Mechanistic Insight into Ethanol Dehydration over SAPO-34 Zeolite by Solid-state NMR Spectroscopy

Mechanistic Insight into Ethanol Dehydration over SAPO-34 Zeolite by Solid-state NMR Spectroscopy
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通过固态核磁共振波谱分析 SAPO-34 沸石上的乙醇脱水机理

DOI:
10.1007/s40242-022-1450-1
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发表时间:
2022-01
影响因子:
3.1
通讯作者:
Feng Deng
Feng Deng
中科院分区:
化学3区
文献类型:
--
作者:
Xue Zhou;Chao Wang;Yueying Chu;Qiang Wang;Jun Xu;Feng Deng

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用固体核磁共振技术研究了乙醇在SAPO-34分子筛上脱水的反应机理。制备了不同硅含量的SAPO-34分子筛,用核磁共振方法表征了其酸性。更高含量的强布朗斯特酸中心与更高的Si含量相关。乙醇在SAPO-34中的布朗斯特酸中心上的吸附导致阻挫刘易斯对(FLP)的形成。在室温下,通过FLP位点的脱水观察到表面乙氧基物种,其可以进一步转化为乙烯产物。在较高的反应温度下,乙醚在布朗斯台德酸中心上的分解是形成乙氧基物种的原因。在反应中形成三乙基氧鎓离子。提出了一个合理的反应机理为乙醇在SAPO-34上脱水。
The reaction mechanism of ethanol dehydration over SAPO-34 zeolite is investigated by using solid-state NMR spectroscopy. SAPO-34 zeolites with different Si contents are prepared and their acidities are characterized by NMR experiments. The higher content of stronger Brønsted acid sites is correlated to the higher Si content. The adsorption of ethanol on the Brønsted acid sites in SAPO-34 leads to the formation of frustrated Lewis pairs(FLPs). Surface ethoxy species is observed by the dehydration of the FLP sites at room temperature, which can be further converted into ethene products. The decomposing of diethyl ether over Brønsted acid sites is responsible for the formation of ethoxy species at higher reaction temperatures. Triethyloxonium ions are formed in the reaction. A plausible reaction mechanism is proposed for the dehydration of ethanol over SAPO-34.
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