催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (6): 1046-1050.DOI: 10.3724/SP.J.1088.2011.01251

• 研究论文 • 上一篇    下一篇

甲醛在 FeS2(100) 完整与 S-缺陷表面吸附的理论研究

杜玉栋 1, 郭欣 2, 陈文凯1,*, 李奕 1, 章永凡 1   

  1. 1 福州大学化学系, 福建福州 350108; 2 华中科技大学煤燃烧国家重点实验室, 湖北武汉 410074
  • 收稿日期:2010-12-24 修回日期:2011-03-07 出版日期:2011-06-21 发布日期:2014-10-31

Theoretical Study of the Adsorption of Formaldehyde on Perfect and S-Deficient FeS2(100) Surfaces

DU Yudong1, GUO Xin2, CHEN Wenkai1,*, LI Yi1, ZHANG Yongfan1   

  1. 1Department of Chemistry, Fuzhou University, Fuzhou 350108, Fujian, China; 2State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 410074, Hubei, China
  • Received:2010-12-24 Revised:2011-03-07 Online:2011-06-21 Published:2014-10-31

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摘要： 运用密度泛函理论广义梯度近似的 PBE 方法结合周期平板模型, 研究了 HCHO 分子在 FeS2(100) 完整与 S-缺陷表面的吸附. 结果表明, 在两种表面上, HCHO 均通过 O 原子与两个表面作用: 稳定吸附于完整表面 Fe-top 位 (Fe 五配位); 而在 S-缺陷表面则存在两种稳定吸附模式, 即 HCHO 分别与表面的一个和两个四配位 Fe 成键. 对体系的态密度、轨道电荷布居和红外振动频率的分析发现, HCHO 在吸附过程中从 FeS2(100) 表面获得电子,吸附后羰基振动频率发生红移, C=O 键长伸长, 羰基被削弱.

关键词: 密度泛函理论, 二硫化铁(100), 完整晶面, S-缺陷表面, 甲醛分子, 吸附

Abstract: The adsorption of HCHO molecules on perfect and S-deficient FeS2(100) surfaces was studied with a periodic slab model by Perdue-Burke-Ernzerhof approach of General Gradient Approximation within the framework of the density functional theory. The calculated results show that HCHO reacted with both surfaces through the O atom. HCHO adsorbed aslant on the Fe-top site on the perfect surface, while there were two stable structures for HCHO on the S-deficient surface, where HCHO bonded with one and two fourfold-coordinate Fe cations, respectively. The calculation of density of states, Mulliken population, and vibrational frequencies of the adsorption systems indicated that the electrons transferred from the substrate to HCHO, and the bond of C=O was elongated and weakened.

Key words: density functional theory, pyrite(100), perfect surface, S-deficient surface, formaldehyde, adsorption