Structure-activity relationship of Cr/Ti-PILC catalysts using a pre-modification method for NO oxidation and their surface species study

被引:53
|
作者
Zhong, Lei [1 ,2 ]
Yu, Yang [2 ,3 ]
Cai, Wei [2 ,3 ]
Geng, Xinxin [3 ]
Zhong, Qin [1 ,2 ,3 ]
机构
[1] Nanjing Univ Sci & Technol, Sch Environm & Biol Engn, Nanjing 210094, Jiangsu, Peoples R China
[2] Nanjing AIREP Environm Protect Technol Co Ltd, Nanjing 210091, Jiangsu, Peoples R China
[3] Nanjing Univ Sci & Technol, Sch Chem Engn, Nanjing 210094, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
MIXED-OXIDE CATALYSTS; IN-SITU FTIR; NO+O-2 COADSORPTION; DEEP OXIDATION; SCR REACTION; REDUCTION; ADSORPTION; CHROMIUM; CR; PERFORMANCE;
D O I
10.1039/c5cp00896d
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
The performances of Cr/Ti-PILC catalysts, which were prepared by the pre-modification method, are studied for the selective catalytic oxidation of NO. The aim of this paper is to elucidate the detailed relationship between physical nanoparticle structure and chemical properties. The maximum NO conversion over the Cr-HP(3)/TP catalyst reached 71.4% at 280 degrees C. The catalysts were characterized by powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction of H-2 (H-2-TPR), temperature-programmed desorption (TPD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) techniques. The characterization results demonstrated that the enhanced catalytic activity was ascribed to several beneficial effects, which were caused by the pre-modification such as the inhibition of crystallite size, improvement of Cr species dispersion and increase of the amount of active sites. XPS and FTIR experiments indicated that two Cr(VI) species, oxidized state CrO3 and chromate species with the anionic form, were generated via pre-modification, which played different roles in the catalytic reaction. In addition, the TPR and TPD results suggest that the increased active sites (Cr(VI) species) were conducive for the preferential adsorption and activation of NO. Furthermore, DRIFTS results revealed that the intermediates, NO+ and nitrates, interacted quickly to generate gaseous NO2.
引用
收藏
页码:15036 / 15045
页数:10
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