Mn-based catalysts supported on γ-Al2O3, TiO2 and MCM-41: a comparison for low-temperature NO oxidation with low ratio of O3/NO

被引:13
作者
Liu, Lijun [1 ]
Shen, Boxiong [1 ,2 ]
Si, Meng [1 ]
Yuan, Peng [1 ]
Lu, Fengju [1 ]
Gao, Hongpei [3 ]
Yao, Yan [4 ]
Liang, Cai [5 ]
Xu, Hongjie [6 ]
机构
[1] Hebei Univ Technol, Sch Energy & Environm Engn, Tianjin, Peoples R China
[2] Hebei Univ Technol, Sch Chem Engn, Tianjin, Peoples R China
[3] Clean Energy Technol Res Inst Co Ltd, China Huaneng Grp, Beijing, Peoples R China
[4] Suzhou TPRI Energy & Environm Technol Co Ltd, Suzhou, Peoples R China
[5] Chengdu Dongfang KWH Environm Protect Catalysts C, Chengdu, Peoples R China
[6] Xian Thermal Engn Inst, Xian, Peoples R China
关键词
MANGANESE OXIDE CATALYSTS; IN-SITU DRIFTS; DEEP OXIDATION; MIXED OXIDES; NITRIC-OXIDE; BENZENE OXIDATION; GASEOUS OZONE; PERFORMANCE; EFFICIENT; REDUCTION;
D O I
10.1039/d1ra01820e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Mn-Based catalysts supported on gamma-Al2O3, TiO2 and MCM-41 synthesized by an impregnation method were compared to evaluate their NO catalytic oxidation performance with low ratio O-3/NO at low temperature (80-200 degrees C). Activity tests showed that the participation of O-3 remarkably promoted the NO oxidation. The catalytic oxidation performance of the three catalysts decreased in the following order: Mn/gamma-Al2O3 > Mn/TiO2 > Mn/MCM-41, indicating that Mn/gamma-Al2O3 exhibited the best catalytic activity. In addition, there was a clear synergistic effect between Mn/gamma-Al2O3 and O-3, followed by Mn/TiO2 and O-3. The characterization results of XRD, EDS mapping, BET, H-2-TPR, XPS and TG showed that Mn/gamma-Al2O3 had good manganese dispersion, excellent redox properties, appropriate amounts of coexisting Mn3+ and Mn4+ and abundant chemically adsorbed oxygen, which ensured its good performance. In situ DRIFTS demonstrated the NO adsorption performance on the catalyst surface. As revealed by in situ DRIFTS experiments, the chemically adsorbed oxygen, mainly from the decomposition of O-3, greatly promoted the NO adsorption and the formation of nitrates. The Mn-based catalysts showed stronger adsorption strength than the corresponding pure supports. Due to the abundant adsorption sites provided by pure gamma-Al2O3, under the interaction of Mn and gamma-Al2O3, the Mn/gamma-Al2O3 catalyst exhibited the strongest NO adsorption performance among the three catalysts and produced lots of monodentate nitrates (-O-NO2) and bidentate nitrates (-O2NO), which were the vital intermediate species for NO2 formation. Moreover, the NO-TPD studies also demonstrated that Mn/gamma-Al2O3 showed the best NO desorption performance among the three catalysts. The good NO adsorption and desorption characteristics of Mn/gamma-Al2O3 improved its high catalytic activity. In addition, the activity test results also suggested that Mn/gamma-Al2O3 exhibited good SO2 tolerance.
引用
收藏
页码:18945 / 18959
页数:15
相关论文
共 81 条
[11]   Gd-modified MnOx for the selective catalytic reduction of NO by NH3: The promoting effect of Gd on the catalytic performance and sulfur resistance [J].
Fan, Zhaoyang ;
Shi, Jian-Wen ;
Gao, Chen ;
Gao, Ge ;
Wang, Baorui ;
Wang, Yao ;
He, Chi ;
Niu, Chunming .
CHEMICAL ENGINEERING JOURNAL, 2018, 348 :820-830
[12]   Identification of MnOx species and Mn valence states in MnOx/TiO2 catalysts for low temperature SCR [J].
Fang, De ;
Xie, Junlin ;
Hu, Hua ;
Yang, Hu ;
He, Feng ;
Fu, Zhengbing .
CHEMICAL ENGINEERING JOURNAL, 2015, 271 :23-30
[13]   Insights on the mechanism of enhanced selective catalytic reduction of NO with NH3 over Zr-doped MnCr2O4: A combination of in situ DRIFTS and DFT [J].
Gao, Erhao ;
Pan, Hua ;
Zhang, Wei ;
Li, Younan ;
Cao, Guanghan ;
Bernards, Matthew T. ;
He, Yi ;
Shi, Yao .
CHEMICAL ENGINEERING JOURNAL, 2020, 386
[14]   Mn2NiO4 spinel catalyst for high-efficiency selective catalytic reduction of nitrogen oxides with good resistance to H2O and SO2 at low temperature [J].
Gao, Fengyu ;
Tang, Xiaolong ;
Yi, Honghong ;
Zhao, Shunzheng ;
Zhu, Wenjuan ;
Shi, Yiran .
JOURNAL OF ENVIRONMENTAL SCIENCES, 2020, 89 :145-155
[15]   High-efficiency catalytic oxidation of nitric oxide over spherical Mn-Co spinel catalyst at low temperature [J].
Gao, Fengyu ;
Chu, Chao ;
Zhu, Wenjuan ;
Tang, Xiaolong ;
Yi, Honghong ;
Zhang, Runcao .
APPLIED SURFACE SCIENCE, 2019, 479 :548-556
[16]   In-situ DRIFTS for the mechanistic studies of NO oxidation over α-MnO2, β-MnO2 and γ-MnO2 catalysts [J].
Gao, Fengyu ;
Tang, Xiaolong ;
Yi, Honghong ;
Chu, Chao ;
Li, Na ;
Li, Jingying ;
Zhao, Shunzheng .
CHEMICAL ENGINEERING JOURNAL, 2017, 322 :525-537
[17]   Identification of neutral and charged NxOy surface species by IR spectroscopy [J].
Hadjiivanov, KI .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2000, 42 (1-2) :71-144
[18]   NOx Removal from Flue Gas Using an Ozone Advanced Oxidation Process with Injection of Low Concentration of Ethanol: Performance and Mechanism [J].
Han, Zhitao ;
Wang, Junming ;
Zou, Tianyu ;
Zhao, Dongsheng ;
Gao, Cong ;
Dong, Jingming ;
Pan, Xinxing .
ENERGY & FUELS, 2020, 34 (02) :2080-2088
[19]   Insight into structure defects and catalytic mechanism for NO oxidation over Ce0.6Mn0.4Ox solid solutions catalysts: Effect of Manganese precursors [J].
Hao, Boyuan ;
Sun, Yonggang ;
Shen, Qun ;
Zhang, Xin ;
Zhang, Zhongshen .
CHEMOSPHERE, 2020, 243
[20]   Preparation and Investigation of Iron-Cerium Oxide Compounds for NOx, Reduction [J].
Hou, Xueyan ;
Qian, Junning ;
Li, Lulu ;
Wan, Fan ;
Li, Bin ;
He, Fenglang ;
Fan, Minguang ;
Tong, Zhangfa ;
Dong, Lihui ;
Dong, Lin .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2018, 57 (49) :16675-16683