Manganese oxide catalysts supported on zinc oxide nanorod arrays: A new composite for selective catalytic reduction of NOx with NH3 at low temperature

被引:28
作者
Yan, Zheng [1 ,2 ]
Yang, Jiayao [1 ,2 ]
Ge, Xinlei [3 ]
Yu, Jingyao [1 ,2 ]
Wei, Lihong [1 ,2 ]
Yang, Tianhua [1 ,2 ]
He, Beini [4 ]
Wang, Xidong [4 ]
Liu, Lili [4 ]
机构
[1] Shenyang Aerosp Univ, Liaoning Key Lab Clean Energy, Coll Energy & Environm, Shenyang 110034, Liaoning, Peoples R China
[2] Shenyang Aerosp Univ, Coll Energy & Environm, Inst Clean Energy & Environm Engn, Shenyang 110034, Liaoning, Peoples R China
[3] Nanjing Univ Informat Sci & Technol, Jiangsu Collaborat Innovat Ctr Atmospher Environm, Jiangsu Key Lab Atmospher Environm Monitoring & P, Sch Environm Sci & Engn, Nanjing 210044, Jiangsu, Peoples R China
[4] Peking Univ, Coll Engn, Beijing Key Lab Solid Waste Utilizat & Management, Beijing 100871, Peoples R China
基金
中国国家自然科学基金;
关键词
Low-temperature SCR; Manganese oxides; Zinc oxide nanorod arrays; NH3-SCR reaction mechanism; In situ DRIFTS; RATIONAL DESIGN; SCR REACTION; PERFORMANCE; MECHANISM; DRIFT; ZNO; MICROSPHERES; REACTIVITY; RESISTANCE; MNOX/TIO2;
D O I
10.1016/j.apsusc.2019.06.185
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
In this study, a new composite of low-temperature selective catalytic reduction (LT-SCR) catalyst is synthesized by impregnating MnOx onto ZnO nanorod arrays integrated with cordierite ceramic substrate (MnOx-ZnO/CC), which exhibits improved activities at 100-250 degrees C compared to its analogue that fabricated from TiO2 nanorod arrays (MnOx-TiO2/CC). By optimizing the synthesis conditions, the MnOx-ZnO/CC catalyst obtains a maximum NOx conversion efficiency of 96.8% at 200 degrees C. The introduction of ZnO nanorod arrays not only provides a high surface area, but also results in the formation of amorphous MnOx. A higher content of Mn4+, proper ratio of surface-adsorbed oxygen (O-alpha), and more Lewis acid sites are found on the surface of the MnOx-ZnO/ CC catalyst than that on the MnOx-TiO2/CC counterpart. Additional information about the reaction mechanism is systematically investigated via in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), the results of which demonstrate that the LT-SCR reactions over the MnOx-ZnO/CC catalyst generally occur between NOx and NH3 species in the adsorption status, following the Langmuir-Hinshelwood pathway. The enhanced activities can be attributed to the generation of abundant NH4NO3 originating from NO2 in the "Fast SCR" route, because the synergistic effect between MnOx and ZnO facilitates the oxidation of NO.
引用
收藏
页码:579 / 589
页数:11
相关论文
共 55 条
[1]   Cu-Mn and Co-Mn catalysts synthesized from hydrotalcites and their use in the oxidation of VOCs [J].
Antonio Aguilera, Daniel ;
Perez, Alejandro ;
Molina, Rafael ;
Moreno, Sonia .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 104 (1-2) :144-150
[2]   Nitrogen-Doped Titanium Dioxide as Visible-Light-Sensitive Photocatalyst: Designs, Developments, and Prospects [J].
Asahi, Ryoji ;
Morikawa, Takeshi ;
Irie, Hiroshi ;
Ohwaki, Takeshi .
CHEMICAL REVIEWS, 2014, 114 (19) :9824-9852
[3]   Preparation of beta-coated cordierite honeycomb monoliths by in situ synthesis -: Utilisation as Pt support for NOx abatement in diesel exhaust [J].
Bueno-López, A ;
Lozano-Castelló, D ;
Such-Basáñez, I ;
García-Cortés, JM ;
Illán-Gómez, MJ ;
de Lecea, CSM .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 58 (1-2) :1-7
[4]   The activity and characterization of MnOx-CeO2-ZrO2/γ-Al2O3 catalysts for low temperature selective catalytic reduction of NO with NH3 [J].
Cao, Fan ;
Xiang, Jun ;
Su, Sheng ;
Wang, Pengying ;
Sun, Lushi ;
Hu, Song ;
Lei, Siyuan .
CHEMICAL ENGINEERING JOURNAL, 2014, 243 :347-354
[5]   TRA and DRIFTS studies of the fast SCR reaction over CeO2/TiO2 catalyst at low temperatures [J].
Cao, Li ;
Chen, Lei ;
Wu, Xiaodong ;
Ran, Rui ;
Xu, Tengfei ;
Chen, Ze ;
Weng, Duan .
APPLIED CATALYSIS A-GENERAL, 2018, 557 :46-54
[6]   DRIFT Study on Cerium-Tungsten/Titiania Catalyst for Selective Catalytic Reduction of NOx with NH3 [J].
Chen, Liang ;
Li, Junhua ;
Ge, Maofa .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (24) :9590-9596
[7]   Selective catalytic reduction over size-tunable rutile TiO2 nanorod microsphere-supported CeO2 catalysts [J].
Cheng, Kai ;
Song, Weiyu ;
Cheng, Ying ;
Liu, Jian ;
Zhao, Zhen ;
Wei, Yuechang .
CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (12) :4478-4490
[8]   Spectroscopic characterisation of MoO3/TiO2 deNOx-SCR catalysts:: Redox and coordination properties [J].
Dall'Acqua, L ;
Nova, I ;
Lietti, L ;
Ramis, G ;
Busca, G ;
Giamello, E .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (21) :4991-4998
[9]   Advanced MnOx/TiO2 Catalyst with Preferentially Exposed Anatase {001} Facet for Low-Temperature SCR of NO [J].
Deng, Shengcai ;
Meng, Tingting ;
Xu, Bolian ;
Gao, Fei ;
Ding, Yuanhua ;
Yu, Lei ;
Fan, Yining .
ACS CATALYSIS, 2016, 6 (09) :5807-5815
[10]   Significant Promotion Effect of Mo Additive on a Novel Ce-Zr Mixed Oxide Catalyst for the Selective Catalytic Reduction of NOx with NH3 [J].
Ding, Shipeng ;
Liu, Fudong ;
Shi, Xiaoyan ;
Liu, Kuo ;
Lian, Zhihua ;
Xie, Lijuan ;
He, Hong .
ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (18) :9497-9506