MnO2的晶相结构和表面性质对低温NH3-SCR反应的影响

doi:10.3866/PKU.WHXB201204175

Abstract

Abstract:

Two manganese oxides with the same nanorod-shaped morphology but different crystal structures, tunnel and layer structures, were synthesized and investigated for selective catalytic reduction of NO_x with NH₃ (NH₃-SCR) at low temperature. Tunneled α-MnO₂ had much higher catalytic activity than layered δ-MnO₂ under the same reaction conditions. Experiment results revealed that the surface area was not the main factor to affect the NH₃-SCR activities over the MnO₂ nanorods and that the activities were structure sensitive. Structure analysis and temperature-programmed desorption experiments of NH₃ (NH₃-TPD) suggested that the exposed (110) plane of α-MnO₂ had many Mn cations in coordinatively unsaturated environment, while all of the Mn cations on the exposed (001) plane of δ-MnO₂ were in coordinatively saturated environment. Thus, α-MnO₂ possessed many more Lewis acid sites. Furthermore, α-MnO₂ has weaker Mn―O bonds and an efficient tunnel structure, which are favorable characteristics for NH₃ adsorption. Moreover, X-ray photoelectron spectroscopy (XPS) and thermal gravimetric (TG) analysis indicated that α-MnO₂ obtained a higher capability for NH₃ and NO_x activation than δ-MnO₂. The crystal structure and surface properties of α-MnO₂ are more suitable to the adsorption of NH₃ and activation of NH₃ and NO_x, which accounts for the higher catalytic activity of the α-MnO₂ nanorods.

Key words: α-MnO₂, δ-MnO₂, Low-temperature, Selective catalytic reduction of NO_x with NH₃, Crystal structure, Surface property

MSC2000:

O643

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DAI Yun, LI Jun-Hua, PENG Yue, TANG Xing-Fu. Effects of MnO₂ Crystal Structure and Surface Property on the NH₃-SCR Reaction at Low Temperature[J].Acta Phys. -Chim. Sin., 2012, 28(07): 1771-1776.

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Effects of MnO₂ Crystal Structure and Surface Property on the NH₃-SCR Reaction at Low Temperature

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Effects of MnO₂ Crystal Structure and Surface Property on the NH₃-SCR Reaction at Low Temperature