活性炭纤维催化氧化NO的量子化学研究

闫志强; 王雷; 杨辉; 王泽安; 刘豪; 曾汉才; 邱建荣

活性炭纤维催化氧化NO的量子化学研究

1.
华中科技大学煤燃烧国家重点实验室, 湖北武汉 430074;
2.
专利局专利审查协作江苏中心材料部, 江苏苏州 215163

基金项目: 国家自然科学基金(51276074, 50976041)。

详细信息

通讯作者:
刘豪, 副教授, E-mail: liuhao@hust.edu.cn。

中图分类号: X511
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- 被引次数: 0
出版历程
- 收稿日期: 2014-04-29
- 修回日期: 2014-09-18
- 刊出日期: 2014-12-30

A quantum study on the mechanism of NO oxidation over the activated carbon fiber catalysts

1.
State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China;
2.
Patent Examination Cooperation Jiangsu Center of the Patent Office, Suzhou 215163, China

摘要

摘要: 利用密度泛函理论的B3LYP方法,6-31G(d)基组,在zigzag型的四并苯模型上对NO、O₂分子在活性炭纤维(ACFs)表面的吸附行为进行研究,并探讨了ACFs催化氧化NO的主要机理路径。研究结果表明,环境气氛中的O₂分子可以先吸附于ACFs表面形成两个半醌基(C-O),之后C-O和吸附态的NO(C-NO)发生氧化反应生成-NO₂;游离态的O₂也可以经过ACFs表面的催化作用形成活性氧原子(O^*)从而直接和吸附态的NO反应生成-NO₂。与NO相比,O₂分子的吸附能大,在同NO的竞争吸附中占据优势,结合统计热力学分析,吸附态的NO和游离态的O₂所产生的活性氧原子发生氧化反应是NO转化为NO₂的主要途径。
- NO /
- 活性炭纤维 /
- 催化氧化 /
- 量子化学
Abstract: The adsorption of NO, O₂ molecules on the surface of activated carbon fibers (ACFs) were comprehensively investigated using a simplified zigzag model based on density functional theory. The ACFs model, products, stable intermediates were optimized at B3LYP/6-31G(d) level and the catalytic oxidation mechanism of NO over ACFs surface was proposed. The results revealed that O₂ molecules are adsorbed on the ACFs surface, forming two simiquinones (C-O), and then the adsorbed NO(C-NO) is oxidized to -NO₂ by the simiquinones. On the other hand, the active oxygen atom (O^*), derived from free O₂ through catalytic process on the carbon surface, reacts with the adsorbed NO, forming -NO₂. However, O₂ adsorption is more thermodynamically favorable than NO. Based on statistical thermodynamic analysis, the transformation of NO to NO₂ was mainly attributed to the reaction between C-NO and O^* generated from the free O₂ in atmosphere.
- NO /
- ACFs /
- catalytic oxidation /
- quantum chemistry

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参考文献(17)

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