Application of Mixed Acid-Modified Hollow TS-1 Zeolite to Vapor-Phase Beckman Rearrangement Reaction

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-08-06 DOI:10.1007/s10562-024-04780-1

Pengyu Yin, Jiayuan Nie, Xiangyu Wen, Zhihui Li, Dongsheng Zhang, Xinqiang Zhao, Yanji Wang

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Abstract

ε-Caprolactam (CPL) is an important organic chemical raw material used as a monomer in the production of nylon 6. The traditional production process employs fuming sulfuric acid as a catalyst, leading to serious equipment corrosion and environmental pollution. While vapor-phase Beckman rearrangement reaction offers a solution to these issues. Unfortunately, the catalyst used is susceptible to carbon deposition and deactivation during the vapor-phase Beckman rearrangement process. Herein, a kind of mixed acid-modified hollow TS-1 zeolite was prepared in this study. It is a hollow structure of TS-1 zeolite formed by secondary crystallization, which is conducive to the shortening of the reaction path and the improvement of the anti-carbon accumulation performance. Further investigation revealed that modification of the hollow TS-1 zeolite with mixed acids facilitates the removal of non-skeletal titanium, and reduces the amount of Lewis acid in the catalyst, thereby improving its catalytic performance. Under optimal conditions, the cyclohexanone oxime (CHO) conversion rate reached 100%, with a caprolactam selectivity exceeding 98%. Notably, the catalytic activity of the catalyst remained stable after 500 h of continuous operation.

Graphical Abstract

Abstract Image

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混合酸改性中空 TS-1 沸石在气相贝克曼重排反应中的应用

ε-己内酰胺（CPL）是一种重要的有机化工原料，用于生产尼龙 6 的单体。传统的生产工艺使用发烟硫酸作为催化剂，导致严重的设备腐蚀和环境污染。而气相贝克曼重排反应可以解决这些问题。遗憾的是，所使用的催化剂在气相贝克曼重排过程中容易发生碳沉积和失活。因此，本研究制备了一种混合酸改性的空心 TS-1 沸石。它是由二次结晶形成的 TS-1 沸石空心结构，有利于缩短反应路径，提高抗积碳性能。进一步研究发现，用混合酸对中空 TS-1 沸石进行改性，有利于去除非骨架钛，减少催化剂中路易斯酸的含量，从而提高催化性能。在最佳条件下，环己酮肟（CHO）的转化率达到 100%，己内酰胺的选择性超过 98%。值得注意的是，催化剂的催化活性在连续运行 500 小时后仍然保持稳定。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.