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采用广义梯度近似下的密度泛函理论方法，研究了不同覆盖度下H2S，HS自由基以及S 原子在Fe（111）表面的吸附结构和吸附特性，计算了吸附能、功函数、差分电荷密度、态密度和电荷布居，讨论了覆盖度对表面吸附的影响作用，对比分析了H2S，HS自由基，S在Fe（111）表面的吸附强弱. 研究结果表明：随着覆盖度的增大，吸附物与表面的作用力逐渐减弱；H2S，HS自由基，S三者与Fe（111）表面的作用力大小依次为：H2SxSy腐蚀产物膜，只是随着覆盖度的不同，其致密度将发生变化. 各吸附物在低指数晶面上的吸附结果表明：Fe（111）面吸附作用最强，而Fe（110）和Fe（100）吸附作用相对较弱，二者吸附能相差不大.In this paper, the geometries and properties of H2S and its decomposition fragments adsorbed on Fe(111) surface are studied by means of the density functional theory based on generalized gradient approximation in wide ranges of coverage; the adsorption energy, work function, charge density difference, density of states, and charge population are calculated; the effect of coverage on surface adsorption is discussed; the adsorbability values of H2S, HS radical and S on Fe(111) are compared and analyzed. The results show that the force between absorbates and surface gradually weaken as the coverage increases, the interactions between the above-mentioned particles and Fe(111) are compared with each other: the magnitudes of their interactions are in the order of H2SxSy corrosion product films are easily formed, and the compactnesses of corrosion product films change with coverage variation. A study of the adsorbability values of various adsorbates in low index crystal plane indicates that the interactive force between adsorbates and Fe(111) surface is strongest, and that between the Fe(100) surface and Fe(110) is relatively weak, the difference in adsorption energy between them is not so much.
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Keywords:
- density functional theory /
- Fe(111) surface /
- surface absorptions /
- decomposition fragments of H2S
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[9] Lucio-Garcia M A, Gonzalez-Rodriguez J G, Casales M, Martinez L, Chacon-Nava J G, Neri-Flores M A, Martinez-Villafañe A 2009 Corros. Sci. 51 2380
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[21] Peng S F, Ho J J 2010 J. Phys. Chem. C 114 19489
[22] Broyden C G 1970 J. Inst. Math. Appl. 6 76
[23] Fletcher R 1970 Comput. J. 13 317
[24] Goldfarb D 1970 Math. Comput. 24 23
[25] Shanno D F 1970 Math. Comput. 24 647
[26] Vanderbilt D 1990 Phys. Rev. B 41 7892
[27] Monkhorst H J, Pack J D 1976 Phys. Rev. B 13 5188
[28] Kittel C 1996 Introduction to Solid State Physics (7th Ed.) (New York: John Wiley & Sons)
[29] Chen H L, Wu S Y, Chen H T, Chang J G, Ju S P, Tsai C, Hsu L C 2010 Langmuir 26 7157
[30] Ma C A, Liu T, Chen L T 2010 Acta Phys. Chim. Sin. 26 155 (in Chinese) [马淳安, 刘婷, 陈丽涛 2010 物理化学学报 26 155]
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[32] Liu W, Pu X L, Bai X D, Zhao H W 2008 Petroleum Drilling Techniques 36 83 (in Chinese) [刘伟, 蒲小林, 白晓东, 赵昊伟 2008 石油钻探技术 36 83]
[33] Huang B S, Lu X, Liu Q Y 2011 Corros. Sci. Protect. Technol. 23 205 (in Chinese) [黄本生, 卢曦, 刘清友 2011 腐蚀科学与防腐技术 23 205]
[34] Xu G G, Wu Q Y, Zhang J M, Chen Z G, Huang Z G 2009 Acta Phys. Sin. 58 1924 (in Chinese) [许桂贵, 吴青云, 张健敏, 陈志高, 黄志高 2009 58 1924]
[35] Li W X, Stampfl C, Scheffler M 2002 Phys. Rev. B 65 075407
[36] Wu X X, Wang Q E, Wang F H, Zhou Y S 2010 Acta Phys. Sin. 59 7278 (in Chinese) [吴小霞, 王乾恩, 王福和, 周云松 2010 59 7278]
