甲醛在FeS2(100)完整与S-缺陷表面吸附的理论研究

催化学报 , 2011, 32(6): 1046-1050. doi: 10.3724/SP.J.1088.2011.01251

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 ^3, , 李奕 ^4, , 章永凡 ^5,

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

3.福州大学化学系,福建福州350108

4.福州大学化学系,福建福州350108

5.福州大学化学系,福建福州350108

基金项目: 华中科技大学煤燃烧国家重点实验室开放基金(FSKLCC0814) 国家自然科学基金(90922022)

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

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

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.

参考文献

[1]	Sekine Y .[J].Atmospheric Environment,2002,36:5543.
[2]	Salthammer T;Mentese S;Marutzky R .[J].Chemical Reviews,2010,110:2536.
[3]	Yang X Z;Shen Y N;Yuan Z F;Zhn H Y .[J].Journal of Molecular Catalysis A:Chemical,2005,237:224.
[4]	Zhang CB;He H;Tanaka K .Catalytic performance and mechanism of a Pt/TiO2 catalyst for the oxidation of formaldehyde at room temperature[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(1/2):37-43.
[5]	Li J;Dasgupta P K;Luke W .[J].Analytica Chimica Acta,2005,531:51.
[6]	Reuss G;Disteldorf W;Gamer,A O;Hilt A.Ullmann'sEncyclopedia of Industrial Chemistry[M].Weinheim:Wiley-VCH,2001:619.
[7]	Lalvani S B;DeNeve B A;Weston A .[J].Corrosion Science,1991,47:55.
[8]	Ogunsola O M;Osseo-Assare K .[J].Fuel,1987,66:467.
[9]	Olson T J;Aplan F F;Chug Y P;Cauldle R D.Processing and Utilization of High Sulfur Coal[M].Amsterdam:Elsevier Science,1987:71.
[10]	Lowson RT .[J].Chemical Reviews,1982,82:461.
[11]	Nordstrom D K .[J].SSSA Special Publication,1982,10:37.
[12]	Huang X;Evangelou V P;Alpers C N;Blowes D W.Environmental Geochemistry of Sulfide Oxidation[M].New York:Oxford Univeristy Press,1994:562.
[13]	Mattila S.;Leiro JA.;Laajalehto K. .Surface XPS core-level shifts of FeS2[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,2003(0):97-100.
[14]	Leiro J A;Mattila S S;Laajalehto K .[J].Surface Science,2003,547:157.
[15]	Mattila S;Leiro JA;Heinonen M .XPS study of the oxidized pyrite surface[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2004(2):1097-1101.
[16]	Kim E J;Batchelor B .[J].Environmental Science and Technology,2009,43:2899.
[17]	Rosso K M;Becker U;Hochella M F Jr .[J].American Mineralogist,1999,84:1549.
[18]	Rosso K M;Becker U;Hochella M F Jr .[J].American Mineralogist,1999,84:1535.
[19]	Guevremont JM.;Schoonen MAA.;Strongin DR. .EFFECTS OF SURFACE IMPERFECTIONS ON THE BINDING OF CH3OH AND H2O ON FES2(100) - USING ADSORBED XE AS A PROBE OF MINERAL SURFACE STRUCTURE[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,1997(1/3):109-124.
[20]	Guevremont JM.;Schoonen MAA.;Strongin DR. .Photoemission of adsorbed xenon, X-ray photoelectron spectroscopy, and temperature-programmed desorption studies of H2O on FeS2(100)[J].Langmuir: The ACS Journal of Surfaces and Colloids,1998(6):1361-1366.
[21]	Guevremont J M;Strongin D R;Schoonen M A A .[J].American Mineralogist,1998,83:1246.
[22]	Stirling A;Bernasconi M;Parrinello M .[J].Journal of Chemical Physics,2003,118:8917.
[23]	Stirling A;Bernasconi M;Parrinello M .[J].Journal of Chemical Physics,2003,119:4934.
[24]	Boehme C;Marx D .[J].Journal of the American Chemical Society,2003,125:13362.
[25]	孙伟;胡岳华;邱冠周;覃文庆 .[J].中南大学学报（自然科学版）,2004,11:386.
[26]	Von Oertzen G U;Skinner W M;Nesbitt H W .[J].Physical Review B,2005,72:235427.
[27]	Nair NN;Schreiner E;Marx D .Glycine at the pyrite-water interface: The role of surface defects[J].Journal of the American Chemical Society,2006(42):13815-13826.
[28]	Stirling A;Bernasconi M;Parrinello M .[J].Physical Review B,2007,75:165406.
[29]	黎全;覃文庆;孙伟;邱冠周 .[J].中南大学学报（自然科学版）,2007,14:618.
[30]	Kleppe A K;Jephcoat A P .[J].Miner Magazine,2004,68:433.
[31]	Du Y D;Chen W K;Zhang Y F;Guo X .[J].Journal of Natural Gas Chemistry,2011,20:60.
[32]	Delley B .[J].Journal of Chemical Physics,1990,92:508.
[33]	Delley B .[J].Journal of Chemical Physics,2000,113:7756.
[34]	Lide D R.CRC Handbook of Chemistry and Physics[M].Boca Raton,Florida,2004
[35]	Alonso-Azcarate J;Rodas M;Fernandez-Diaz;Bottrell S H Mas J R Lopez-Andres S .[J].Geolog J,2001,36:159.
[36]	蒋仕宇,滕波涛,鲁继青,刘雪松,杨培芳,杨飞勇,罗孟飞.甲醛在CeO2（111）表面吸附的密度泛函理论研究[J].物理化学学报,2008(11):2025-2031.
[37]	Nakanaga T;Kondo S;Saeki S .[J].Journal of Chemical Physics,1982,76:3860.

上一张下一张

计量

下载量()
访问量()

作者相关

文章评分

您的评分：
1

0%
2

0%
3

0%
4

0%
5

0%

材料期刊网

甲醛在FeS2(100)完整与S-缺陷表面吸附的理论研究

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

参考文献