Effect of Water on Active Iron Sites for N2O Decomposition over Fe/ZSM-5 Catalyst

被引:22
|
作者
Xia, Haian [1 ]
Sun, Keqiang [1 ]
Feng, Zhaochi [1 ]
Li, Can [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2011年 / 115卷 / 02期
基金
中国国家自然科学基金;
关键词
NITROUS-OXIDE DECOMPOSITION; HIGH-TEMPERATURE TREATMENT; CHEMICAL-VAPOR-DEPOSITION; EX-FRAMEWORK FEZSM-5; SELECTIVE OXIDATION; MFI ZEOLITES; COMPREHENSIVE DFT; KINETIC-ANALYSIS; NOX REDUCTION; FE-SILICALITE;
D O I
10.1021/jp1094917
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 effect of H2O on N2O decomposition in Fe/ZSM-5 catalyst was investigated by steady-state kinetics, transient response methods, in situ Raman, and IR spectroscopies. Fe/ZSM-5 catalysts show very high activity in N2O decomposition but are deactivated rapidly when trace amounts of water are present. In situ Raman spectra results indicate that the peroxide bridge on the binuclear Fe sites are converted to the hydroxylated binuclear Fe sites when exposed to water. It was found that the Raman band at 743 cm(-1) and the IR bands at 3628 and 3672 cm(-1) are associated with the deactivation of the catalyst during N2O decomposition. The catalyst was regenerated after calcination at a temperature over 773 K. The inhibiting effect of H2O on N2O decomposition indicates that the presence of water leads to the structural transformation from the dehydroxylated binuclear Fe sites to the hydroxylated binuclear Fe sites on Fe/ZSM-5.
引用
收藏
页码:542 / 548
页数:7
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