Relationship between structure and performance of a novel highly dispersed MnOx on Co-Al layered double oxide for low temperature NH3-SCR

被引:136
作者
Wang, Ruihua [1 ]
Hao, Zhifei [1 ]
Li, Yi [2 ]
Liu, Guoquan [1 ]
Zhang, He [1 ]
Wang, Haitao [1 ]
Xia, Yuguo [3 ]
Zhan, Sihui [1 ]
机构
[1] Nankai Univ, Tianjin Key Lab Environm Remediat & Pollut Contro, MOE Key Lab Pollut Proc & Environm Criteria,Ctr R, Tianjin Key Lab Rare Earth Mat & Applicat,Coll En, Tianjin 300350, Peoples R China
[2] Tianjin Univ, Dept Chem, Tianjin 300072, Peoples R China
[3] Shandong Univ, Natl Engn Res Ctr Colloidal Mat, Sch Chem & Chem Engn, Jinan 250100, Shandong, Peoples R China
关键词
Mn(x)/LDO catalysts; Lewis acid sites; Low temperature; NH3-SCR; Reaction mechanism; SELECTIVE CATALYTIC-REDUCTION; NOX REDUCTION; SCR CATALYST; MIXED-OXIDE; NH3; NANOSHEET; REMOVAL; FABRICATION; OXIDATION; METALS;
D O I
10.1016/j.apcatb.2019.117983
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
A series of novel highly dispersed MnOx on Co-Al layered double oxide catalysts were fabricated for the low temperature NH3-SCR reaction. The Mn(0.25)/LDO exhibited outstanding catalytic performance with a unique multi-layered structure, which could achieve approximately 100% conversion of NOx in the range of 150-300 degrees C with a GHSV of 40,000 h(-1), as well as excellent H2O or SO2 tolerance and thermal stability. Various characterized techniques were applied to investigate the structural-activity relationship in the SCR reaction. The relative results indicated that the manganese addition could increase the quantity of Mn4+, surface adsorbed oxygen species, reducibility and ammonia adsorption capacity. Meanwhile, this strong interaction between Co-Al LDO and highly dispersed manganese species could significantly increase the positive charge density around Mn cations (Lewis acid sites) based on DFT calculated and in situ DRIFTS. Furthermore, it is proved that the NH3-SCR reaction over Mn(x)/LDO mainly follow E-R reaction pathway.
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页数:9
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