Transient Bronsted Acid Sites in Propene Aromatization over Zn-Modified HZSM-5 Detected by Operando Dual-Beam FTIR

被引：10

作者：

Liu, Jiaxu ^{[1
,2
]}

Lin, Long ^{[1
,2
]}

Wang, Jilei ^{[1
,2
]}

Zhou, Wei ^{[1
,2
]}

Miao, Cuilan ^{[1
,2
]}

Liu, Chunyan ^{[1
,2
]}

He, Ning ^{[1
,2
]}

Xin, Qin ^{[3
]}

Guo, Hongchen ^{[1
,2
]}

机构：

[1] Dalian Univ Technol, State Key Lab Fine Chem, 2 Linggong Rd, Dalian 116024, Peoples R China

[2] Dalian Univ Technol, Sch Chem Engn, 2 Linggong Rd, Dalian 116024, Peoples R China

[3] Chinese Acad Sci, State Key Lab Catalysis, Dalian Inst Chem Phys, Dalian 116023, Peoples R China

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2019年 / 123卷 / 12期

基金：

中国国家自然科学基金;

关键词：

PROPANE AROMATIZATION; ACTIVATION; CATALYSIS; CATIONS;

D O I：

10.1021/acs.jpcc.9b01415

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

An operando dual-beam Fourier transform infrared spectrometer was developed to identify the transient Bronsted acid sites (BAS) in propene aromatization over acidic HZSM-5 and Zn-modified HZSM-5 catalysts under real reaction conditions. The eliminated signals include gas-phase I molecular vibrations and heat irradiation at reaction temperatures. We directly observed that the initial activation of propene over Zn2+ of Zn-modified HZSM-5 generated a substantial number of transient BAS, which serve as active sites for the subsequent aromatization reactions. Moreover, during Transient Bronsted Acid Sites the propene aromatization process, the desorption of aromatic precursors over the Zn2+ of Zn/HZSM-5 is easier than that over the H+ of HZSM-5, resulting in an enhanced aromatics productivity. A density functional theory calculation certified the priority of the metallic Zn2+ sites over BAS in the competitive activation of propene molecules. The generation of transient BAS is energetically favorable.

引用

页码：7283 / 7289

页数：7

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