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[1] Chinese Cankerous and Protection Society, Lu Q M 2001 Corrosion and Protection in oil industry (Beijing: Chemical Industry Press) p4 (in Chinese) [中国腐蚀与防护学会, 卢绮敏 2001 石油工业中的腐蚀与防护 (北京: 化学工业出版社) 第4页]
[2] Kuzyukov A N 2002 Int. J. Hydrogen Energy 27 813
[3] Siddiqui R A 2005 J. Mater. Process. Technol. 170 430
[4] Kashkovskiy R V, Kuznetsov Yu I, Kazansky L P 2012 Corros. Sci. 64 126
[5] Chumalo H V 2012 Mater. Sci. 48 176
[6] Kudryavtsev D B, Panteleeva A R, Yurina A V, Lukashenko S S, Khodyrev Y P, Galiakberov R M, Khaziakhmetov D N, Kudryavtseva L A 2009 Petroleum Chem. 49 193
[7] Qi Y M, Luo H Y, Zheng S Q, Chen C F, Wang D N 2013 Corros. Sci. 69 164
[8] Braun F, Miller J B, Gellman A J, Tarditi A M, Fleutot B, Kondratyuk P, Cornaglia L M 2012 Int. J. Hydrogen Energy 37 18547
[9] Lucio-Garcia M A, Gonzalez-Rodriguez J G, Casales M, Martinez L, Chacon-Nava J G, Neri-Flores M A, Martinez-Villafañe A 2009 Corros. Sci. 51 2380
[10] Taheri H, Kakooei S, Ismail M C, Dolati A 2012 Casp. J. Appl. Sci. Res. 1 41
[11] Jiang D E, Carter E A 2005 Surf. Sci. 583 60
[12] Jiang D E, Carter E A 2004 J. Phys. Chem. B 108 19140
[13] Luo Q, Tang B, Zhang Z, Ran Z L 2013 Acta Phys. Sin. 62 077101 (in Chinese) [罗强, 唐斌, 张智, 冉曾令 2013 62 077101]
[14] Hohenberg P, Kohn W 1964 Phys. Rev. B 136 864
[15] Kohn W, Sham L J 1965 Phys. Rev. A 140 1133
[16] Payne M C, Allan D C, Arias T A, Joannopoulos J D 1992 Rev. Mod. Phys. 64 1045
[17] Milman V, Winkler B, White J A, Pickard C J, Payne M C, Akhmataskaya E V, Nobes R H 2000 Int. J. Quantum Chem. 77 895
[18] White J A, Bird D M 1994 Phys. Rev. B 50 4954
[19] Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
[20] Zhang Y, Yang W 1998 Phys. Rev. B 80 890
[21] Peng S F, Ho J J 2010 J. Phys. Chem. C 114 19489
[22] Broyden C G 1970 J. Inst. Math. Appl. 6 76
[23] Fletcher R 1970 Comput. J. 13 317
[24] Goldfarb D 1970 Math. Comput. 24 23
[25] Shanno D F 1970 Math. Comput. 24 647
[26] Vanderbilt D 1990 Phys. Rev. B 41 7892
[27] Monkhorst H J, Pack J D 1976 Phys. Rev. B 13 5188
[28] Kittel C 1996 Introduction to Solid State Physics (7th Ed.) (New York: John Wiley & Sons)
[29] Chen H L, Wu S Y, Chen H T, Chang J G, Ju S P, Tsai C, Hsu L C 2010 Langmuir 26 7157
[30] Ma C A, Liu T, Chen L T 2010 Acta Phys. Chim. Sin. 26 155 (in Chinese) [马淳安, 刘婷, 陈丽涛 2010 物理化学学报 26 155]
[31] Song J J, Pei J F, Deng X F, Qin Z J, Tang X G 2012 Corros. Protect. 33 649 (in Chinese) [宋佳佳, 裴峻峰, 邓学风, 秦志坚, 汤学耕 2012 腐蚀与防护 33 649]
[32] Liu W, Pu X L, Bai X D, Zhao H W 2008 Petroleum Drilling Techniques 36 83 (in Chinese) [刘伟, 蒲小林, 白晓东, 赵昊伟 2008 石油钻探技术 36 83]
[33] Huang B S, Lu X, Liu Q Y 2011 Corros. Sci. Protect. Technol. 23 205 (in Chinese) [黄本生, 卢曦, 刘清友 2011 腐蚀科学与防腐技术 23 205]
[34] Xu G G, Wu Q Y, Zhang J M, Chen Z G, Huang Z G 2009 Acta Phys. Sin. 58 1924 (in Chinese) [许桂贵, 吴青云, 张健敏, 陈志高, 黄志高 2009 58 1924]
[35] Li W X, Stampfl C, Scheffler M 2002 Phys. Rev. B 65 075407
[36] Wu X X, Wang Q E, Wang F H, Zhou Y S 2010 Acta Phys. Sin. 59 7278 (in Chinese) [吴小霞, 王乾恩, 王福和, 周云松 2010 59 7278]
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