of the surface reactive oxygen sites. The synergistic reaction between SO2 and NO2 on mineral oxides resulted in the formation of internal mixtures of sulfate, nitrate, and mineral oxides. The change of mixture state will affect the physicochemical properties of atmospheric particles and therefore further influence their environmental and climate effects.