Effect of Formaldehyde on the Heterogeneous Reaction of Nitrogen Dioxide on γ-Alumina.
Effect of Formaldehyde on the Heterogeneous Reaction of Nitrogen Dioxide on γ-Alumina.
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DOI：
10.1021/acs.jpca.5b06632
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发表时间：
2015-08
期刊：
影响因子：
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通讯作者：
Zhenyu Sun;Lingdong Kong;Xi Zhao;Xiaoxia Ding;Hongbo Fu;T. Cheng;Xin Yang;Jianmin Chen
中科院分区：
文献类型：
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作者：
Zhenyu Sun;Lingdong Kong;Xi Zhao;Xiaoxia Ding;Hongbo Fu;T. Cheng;Xin Yang;Jianmin Chen
NO2在各种矿物气溶胶颗粒上的非均相反应在以前的许多研究中已经进行了研究，但甲醛的吸附如何影响NO2的非均相反应的基本认识仍然不清楚。采用漫反射红外傅里叶变换光谱（DRIFTS）研究了298 K和常压下甲醛预吸附对NO2在γ-Al 2 O3表面非均相反应的影响。结果表明，HCHO在γ-Al 2 O3上的预吸附抑制了硝酸盐的生成，且硝酸盐的生成速率随预吸附量的增加而降低;而随后的NO2非均相吸附则抑制了HCHO的水合反应，促进了HCOO（-）的生成。表面亚硝酸盐的形成和鉴定是一个中间产物，并逐渐消失，随着反应的进行。亚硝酸盐的生成量随甲醛添加量的增加而减少。非均相反应的吸收系数进行了计算，发现是敏感的甲醛的吸附。提出了甲醛吸附对γ-Al 2 O3上NO2非均相转化影响的可能机理，并对这些结果的大气意义进行了讨论。
Heterogeneous reactions of NO2 on various mineral aerosol particles have been investigated in many previous studies, but a fundamental understanding of how the adsorption of formaldehyde influences the heterogeneous reactions of NO2 remains unclear. In this work, the effect of formaldehyde preadsorption on heterogeneous reaction of NO2 on the surface of γ-Al2O3 at 298 K and ambient pressure was investigated by using diffuse reflectance infrared Fourier transform spectrometry (DRIFTS). It was found that the preadsorption of HCHO on γ-Al2O3 could suppress the formation of nitrate, and the rate of nitrate formation decreased with increasing amount of preadsorbed HCHO, whereas the following heterogeneous uptake of NO2 could suppress the hydration reaction of HCHO and promote the production of HCOO(-) during the reaction. Surface nitrite was formed and identified to be an intermediate product and gradually disappeared as the reaction proceeded. The amount of the formed nitrite decreased when the amount of HCHO increased. Uptake coefficients of heterogeneous reactions were calculated and found to be sensitive to the adsorption of HCHO. A possible mechanism for the influence of HCHO adsorption on the heterogeneous conversion of NO2 on γ-Al2O3 was proposed, and atmospheric implications based on these results were discussed.