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钾掺杂的C12A7-O-催化剂上NO的还原特性

Reduction features of NO over a potassium-doped C12A7-O- catalyst.

作者信息

Gao Aimei, Zhu Xifeng, Wang Huajing, Tu Jing, Lin Peiyan, Torimoto Youshifumi, Sadakata Masayoshi, Li Quanxin

机构信息

Lab of Biomass Clean Energy, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, People's Republic of China.

出版信息

J Phys Chem B. 2006 Jun 22;110(24):11854-62. doi: 10.1021/jp060178t.

Abstract

The NO reduction features over a noble-metal-free NO(x) storage/reduction catalyst (Ca24Al28O644O-/K, defined as C12A7-O-/K), including the NO conversion, the N2 selectivity, and sulfur tolerance, were investigated with hydrogen and C3H6 as the reducing agents in a fixed-bed continuous flow reactor. The NO conversion and the N2 selectivity on the C12A7-O-/K catalyst mainly depends on the sample temperature, the percentage of potassium, the reducing agents, and the composition of the mixture of gases. The C12A7-O-/10%K catalyst possessed the highest selective reduction ability (to N2) among the catalysts C12A7-O-/x%K. Over 50% of NO can be reduced to N2 with H2 as the reduction agent at 550-700 degrees C. The C12A7-O-/K catalyst also shows higher NO(x) storage capacity (183.9 micromol/g at about 550 degrees C) as well as sulfur tolerance for both the NO(x) storage and the reduction processes. The catalyst characteristics and the intermediate species formed in the NO storage and reduction processes were investigated by the X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and time-of-flight mass spectrometry. The mechanism of NO(x) reduction was addressed according to the above investigations.

摘要

在固定床连续流动反应器中,以氢气和C3H6作为还原剂,研究了无贵金属的氮氧化物存储/还原催化剂(Ca24Al28O644O-/K,定义为C12A7-O-/K)上的NO还原特性,包括NO转化率、N2选择性和耐硫性。C12A7-O-/K催化剂上的NO转化率和N2选择性主要取决于样品温度、钾含量、还原剂以及气体混合物的组成。在C12A7-O-/x%K催化剂中,C12A7-O-/10%K催化剂具有最高的(对N2的)选择性还原能力。在550-700℃下,以H2作为还原剂时,超过50%的NO可被还原为N2。C12A7-O-/K催化剂还表现出较高的氮氧化物存储容量(在约550℃时为183.9微摩尔/克)以及在氮氧化物存储和还原过程中的耐硫性。通过X射线衍射、X射线光电子能谱、傅里叶变换红外光谱和飞行时间质谱研究了催化剂特性以及在NO存储和还原过程中形成的中间物种。根据上述研究探讨了氮氧化物还原的机理。

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