高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

甲醛在α-Al2O3颗粒物表面的非均相反应研究

徐冰烨, 朱彤, 唐孝炎, 丁杰, 李宏军   

  1. 北京大学环境学院, 环境模拟与污染控制国家重点实验室, 北京 100871
  • 收稿日期:2005-12-06 修回日期:1900-01-01 出版日期:2006-10-10 发布日期:2006-10-10
  • 通讯作者: 朱彤

Heterogeneous Reaction of Formaldehyde on Surface of α-Al2O3 Particles

XU Bing-Ye, ZHU Tong, TANG Xiao-Yan, DING Jie, LI Hong-Jun   

  1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences, Peking University, Beijing 100871, China
  • Received:2005-12-06 Revised:1900-01-01 Online:2006-10-10 Published:2006-10-10
  • Contact: ZHU Tong

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摘要： 使用漫反射傅里叶变换红外光谱(DRIFTS)原位反应器研究了273~333 K下甲醛与α-Al2O3颗粒物表面的非均相反应. 结果表明, 甲醛在α-Al2O3颗粒物表面生成产物主要为甲酸盐、二氧亚甲基以及少量多聚甲醛和吸附态甲醛, 甲酸盐是由中间产物二氧亚甲基进一步氧化生成的. 在293 K下, 甲醛在α-Al2O3颗粒物表面的反应级数为0.81±0.05, 以样品池几何面积计算的初始摄取系数γ0GEO为(2.3±0.5)×10-5, 以颗粒物BET面积计算的初始摄取系数γ0BET为(9.4±1.7)×10-9, 表观活化能为33.5 kJ/mol.

关键词: 甲醛, α-Al2O3, 漫反射傅里叶变换红外光谱(DRIFTS), 非均相反应

Abstract: Formaldehyde is one of the most important carbonyl organic compounds. Heterogeneous reactions of formaldehyde on the surfaceof oxides of crustal elements could be an import sink for formaldehyde in atmosphere. In this study, the kinetics of the heterogeneous reaction of formaldehyde on the surface of α-Al2O3 were in situ investigated by diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) over the temperature range of 273—333 K. The adsorbed species, formate(Ⅰ), dioxymehtylene(Ⅱ), polyoxymethylene(Ⅲ) and formaldyhyde(Ⅳ), on α-Al2O3 particles were identified with infrared spectrum: on the surface of α-Al2O3 particles, formaldyhyde was oxidized at first to dioxymehtylene which was further oxidized to formate. The reaction order was determined as 0.81±0.05, and the initial reactive uptake coefficients at 293 K were calculated with the geometric and the BET specific surface areas are(2.3±0.5)×10-5 and (9.4±1.7)×10-9, respectively. The apparent activation energy of the reaction was etermined as 33.5 kJ/mol.

Key words: Formaldyhyde, α-Al2O3, DRIFT S, Heterogeneous reaction

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