Citation: 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 Physico-Chimica Sinica, ;2012, 28(07): 1771-1776. doi: 10.3866/PKU.WHXB201204175 shu

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

DAI Yun ¹ ,
LI Jun-Hua ^1, ,
PENG Yue ¹ ,
TANG Xing-Fu ²

1.
1. State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, P. R. China;
2. Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, P. R. China

Received Date: 6 March 2012
Available Online: 17 April 2012
Fund Project: 国家自然科学基金(51078203) (51078203)国家高技术研究发展计划项目(863) (2010AA065002, 2009AA06Z301)资助 (863) (2010AA065002, 2009AA06Z301)

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