Heterogeneous reactions between NO2 and anthracene adsorbed on SiO2 and MgO

Heterogeneous reactions between NO2 and anthracene adsorbed on SiO2 and MgO
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NO2与SiO2和MgO上吸附的蒽的非均相反应

DOI:
10.1016/j.atmosenv.2010.11.012
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发表时间:
2011-02
影响因子:
5
通讯作者:
He, Hong
He, Hong
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Ma, Jinzhu;Liu, Yongchun;He, Hong

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利用DRIFTS、GCMS和UV-Vis研究了二氧化氮与蒽吸附在二氧化硅和氧化镁上的非均相反应。通过拟合吸附多环芳烃浓度随反应时间的指数衰减,得到了蒽在sio2和MgO上的准一级速率常数。当no2浓度为3.69 × 1012分子cm−3时,在sio2上的反应速度比在MgO上的反应快近2倍。9-硝基蒽和9,10-蒽醌都是蒽吸附在sio2上的硝化产物,而9,10-蒽醌是二氧化氮与MgO吸附的蒽反应的唯一产物。这些结果表明,矿物氧化物不仅控制了多环芳烃与NO2的反应动力学,而且改变了多环芳烃与NO2的非均相反应途径。NO2与蒽吸附在SiO2和MgO上的非均相反应活性差异的主要原因是在SiO2上形成hno3,而hno3可以催化NO2对PAHs的硝化作用。由于硝基蒽和氧基蒽的形成,no2与蒽的非均相反应也改变了吸附蒽的矿物氧化物的光学性质。
The heterogeneous reactions of NO2with anthracene adsorbed on SiO2and MgO were investigated under dark conditions at 298 K using DRIFTS, GCMS, and UV–Vis. The pseudo-first-order rate constants of anthracene on SiO2and MgO were obtained by fitting the exponential decay of adsorbed PAH concentrations versus reaction time. The reaction on SiO2was almost two times faster than on MgO when the concentration of NO2was 3.69 × 1012molecules cm−3. Both 9-nitroanthracene and 9,10-anthraquinone were the products of the nitration of anthracene adsorbed on SiO2whereas 9,10-anthraquinone was the only product formed by NO2reaction with anthracene adsorbed on MgO. These results suggest that mineral oxides not only control the reaction kinetics of PAHs with NO2but also alter the reaction pathway for the heterogeneous reaction of PAHs with NO2. The difference in the heterogeneous reactivity of NO2with anthracene adsorbed on SiO2and MgO was ascribed to the formation of HNO3on SiO2, which can catalyze the nitration of PAHs by NO2. Due to the formation of nitro-anthracene and oxy-anthracene, the heterogeneous reactions of NO2with anthracene also altered the optical properties of the mineral oxides on which anthracene were adsorbed.
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发表时间: 2005-11
影响因子: 5
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