MAO在不同二氧化硅晶面上的吸附研究
|
摘要
通过Material Studio中CASTEP模块对不同二氧化硅晶面进行计算,考察甲基铝氧烷(MAO)在二氧化硅不同晶面产生的吸附行为。结果表明,MAO在不同二氧化硅晶面吸附产生的结构均可得到优化。MAO在SiO2(100)晶面和SiO2(111)晶面产生的吸附趋势基本一致,而与SiO2(110)晶面产生的吸附趋势相差较大。SiO2(110)晶面相对于SiO2(100)晶面和SiO2(111)晶面而言,对MAO产生的吸附机率较小,吸附较为困难。态密度计算发现,MAO吸附在SiO2(110)晶面上形成的PDOS上出现许多尖锐的峰,表明MAO在SiO2(110)表面上具有多重吸附。
The different silica crystal planes were calculated using the CASTEP module in Material Studio to investigate the adsorption behavior of methylaluminoxane(MAO) on different crystal faces of silica. The results showed that the structures of MAO adsorbed on different silica crystal faces could be optimized. The adsorption of MAO on the SiO2(100) and SiO2(111) planes were basically the same,while the adsorption on the Si O2(110)plane was quite different. Compared with the SiO2(100) and SiO2(111) crystal planes,the SiO2(110) crystal surface had a lower adsorption probability for MAO and the adsorption was more difficult. The DOS calculation showed that there were many sharp peaks on the PDOS formed on the SiO2(110) crystal surface by MAO adsorption,indicating that MAO had multiple adsorption on the SiO2(110) surface.
The different silica crystal planes were calculated using the CASTEP module in Material Studio to investigate the adsorption behavior of methylaluminoxane(MAO) on different crystal faces of silica. The results showed that the structures of MAO adsorbed on different silica crystal faces could be optimized. The adsorption of MAO on the SiO2(100) and SiO2(111) planes were basically the same,while the adsorption on the Si O2(110)plane was quite different. Compared with the SiO2(100) and SiO2(111) crystal planes,the SiO2(110) crystal surface had a lower adsorption probability for MAO and the adsorption was more difficult. The DOS calculation showed that there were many sharp peaks on the PDOS formed on the SiO2(110) crystal surface by MAO adsorption,indicating that MAO had multiple adsorption on the SiO2(110) surface.
引文
[1]M. O'Keeffe,B. G. Hyde,Acta Cryst,1976,B32,2923.
[2]R. K. Iler,Cornell University Press,Ithaca,New York 1955.
[3]J. R. Severn,J. R. Severn,J. C. Chadwick,Wiley-VCH Verlag GmbH&Co. KGaA,Weinheim,2008,98,138.
[4] C. Tautermann,D. Clary,Phys. Chem. Chem.Phys,2006,12,1437.
[5]K. M. Neyman,F. Illas,Catal. Today,2005,105,1.
[6] C. Lomenech,G. Bery,D. Costa,L. Stievano,J. F. Lambert,ChemPhysChem,2005,6,1061.
[7]A. Rimola,M. Sodupe,S. Tosoni,B. Civalleri,P.Ugliengo,Langmuir,2006,22,6593.
[8]D. Costa,A. Tougerti,F. Tielens,C. Gervais,L.Stievano,J. F. Lambert,Phys. Chem. Chem.Phys,2008,42,6360.
[9]A. Rimola,M. Sodupe,P. Ugliengo,J. Phys.Chem C,2009,113,5741.
[10] A. Abbasi,E. Nadimi,P. Planitz,C. Radehaus,Surface Science,2009,603,2502.
[11] Alfredo Juan,Daniel Damiani,Carolina Pistonesi,Alejandro García,Macromol. Theory Simul.,2001,10,485.
[12]M. J. Frisch,G. W. Trucks,H. B. Schlegel,P. M. W. Gill,B. G. Johnson,M. W. Wong,J. B. Foresman,M. A. Robb,M. Head-Gordon,E. S. Replogle,R. Gomperts,J. L. Andres,K. Raghavachari,J. S. Binkley,C.Gonzalez,L. Martin,D. J. Fox,D. J. Defrees,J. Baker,J. J. P. Stewart,J. A. Pople,Gaussian 92/DFT,Revision G. 2,Gaussian,Inc.,Pittsburgh,PA 1993.
[13] J. P. Perdew,K. Burke,M. Ernzerhof,Phys.Rev. Lett.,1996,77,3865.
[2]R. K. Iler,Cornell University Press,Ithaca,New York 1955.
[3]J. R. Severn,J. R. Severn,J. C. Chadwick,Wiley-VCH Verlag GmbH&Co. KGaA,Weinheim,2008,98,138.
[4] C. Tautermann,D. Clary,Phys. Chem. Chem.Phys,2006,12,1437.
[5]K. M. Neyman,F. Illas,Catal. Today,2005,105,1.
[6] C. Lomenech,G. Bery,D. Costa,L. Stievano,J. F. Lambert,ChemPhysChem,2005,6,1061.
[7]A. Rimola,M. Sodupe,S. Tosoni,B. Civalleri,P.Ugliengo,Langmuir,2006,22,6593.
[8]D. Costa,A. Tougerti,F. Tielens,C. Gervais,L.Stievano,J. F. Lambert,Phys. Chem. Chem.Phys,2008,42,6360.
[9]A. Rimola,M. Sodupe,P. Ugliengo,J. Phys.Chem C,2009,113,5741.
[10] A. Abbasi,E. Nadimi,P. Planitz,C. Radehaus,Surface Science,2009,603,2502.
[11] Alfredo Juan,Daniel Damiani,Carolina Pistonesi,Alejandro García,Macromol. Theory Simul.,2001,10,485.
[12]M. J. Frisch,G. W. Trucks,H. B. Schlegel,P. M. W. Gill,B. G. Johnson,M. W. Wong,J. B. Foresman,M. A. Robb,M. Head-Gordon,E. S. Replogle,R. Gomperts,J. L. Andres,K. Raghavachari,J. S. Binkley,C.Gonzalez,L. Martin,D. J. Fox,D. J. Defrees,J. Baker,J. J. P. Stewart,J. A. Pople,Gaussian 92/DFT,Revision G. 2,Gaussian,Inc.,Pittsburgh,PA 1993.
[13] J. P. Perdew,K. Burke,M. Ernzerhof,Phys.Rev. Lett.,1996,77,3865.