Regulating Titanium Species on TS-1 Zeolites by Na+ for Liquid-Phase Epoxidation of Propylene and H2O2

IF 3.8 3区 工程技术 Q2 ENGINEERING, CHEMICAL Industrial & Engineering Chemistry Research Pub Date : 2024-12-08 DOI:10.1021/acs.iecr.4c0204710.1021/acs.iecr.4c02047
Yue Li, Yanhui Yi*, Bize Gao, Tian Mi, Rujing Pei, Yitong Guo, Jing Liu, Dan Xu, Guoxing Wu, Zhaochi Feng and Hongchen Guo*, 
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Abstract

This paper focuses on the hydrothermal modification of as-synthesized TS-1 zeolites with Na+ ion-containing TPAOH solutions. The effects of NaNO3 dosage, TPAOH concentration, and modification time are investigated in detail. Multiple techniques including XRD, XRF, transmission electron microscopy, Ar physisorption, FT-IR (skeletal vibration and hydroxyl stretching), UV–vis, and UV–Raman (excited by 257 and 266 nm laser lines, respectively) are employed to characterize the parent zeolites and their modified catalyst samples, with emphasis on revealing the changes of both the microenvironment and coordination state of titanium species in the modified zeolites. Besides, propylene and H2O2 liquid-phase epoxidation is used as a probe reaction to evaluate the catalytic performance of the modified catalysts, which is carried out in both the batch reactor and fixed-bed reactor. Results show that the hydrothermal modification of the TS-1 zeolite with a Na+ ion-containing TPAOH solution is a very useful method to simultaneously regulate the microenvironment and coordination state of titanium species as well as the diffusivity of the micropore in the TS-1 zeolite and, therefore, to remarkably improve its selectivity and catalytic activity.

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本文重点研究了用含 Na+ 离子的 TPAOH 溶液对合成的 TS-1 沸石进行水热改性的过程。详细研究了 NaNO3 用量、TPAOH 浓度和改性时间的影响。采用 XRD、XRF、透射电子显微镜、氩气物理吸附、傅立叶变换红外光谱(骨架振动和羟基伸展)、紫外可见光和紫外拉曼光谱(分别由 257 和 266 纳米激光线激发)等多种技术对母体沸石及其改性催化剂样品进行了表征,重点揭示了改性沸石中钛物种的微环境和配位状态的变化。此外,以丙烯和 H2O2 液相环氧化反应为探针反应,在间歇反应器和固定床反应器中评价改性催化剂的催化性能。结果表明,用含 Na+ 离子的 TPAOH 溶液对 TS-1 沸石进行水热改性是一种非常有用的方法,可以同时调节钛物种的微环境和配位状态以及 TS-1 沸石微孔的扩散性,从而显著提高其选择性和催化活性。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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