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密度泛函理论研究Al在丝光沸石骨架中的取代位置和NH3的吸附

郭海燕 ,  任君 ,  冯刚 ,  李昌盛 ,  彭兴 ,  曹端林

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引用本文: 郭海燕, 任君, 冯刚, 李昌盛, 彭兴, 曹端林. 密度泛函理论研究Al在丝光沸石骨架中的取代位置和NH3的吸附[J]. 燃料化学学报, 2014, 42(5): 582-590. shu
Citation:  GUO Hai-yan, REN Jun, FENG Gang, LI Chang-sheng, PENG Xing, CAO Duan-lin. Distribution of Al and adsorption of NH3 in mordenite:A computational study[J]. Journal of Fuel Chemistry and Technology, 2014, 42(5): 582-590. shu

密度泛函理论研究Al在丝光沸石骨架中的取代位置和NH3的吸附

    通讯作者: REN Jun, E-mail: junren2003@sxicc.ac.cn, Tel: +86-351-3922117; FENG Gang E-mail: fengg.sshy@sinopec.com, Tel: +86-21-68462197.; REN Jun, E-mail: junren2003@sxicc.ac.cn, Tel: +86-351-3922117; FENG Gang E-mail: fengg.sshy@sinopec.com, Tel: +86-21-68462197.
  • 基金项目:

    Supported by the National Science Foundation of China (21371159) (21371159)

    the Natural Science Foundation of Shanxi Province (2009011014) (2009011014)

    Shenzhen Strategic Emerging Industries Special Fund Program of China (GGJS20120619101655715). (GGJS20120619101655715)

摘要: 采用色散校正密度泛函方法(DFT-D2)计算了Al同晶取代进入H-[Al]MOR丝光沸石骨架中可能的位置及其对NH3分子吸附表征Brönsted酸性。热力学上,Al优先取代位是T2O5位,接着是T4O2、T1O7和T3O1位,能量差仅在0.03~0.07 eV,表明Al可能分布在四种非等价晶体T位。同时,电荷平衡质子的位置影响Al取代位的稳定性,数据表明电荷平衡质子与O5位结合的可能性最大。另外,用DFT和 DFT-D2方法计算了NH3分子在每一个Al取代的T位的吸附能,通过比较,DFT低估了NH3吸附能0.41 eV,表明色散校正DFT-D2方法对于NH3吸附是很有必要的,T2O5位的Brönsted酸性最强。

English

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  • 收稿日期:  2013-10-31
  • 网络出版日期:  2014-01-07
通讯作者: 陈斌, bchen63@163.com
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