采用量子化学中的密度泛函理论结合平板周期模型方法,研究了苯在Ag(100)面上的吸附方式和相对稳定性. 通过对不同吸附位置的吸附能和几何构型参数的比较发现,苯在Ag(100)表面的吸附属于较强的化学作用,穴位吸附的稳定性优于桥位,顶位吸附最不稳定. 吸附的苯分子的平衡构型发生扭曲, C - C键有较大程度的伸长;C - H键的键长基本不变,但是偏离苯环平面,并背离Ag(100)表面. 在吸附过程中,电子由苯向表面银原子转移. 本文给出了详细的轨道示意图和电荷布居分析,并且与相关的实验和理论研究结果进行了比较.
参考文献
| [1] | 陈诵英;孙予罕;丁云杰;周仁贤,罗孟飞.吸附与催化[M].郑州:河南科学技术出版社,2001:102. |
| [2] | Wan L J;Wang C;Bai C L;Osawa M .[J].Journal of Physical Chemistry B,2001,105(35):8399. |
| [3] | Yannoulis P;Dudde R;Frank K H;Koch E E .[J].Surface Science Spectra,1987,189/190(01):519. |
| [4] | Lomas J R;Baddeley C J;Tikhov M S;Lambert R M .[J].Chemical Physics Letters,1996,263(3-4):591. |
| [5] | Nilsson A;Weinelt M;Wiell T;Bennich P;Karis O;Wassdahl N;Stohr J;Samant MG .An atom-specific look at the surface chemical bond[J].Physical review letters,1997(14):2847-2850. |
| [6] | Pascual J I;Jackiw J J;Song I;Weiss P S,Conrad H,Rust H P .[J].Surface Science Spectra,2002,502-503:1. |
| [7] | Koretsky GM.;Knickelbein MB. .INFRARED PHOTODISSOCIATION SPECTROSCOPY OF AG-N(C6H6)(M) AND AG-N(C6D6)(M) CLUSTERS - EVIDENCE OF ADSORPTION-INDUCED SYMMETRY REDUCTION IN BENZENE[J].Chemical Physics Letters,1997(5-6):485-490. |
| [8] | 李艳茶,王文宁,曹勇,范康年.苯在Si（111）-7×7表面化学吸附的理论研究[J].化学学报,2002(04):653-659. |
| [9] | Lu X.;Wang XL.;Yuan QH.;Zhang Q. .Diradical mechanisms for the cycloaddition reactions of 1,3-butadiene, benzene, thiophene, ethylene, and acetylene on a Si(111)-7x7 surface[J].Journal of the American Chemical Society,2003(26):7923-7929. |
| [10] | Lu X;Lin M C;Xu X;Wang N Q,Zhang Q E .[J].Phys Chem Commun,2001,4(13):60. |
| [11] | 周公度;段连运.结构化学基础[M].北京:北京大学出版社,2002:242. |
| [12] | Gland J L;Somorjai G A .[J].Surface Science Spectra,1973,38(01):157. |
| [13] | Wan LJ.;Itaya K. .IN SITU SCANNING TUNNELLING MICROSCOPY OF BENZENE, NAPHTHALENE, AND ANTHRACENE ADSORBED ON CU(111) IN SOLUTION[J].Langmuir: The ACS Journal of Surfaces and Colloids,1997(26):7173-7179. |
| [14] | Morin C;Simon D;Sautet P .[J].Journal of Physical Chemistry B,2004,108(18):5653. |
| [15] | Morin C;Simon D;Sautet P .[J].Journal of Physical Chemistry B,2004,108(32):12084. |
| [16] | Saeys M;Reyniers M F;Marin G B .[J].Journal of Physical Chemistry B,2002,106(30):7489. |
| [17] | Mittendorfer F;Hafner J .[J].Surface Science Spectra,2001,472(1-2):133. |
| [18] | 曹梅娟,陈文凯,刘书红,许莹,李俊汉.苯在Au（100）表面化学吸附的周期性密度泛函理论研究[J].物理化学学报,2006(01):11-15. |
| [19] | Chen WK;Cao MJ;Liu SH;Lu CH;Xu Y;Li JQ .A first-principles study of the chemi-adsorption of benzene on Au(100) surface[J].Chemical Physics Letters,2006(4-6):414-418. |
| [20] | 陈文凯,曹梅娟,刘书红,许莹,李奕,李俊篯.苯分子在Cu（100）面平板模型上吸附的密度泛函理论研究[J].物理化学学报,2005(08):903-908. |
| [21] | Chen WK;Cao MJ;Liu SH;Xu Y;Li JQ .On the coverage-dependent orientation of benzene adsorbed on Cu(100): A density functional theory study[J].Chemical Physics Letters,2005(4-6):414-418. |
| [22] | Delley B .[J].Journal of Chemical Physics,1990,92(01):508. |
| [23] | Delley B .[J].Journal of Chemical Physics,2000,113(18):7756. |
| [24] | Vosko S H;Wilk L;Nusair M .[J].Canadian Journal of physics,1980,58(08):1200. |
| [25] | Yamagishi S;Jenkins S J;King D A .[J].Journal of Chemical Physics,2001,114(13):5765. |
| [26] | Saeys M;Reyniers M F;Neurock M;Marin G B .[J].Journal of Physical Chemistry B,2003,107(16):3844. |
| [27] | Soon A;Sohnel T;Idriss H .[J].Surface Science Spectra,2005,579(2-3):131. |
| [28] | Yin X;Han H;Kubo M;Miyamoto A .[J].Theoretical Chemistry Accounts,2003,109(04):190. |
| [29] | Lide D R.CRC Handbook of Chemistry and Physics[M].Florida:CRC Press,2000:27. |
| [30] | Lorente N;Hedouin M F G;Palmer R E;Persson M .[J].Physical Review B,2003,68(01):155401. |
| [31] | 辛勤,梁长海.固体催化剂的研究方法第八章 红外光谱法（上）[J].石油化工,2001(01):72-85. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%