A DFT study of the models of the bronsted acid sites of zeolite catalysts
文献类型：期刊论文
| 作者 | Gu, JD ; Gorb, L; Leszczynski, J
|
| 刊名 | STRUCTURAL CHEMISTRY
 |
| 出版日期 | 1998-10 |
| 卷号 | 9期号:5页码:319-326 |
| 关键词 | zeolites cluster models Bronsted acid site DFT calculation |
| ISSN号 | 1040-0400 |
| DOI | 10.1023/A:1022406808935 |
| 文献子类 | Article |
| 英文摘要 | A systematic study of the different cluster models of the Bronsted site has been carried out in order to predict how the local structure influences the geometric parameters of the SiO(H)Al site and the harmonic frequencies of the characteristics vibrational modes of the bridging surface hydroxyl group. The performance of the B3LYP variant of the density functional theory (DFT) method is examined and compared with both SCF HF and MP2 approximations. In order to find the best molecular model for the Bronsted site, two series of derivatives based on the prototype model cores SiO(H)Al and HAlO4 were considered. In the HAlO4 series, H3SiO(H)Al(OH)(2)OSiH3 and H3SiO(H)Al(OSiH3)(3) were investigated. Among the models in the SiO(H)Al series were H3SiO(H)AlH3, H3SiO(H)Al(OH)(3), H-2(OH)SiO(H)Al(OH)(3), (OH)(3)SiO(H)Al(OH)(3), and (H3SiO)(3)SiO(H)Al(OSiH3)(3). The research reveals that the acidic OH bond length and its stretching frequency are greatly influenced by the H bond formed between the acidic proton and its next-nearest neighbor oxygen on the aluminum atom. The geometry and the frequencies for the larger models predicted at the B3LYP/D95(d,p) level are in good agreement with the experiments, suggesting that the B3LYP/D95(d,p) theory is reliable for a study of the Bronsted site. This study also suggests that the OH terminated models are not suitable as models for the SiO(H)Al site due to the strong dipole moment of the OH group, which strongly affects the acidic H. |
| WOS关键词 | AB-INITIO CALCULATIONS ; FIRST-PRINCIPLES ; HYDROXYL-GROUPS ; METHANOL ; ADSORPTION ; SILICA ; WATER ; ALUMINOSILICATES ; ACTIVATION ; COMPLEXES |
| WOS研究方向 | Chemistry ; Crystallography |
| 语种 | 英语 |
| WOS记录号 | WOS:000077636800002 |
| 出版者 | KLUWER ACADEMIC/PLENUM PUBL |
| 源URL | [http://119.78.100.183/handle/2S10ELR8/274805]  |
| 专题 | 新药研究国家重点实验室 中科院受体结构与功能重点实验室 |
| 通讯作者 | Leszczynski, J |
| 作者单位 | 1.Jackson State Univ, Dept Chem, Jackson, MS 39217 USA 2.Acad Sinica, Shanghai Inst Mat Med, State Key Lab Drug Res, Shanghai 200031, Peoples R China 3.Natl Acad Sci Ukraine, Inst Water & Colloid Chem, Kiev, Ukraine |
| 推荐引用方式 GB/T 7714 | Gu, JD,Gorb, L,Leszczynski, J. A DFT study of the models of the bronsted acid sites of zeolite catalysts[J]. STRUCTURAL CHEMISTRY,1998,9(5):319-326. |
| APA | Gu, JD,Gorb, L,&Leszczynski, J.(1998).A DFT study of the models of the bronsted acid sites of zeolite catalysts.STRUCTURAL CHEMISTRY,9(5),319-326. |
| MLA | Gu, JD,et al."A DFT study of the models of the bronsted acid sites of zeolite catalysts".STRUCTURAL CHEMISTRY 9.5(1998):319-326. |
入库方式： OAI收割
来源：上海药物研究所
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