Design of MoFe/Beta@CeO2 catalysts with a core-shell structure and their catalytic performances for the selective catalytic reduction of NO with NH3

被引:102
|
作者
Liu, Jixing [1 ,2 ]
Du, Yuhao [1 ,2 ]
Liu, Jian [1 ,2 ,4 ]
Zhao, Zhen [1 ,2 ]
Cheng, Kai [1 ,2 ]
Chen, Yongsheng [3 ]
Wei, Yuechang [1 ,2 ]
Song, Weiyu [1 ,2 ]
Zhang, Xiao [1 ,2 ]
机构
[1] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[2] China Univ Petr, Beijing Key Lab Oil & Gas Pollut Control, Beijing 102249, PR, Peoples R China
[3] Chinese Univ Hong Kong, William MW Mong Engn Bldg, Shatin, Hong Kong, Peoples R China
[4] 18 Fuxue Rd, Beijing 102249, Peoples R China
基金
北京市自然科学基金; 中国国家自然科学基金;
关键词
MoFe/Beta; CeO2; Core-shell; SO2; tolerance; Selective catalytic reduction; FE-BEA; STRUCTURE DEPENDENCE; SO2; RESISTANCE; SCR CATALYST; H-BEA; NH3-SCR; OXIDATION; FE-ZSM-5; CEO2; MECHANISM;
D O I
10.1016/j.apcatb.2016.10.039
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
MoFe/Beta@CeO2 core-shell catalyst was designed with nano-size Beta supporting MoFe bimetallic oxides as the core and CeO2 thin film as the shell. The structure and physico-chemical properties of the coated and uncoated CeO2 catalysts were characterized by TEM, SEM, XRD, N-2 adsorption-desorption, XPS, XANES, ICP-AES, NH3-TPD, H-2-TPR and in-situ DRIFTS. The catalytic activity tests for NH3-SCR of NO indicated that the catalyst coated by CeO2 shell exhibits a remarkable improvement of deNO(x) activity, excellent tolerance to SO2 and H2O, as well as high thermal stability. The both chemisorbed oxygen species (O-2(-), O-) and specific surface area increased for the catalysts after the coating of CeO2 shells. CeO2 shells not only increase the acid amount but also improve its acid strength, which could be beneficial to improving NO oxidation to NO2 during NH3-SCR. Furthermore, there is a strong interaction among the iron oxides, molybdenum oxides and CeO2 shells. CeO2 shells can serve as an effective barrier to inhibit the active metal oxides nanoparticles from aggregating at high temperature. As a result, the coated catalyst with CeO2 thin film shows a better thermal stability than the uncoated one. What's more, CeO2 shells can not only suppress the formation of ammonium nitrate and sulfate species blocking the active iron sites but also restrain the generation of iron sulfate, leading to a higher SO2 and H2O-tolerance. The above results demonstrate that the design of a core-shell structure catalyst is favorable for improving the performance of deNO(x) catalysts. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:704 / 714
页数:11
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