硝酸铵对SO2在大气颗粒物表面气-粒转化影响的模拟研究

高等学校化学学报 ›› 2010, Vol. 31 ›› Issue (4): 751.

硝酸铵对SO₂在大气颗粒物表面气-粒转化影响的模拟研究

林立, 孔令东, 陈建民

复旦大学环境科学与工程系大气化学研究中心, 上海 200433

收稿日期:2009-09-25 出版日期:2010-04-10 发布日期:2010-04-10
通讯作者: 孔令东, 男, 博士, 讲师, 主要从事大气化学与物理研究. E-mail: ldkong@fudan.edu.cn
基金资助:
国家自然科学基金(批准号: 40775079, 40875073, 40728006和40533017)资助.

Experimental Study of the Effects of Ammonium Nitrate on SO₂ Gas-particle Transfer on the Surface of Atmospheric Aerosols

LIN Li, KONG Ling-Dong*, CHEN Jian-Min

Center for the Atmospheric Chemistry Study, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China

Received:2009-09-25 Online:2010-04-10 Published:2010-04-10
Contact: KONG Ling-Dong. E-mail: ldkong@fudan.edu.cn
Supported by:
国家自然科学基金(批准号: 40775079, 40875073, 40728006和40533017)资助.

摘要/Abstract

摘要：

利用流动态的原位傅里叶变换红外漫反射光谱(DRIFTS)对含硝酸铵气溶胶(以α-Fe₂O₃为主模拟气溶胶)与SO₂的非均相反应进行了研究, 比较了硝酸铵与其它金属氧化物(CaO, MgO, α-Al₂O₃和SiO₂)与SO₂反应的情况.实验结果表明, 硝酸铵和α-Fe₂O₃混合颗粒物比硝酸铵和其它金属氧化物混合颗粒与SO₂反应的吸附系数高, 表明α-Fe₂O₃比其它金属氧化物催化能力变强.利用BET面积作为反应活性表面积, 发现含有6％(质量分数)NH₄NO₃的α-Fe₂O₃混合颗粒物与SO₂反应具有最高的比表面积吸附系数(γ_BET=2.42×10^-9), 比纯氧化铁的反应高了近1.8倍.而纯NH₄NO₃颗粒与SO₂不发生反应, 表明少量硝酸铵的存在在一定程度上提高了SO₂在气溶胶颗粒物表面转化成硫酸盐的能力. 本文还讨论了含硝酸铵气溶胶与SO₂的反应机制及其对大气环境的影响.

关键词: 含硝酸铵气溶胶; 二氧化硫; 红外漫反射; 非均相反应

Abstract:

Heterogeneous oxidation of gaseous SO₂ on NH₄NO₃-containing hematite compared to other NH₄NO₃-containing oxides(MgO, Al₂O₃, CaO, SiO₂) were first studied using an in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS). Obvious sulfate formation can be seen from the infrared spectrum of NH₄NO₃-containing oxides, and the catalytic activity of hematite is much higher compared to other oxides. Using BET area as the reactive surface area, the hematite sample containing 6%(mass fraction) of NH₄NO₃ presents the highest γ_BET value(2.42×10^-9), which is about 1.8 times larger than that of hematite. No formation of sulfate is observed on the pure NH₄NO₃. The results show that appropriate NH₄NO₃ increases the sulfate formation while more NH₄NO₃ impedes. Mechanism is discussed.

Key words: NH4NO3-Containing aerosols; Sulfur dioxide; In-situ diffuse reflectance infrared Fourier transform spectroscopy; Heterogeneous reaction

TrendMD:

林立, 孔令东, 陈建民. 硝酸铵对SO₂在大气颗粒物表面气-粒转化影响的模拟研究. 高等学校化学学报, 2010, 31(4): 751.

LIN Li, KONG Ling-Dong*, CHEN Jian-Min. Experimental Study of the Effects of Ammonium Nitrate on SO₂ Gas-particle Transfer on the Surface of Atmospheric Aerosols. Chem. J. Chinese Universities, 2010, 31(4): 751.

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硝酸铵对SO₂在大气颗粒物表面气-粒转化影响的模拟研究

Experimental Study of the Effects of Ammonium Nitrate on SO₂ Gas-particle Transfer on the Surface of Atmospheric Aerosols

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