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An Active Alkali-Exchanged Faujasite Catalyst for p-Xylene Production via the One-Pot Diels-Alder Cycloaddition/Dehydration Reaction of 2,5-Dimethylfuran with Ethylene.
ACS Catalysis ( IF 12.9 ) Pub Date : 2017-12-07 , DOI: 10.1021/acscatal.7b03343
Roderigh Y Rohling 1 , Evgeny Uslamin 1 , Bart Zijlstra 1 , Ionut C Tranca 1 , Ivo A W Filot 1 , Emiel J M Hensen 1 , Evgeny A Pidko 1, 2
Affiliation  

The one-pot Diels-Alder cycloaddition (DAC)/dehydration (D) tandem reaction between 2,5-dimethylfuran and ethylene is a potent pathway toward biomass-derived p-xylene. In this work, we present a cheap and active low-silica potassium-exchanged faujasite (KY, Si/Al = 2.6) catalyst. Catalyst optimization was guided by a computational study of the DAC/D reaction mechanism over different alkali-exchanged faujasites using periodic density functional theory calculations complemented by microkinetic modeling. Two types of faujasite models were compared, i.e., a high-silica alkali-exchanged faujasite model representing isolated active cation sites and a low-silica alkali-exchanged faujasite in which the reaction involves several cations in the proximity. The mechanistic study points to a significant synergetic cooperative effect of the ensemble of cations in the faujasite supercage on the DAC/D reaction. Alignment of the reactants by their interactions with the cationic sites and stabilization of reaction intermediates contribute to the high catalytic performance. Experiments confirmed the prediction that KY is the most active catalyst among low-silica alkali-exchanged faujasites. This work is an example of how the catalytic reactivity of zeolites depends on multiple interactions between the zeolite and reagents.

中文翻译:

通过2,5-二甲基呋喃与乙烯的一锅Diels-Alder环加成/脱水反应生产对二甲苯的活性碱交换八面沸石催化剂。

2,5-二甲基呋喃和乙烯之间的一锅Diels-Alder环加成(DAC)/脱水(D)串联反应是生物质衍生的对二甲苯的有效途径。在这项工作中,我们提出了一种廉价,活性低硅钾交换八面沸石(KY,Si / Al = 2.6)催化剂。通过周期性密度泛函理论计算和微动力学模型的补充,对不同碱交换八面沸石上的DAC / D反应机理进行了计算研究,从而指导了催化剂的优化。比较了两种类型的八面沸石模型,即代表孤立的活性阳离子位点的高二氧化硅碱交换的八面沸石模型和其中反应涉及附近几个阳离子的低二氧化硅碱交换的八面沸石。机理研究表明,八面沸石超笼中阳离子的集合对DAC / D反应具有显着的协同作用。反应物通过其与阳离子位点的相互作用而排列和反应中间体的稳定化有助于高催化性能。实验证实了这一预测,即KY是低硅碱交换的八面沸石中活性最高的催化剂。这项工作是一个例子,说明了沸石的催化反应性如何取决于沸石和试剂之间的多重相互作用。实验证实了这一预测,即KY是低硅碱交换的八面沸石中活性最高的催化剂。这项工作是一个例子,说明了沸石的催化反应性如何取决于沸石和试剂之间的多重相互作用。实验证实了这一预测,即KY是低硅碱交换的八面沸石中活性最高的催化剂。这项工作是一个例子,说明了沸石的催化反应性如何取决于沸石和试剂之间的多重相互作用。
更新日期:2017-12-27
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