Heterometal Incorporation in Metal-Exchanged Zeolites Enables Low-Temperature Catalytic Activity of NOx Reduction

被引：51

作者：

Yang, Xiaofan ^{[1
]}

Wu, Zili ^{[2
,3
]}

Moses-Debusk, Melanie ^{[1
]}

Mullins, David R. ^{[3
]}

Mahurin, Shannon M. ^{[3
]}

Geiger, Robert A. ^{[1
]}

Kidder, Michelle ^{[3
]}

Narula, Chaitanya K. ^{[1
]}

机构：

[1] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA

[2] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA

[3] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2012年 / 116卷 / 44期

关键词：

SITU XAFS SPECTROSCOPY; NITRIC-OXIDE; IRON SITES; ZSM-5; ZEOLITES; HYDROTHERMAL STABILITY; PROTONATED NITROSAMIDE; SELECTIVE REDUCTION; FE-ZEOLITES; AB-INITIO; FE-ZSM-5;

D O I：

10.1021/jp3056043

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：

A series of new heterobimetallic zeolites has been synthesized by incorporating a secondary metal cation M (Sc3+, Fe3+, In3+, and La3+) in Cuexchanged ZSM-5, zeolite-beta, and SSZ-13 zeolites under carefully controlled experimental conditions. Characterization by diffuse-reflectance ultraviolet-visible spectroscopy (UV-vis), X-ray powder diffraction (XRD), extended X-ray absorption fine structure spectroscopy (EXAFS), and electron paramagnetic resonance spectroscopy (EPR) does not permit conclusive structural determ nation but supports the proposal that M3+ is hosted in zeolite structures in the vicinity of Cu(II), resulting in high NOx conversion activity at 150 degrees C. Among various zeolites reported here, CuFe-SSZ-13 offers the best NOx conversion activity in the 150-650 degrees C range and is hydrothermally stable when tested under accelerated aging conditions. Mechanistic studies employing stopped-flow diffuse reflectance FT-IR spectroscopy (DRIFTS) suggest that the high concentration of NO+ generated by heterobimetallic zeolites is probably responsible for their superior low-temperature NOx activity.

引用

页码：23322 / 23331

页数：10

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