| 磷在P-ZSM-5沸石中存在的形态 |
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| 引用本文： | 杨静,孙迎新,赵立峰,孙淮. 磷在P-ZSM-5沸石中存在的形态[J]. 物理化学学报, 2011, 27(8): 1823-1830. DOI: 10.3866/PKU.WHXB20110733 |
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| 作者姓名： | 杨静 孙迎新 赵立峰 孙淮 |
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| 作者单位： | School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China |
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| 基金项目： | 国家自然科学基金(21073119); 国家重点基础研究发展计划(973)(2007CB209701); 上海石油化工研究院资助项目~~ |
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| 摘 要： | 用密度泛函理论和ONIOM (our own N-layer integrated molecular orbital molecular mechanics)方法研究磷改性的ZSM-5沸石中含磷基团的可能存在形态. 计算的反应焓和自由能数据表明P-ZSM-5沸石中以磷进入骨架和在骨架外的形成磷酸根离子对是合理的稳定结构. 而且, 计算结果表明离子对模型F和G更适合在室温下存在, 磷进入骨架的酸性结构C'在高温下更稳定, 而磷进入骨架的结构C对温度变化不敏感. 计算得到的27Al, 31P, 29Si化学位移、酸性的变化趋势和结构参数与相关实验数据吻合.
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| 关 键 词： | H-ZSM-5沸石 磷改性 ONIOM方法 密度泛函理论 |
| 收稿时间： | 2011-04-29 |
| 修稿时间： | 2011-06-03 |
Phosphorous Moieties in P-ZSM-5 Zeolites |
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| YANG Jing,SUN Ying-Xin,ZHAO Li-Feng,SUN Huai. Phosphorous Moieties in P-ZSM-5 Zeolites[J]. Acta Physico-Chimica Sinica, 2011, 27(8): 1823-1830. DOI: 10.3866/PKU.WHXB20110733 |
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| Authors: | YANG Jing SUN Ying-Xin ZHAO Li-Feng SUN Huai |
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| Affiliation: | School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China |
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| Abstract: | Phosphorus modified ZSM-5(P-ZSM-5) zeolite was investigated using quantum mechanics density functional theory and our own N-layer integrated molecular orbital molecular mechanics method(ONIOM).Extra-framework phosphate and in-framework moieties containing phosphorus were found to be plausible local structures in P-ZSM-5 zeolites based on the calculated heats of formation and the free energy data from the hypothetical reactions.Furthermore,we find that the cationic moieties are favored at room temperature.Th... |
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| Keywords: | H-ZSM-5 zeolite P-modification ONIOM method Density functional theory |
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