C-13 Chemical Shift of Adsorbed Acetone for Measuring the Acid Strength of Solid Acids: A Theoretical Calculation Study
文献类型：期刊论文
| 作者 | Fang, Hanjun1,2; Zheng, Anmin1; Chu, Yueying1,2; Deng, Feng1 |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY C
 |
| 出版日期 | 2010-07-29 |
| 卷号 | 114期号:29页码:12711-12718 |
| 产权排序 | 第一 |
| 英文摘要 | Adsorption of basic probe molecules is one of the widely used methods to characterize the acid strength of solid acids. In this contribution, the adsorptions of acetone on various Bronsted and Lewis acid sites (from weak acid to superacid) are theoretically studied, in order to elucidate the quantitative relationships between C-13 chemical shifts of acetone and intrinsic acid strength of solid acids. The Bronsted acid sites are represented by a series of 8T zeolite models with varying terminal Si-H bond lengths, and the different extents of acidic proton transfer from these acid sites to acetone are revealed explicitly. We found that three adsorption conformations (hydrogen-bonded, proton-shared, and ion-pair) exist for acetone, and concurrently, a correlation of three-broken lines is obtained for the C-13 chemical shift of acetone versus the deprotonation energy (DPE). The correlation can be used as a scale for quantitatively measuring the Bronsted acid strength of solid acids. A threshold of 245 ppm is determined for superacidity, in good agreement with the experimental value (244 ppm). The Lewis acid sites are modeled by tricoordinate framework aluminum species and various extra-framework aluminum cations or neutral species such as Al3+, AlO+, AlOH2+, Al(OH)(2)(+), Al(OH)(3), and AlOOH. We found that acetone is coordinately adsorbed on the aluminum atoms of Lewis acid sites and that the C-13 chemical shift of acetone is almost linear to the lowest unoccupied molecular orbital (LUMO) energy of the acid sites. |
| WOS标题词 | Science & Technology ; Physical Sciences ; Technology |
| 学科主题 | 波谱分析 |
| 类目[WOS] | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| 研究领域[WOS] | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| 关键词[WOS] | STATE NMR-SPECTROSCOPY ; DENSITY-FUNCTIONAL THEORY ; IN-SITU NMR ; TRIMETHYLPHOSPHINE OXIDE ; BRONSTED ACIDITY ; LEWIS ACIDITY ; ALUMINUM-CHLORIDE ; CARBONYL GROUP ; ZEOLITE ZSM-5 ; CATALYSTS |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000280070900046 |
| 源URL | [http://ir.wipm.ac.cn/handle/112942/2017]  |
| 专题 | 武汉物理与数学研究所_2011年以前论文发表（包括2011年） |
| 作者单位 | 1.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China 2.Chinese Acad Sci, Grad Sch, Beijing 100049, Peoples R China |
| 推荐引用方式 GB/T 7714 | Fang, Hanjun,Zheng, Anmin,Chu, Yueying,et al. C-13 Chemical Shift of Adsorbed Acetone for Measuring the Acid Strength of Solid Acids: A Theoretical Calculation Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2010,114(29):12711-12718. |
| APA | Fang, Hanjun,Zheng, Anmin,Chu, Yueying,&Deng, Feng.(2010).C-13 Chemical Shift of Adsorbed Acetone for Measuring the Acid Strength of Solid Acids: A Theoretical Calculation Study.JOURNAL OF PHYSICAL CHEMISTRY C,114(29),12711-12718. |
| MLA | Fang, Hanjun,et al."C-13 Chemical Shift of Adsorbed Acetone for Measuring the Acid Strength of Solid Acids: A Theoretical Calculation Study".JOURNAL OF PHYSICAL CHEMISTRY C 114.29(2010):12711-12718. |
入库方式： OAI收割
来源：武汉物理与数学研究所
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