Heterogeneous reaction of NO2 on Al2O3: the effect of temperature on the nitrite and nitrate formation.
Heterogeneous reaction of NO2 on Al2O3: the effect of temperature on the nitrite and nitrate formation.
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DOI：
10.1021/jp402773c
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发表时间：
2013-05
期刊：
影响因子：
--
通讯作者：
Lingyan Wu;Shengrui Tong;Maofa Ge
中科院分区：
文献类型：
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作者：
Lingyan Wu;Shengrui Tong;Maofa Ge
虽然最近的证据表明，NO2在矿物气溶胶表面的非均相反应在大气化学中起着重要的作用，但对温度如何影响硝酸盐形成过程的速率和程度的基本理解仍然不清楚。本文首次在实验室研究了常压、250-318 K温度范围内NO_2在γ-Al_2O_3表面上的非均相反应。红外光谱分析表明，在250 ~ 318 K温度范围内，亚硝酸根是中间产物。实验证明，随着反应的进行，亚硝酸根会转化为双齿硝酸根。此外，有趣的是发现转化率随着温度的降低而增加。沿着亚硝酸盐的减少，硝酸盐的初始生成速率增加，而稳定区的硝酸盐生成速率随温度的降低而降低。在季节性温度下的吸收系数被确定为第一次，并被发现是敏感的温度。最后，大气中的温度的作用的非均相反应的NO2与矿物气溶胶的影响进行了讨论。
Although recent evidence suggests that the heterogeneous reaction of NO2 on the surface of mineral aerosol plays an important role in the atmospheric chemistry, a fundamental understanding of how temperature influences the rate and extent of nitrate formation processes remains unclear. This work presents the first laboratory study of the effect of temperature on heterogeneous reaction of NO2 on the surface of γ-Al2O3 in the temperature range of 250-318 K at ambient pressure. From the analysis of IR spectra, nitrite was found to be an intermediate product at temperatures between 250 and 318 K. It is proved by our experiments that nitrite would convert to the bidentate nitrate as the reaction proceeded. In addition, it is interesting to find that the rate of conversion increased with decreasing temperature. Along with nitrite decrease, the initial rate of nitrate formation increased while the rate of nitrate formation in the steady region decreased with decreasing temperature. The uptake coefficients at seasonal temperatures were determined for the first time and were found to be sensitive to temperature. Finally, atmospheric implications of the role of temperature on the heterogeneous reaction of NO2 with mineral aerosol are discussed.