Insight into the formation of the tert-butyl cation confined inside H-ZSM-5 zeolite from NMR spectroscopy and DFT calculations
Insight into the formation of the tert-butyl cation confined inside H-ZSM-5 zeolite from NMR spectroscopy and DFT calculations
复制标题
通过 NMR 光谱和 DFT 计算深入了解限制在 H-ZSM-5 沸石内部的叔丁基阳离子的形成
DOI：
10.1039/c6cc04943e
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发表时间：
2016
影响因子：
4.9
通讯作者：
Deng Feng
中科院分区：
文献类型：
--
作者：
Huang Mengdi;Wang Qiang;Yi Xianfeng;Chu Yueying;Dai Weili;Li L;ong;Zheng Anmin;Deng Feng
用固体核磁共振实验和密度泛函理论计算确定了~(13)C标记叔丁醇与NH_3在酸性H-ZSM-5沸石上的络合结构。结果表明，除叔丁醇/NH4+络合物被物理吸附在Brnsted酸中心外，还生成了叔丁胺阳离子，证实了叔丁基阳离子的存在局限于沸石孔道中。此外，采用13C-27Al双共振固体核磁共振谱研究了碳正离子与沸石骨架之间的主客体相互作用。
Solid-state NMR experiments and DFT calculations have been carried out to determine the complex structures of coadsorbed 13C-labeled tert-butanol and NH3 in acidic H-ZSM-5 zeolite. It is found, besides the physically adsorbed tert-butanol/NH4+ complex on Brønsted acid sites, the tert-butylamine cation is formed as well, confirming the presence of the tert-butyl cation confined in zeolite channels. Furthermore, 13C–27Al double-resonance solid-state NMR spectroscopy is adopted to determine the host/guest interaction between the carbocation and the zeolite framework.