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Ce改性对Y型分子筛酸性及其催化转化性能的调变机制

张畅 秦玉才 高雄厚 张海涛 莫周胜 初春雨 张晓彤 宋丽娟

物理化学学报Issue(2):344-352,9.
物理化学学报Issue(2):344-352,9.DOI:10.3866/PKU.WHXB201412163

Ce改性对Y型分子筛酸性及其催化转化性能的调变机制

Modulation of the Acidity and Catalytic Conversion Properties of Y Zeolites Modified by Cerium Cations

张畅 1秦玉才 1高雄厚 2张海涛 2莫周胜 3初春雨 1张晓彤 1宋丽娟1

作者信息

  • 1. 辽宁石油化工大学,辽宁省石油化工催化科学与技术重点实验室,辽宁抚顺113001
  • 2. 中国石油天然气股份有限公司石油化工研究院兰州化工研究中心,兰州730060
  • 3. 中国石油大学 华东,化学工程学院,山东青岛266555
  • 折叠

摘要

Abstract

Y-type zeolites with different cerium ion content were prepared by liquid phase ion exchange (LPIE) and their structural properties were characterized by inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray diffraction (XRD), N2 adsorption isotherm, and temperature-programmed desorption of ammonia (NH3-TPD). The influence of cerium ion modification of the Y-type zeolites on the acidity and catalytic behavior was studied by in situ Fourier transform infrared spectroscopy (in situ FTIR) techniques with pyridine and thiophene as probe molecules. The results indicate that the original crystal structures of the zeolites remain unchanged after modification with cerium ions. During the modification process the Ce species tend to be located in sodalite (SOD) cages after calcination and remain in the supercages upon a gradual increase in Ce cation content. The amount and strength of the Brönsted (B) acid sites in the zeolites generated by the modification increases initial y and then stabilizes with an increase in Ce ion content. The strong and weak Lewis (L) acid sites related to the non-framework aluminum and the rare earth species increase continuously during the modification process. Thiophene adsorption FTIR spectra indicate that the adsorbed thiophene molecules protonate at the strong Brönsted acid sites of the zeolites. The protonated products then oligomerize. The synergy between Ce species and B acid sites is favorable for the thiophene oligomerization reaction.

关键词

原位傅里叶变换红外光谱/CeY/酸性/噻吩/催化转化

Key words

In situ Fourier transform Infrared spectroscopy/CeY/Acidity/Thiophene/Catalytic conversion

分类

化学化工

引用本文复制引用

张畅,秦玉才,高雄厚,张海涛,莫周胜,初春雨,张晓彤,宋丽娟..Ce改性对Y型分子筛酸性及其催化转化性能的调变机制[J].物理化学学报,2015,(2):344-352,9.

基金项目

The project was supported by the National Natural Science Foundation of China (21076100,21376114) and Major Program of Petroleum Refining of Catalyst of Petro China Company Limited, China (10-01A-01-01-01).国家自然科学基金(21076100,21376114)和中国石油天然气股份有限公司炼油催化剂重大专项(10-01A-01-01-01)资助项目 (21076100,21376114)

物理化学学报

OA北大核心CSCDCSTPCDSCI

1000-6818

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