Unveiling the enzyme-like acidic microenvironment in FER zeolite for N-alkylation of aniline with benzyl alcohol

IF 5.4 2区化学 Q2 CHEMISTRY, PHYSICAL

Colloids and Surfaces A: Physicochemical and Engineering Aspects Pub Date : 2025-07-23 DOI:10.1016/j.colsurfa.2025.137847

Xinghao Shi, Lei Chen, Biao Meng, Xiaoling Liu, Jiao Wei, Meng Xu, Xinyu Zhu, Yang Yang, Yu Zhou, Jun Wang

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引用次数: 0

Abstract

The ordered microchannels of zeolites provide a feasible opportunity to modulate the adsorption and diffusion of guest molecules depending on the matching of the molecular structure and porous characteristics, encouraging the exploration of enzyme-like specificity of zeolites in heterogeneous catalysis. In this work, we investigated the activity of FER, MFI, MOR, and BEA zeolites in the amination of aniline with benzyl alcohol. The influence of acid properties, morphology, and topology-related adsorption behavior was specially studied to uncover how the micro-environment determined the activities from the molecular level through Rietveld refinement. FER zeolites were found extremely active in the amination to give the 99 % conversion of aniline and 98.7 % yield of secondary amines. The T1 site in the cross-section of the 10-membered-ring (MR) channel and FER cavity was found as the active site. Aniline and benzyl alcohol adsorption on the T1 site was respectively preferred in the FER cavity and 10-MR channel, increasing the collision probability and thus enhancing the activity. This unique molecular recognition behavior in the confined space of zeolite is responsive to the remarkable and stable amination activity.

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揭示了FER沸石中苯胺与苯甲醇n -烷基化的酶样酸性微环境

沸石有序的微通道为调节客体分子的吸附和扩散提供了一个可行的机会，这取决于分子结构和多孔特性的匹配，鼓励探索沸石在非均相催化中的类酶特异性。在这项工作中，我们研究了FER、MFI、MOR和BEA沸石在苯胺与苯甲醇胺化反应中的活性。特别研究了酸性质、形态和拓扑相关吸附行为的影响，以揭示微环境如何通过Rietveld细化从分子水平决定活性。fe分子筛在胺化反应中非常活跃，苯胺的转化率为99% %，仲胺的收率为98.7 %。在10元环（MR）通道和FER腔的横截面上发现T1位点为活性位点。在FER腔和10-MR通道中，苯胺和苯甲醇分别优先吸附在T1位点，增加了碰撞概率，从而提高了活性。这种独特的分子识别行为在沸石的有限空间是响应显著和稳定的胺化活性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Colloids and Surfaces A: Physicochemical and Engineering Aspects 化学-物理化学

CiteScore

8.70

自引率

9.60%

发文量

2421

审稿时长

56 days

期刊介绍： Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.