Unraveling the structure and role of Mn and Ce for NOx reduction in application-relevant catalysts

被引:77
作者
Gevers, Lieven E. [1 ]
Enakonda, Linga R. [1 ]
Shahid, Ameen [1 ]
Ould-Chikh, Samy [1 ]
Silva, Cristina I. Q. [1 ]
Paalanen, Pasi P. [1 ]
Aguilar-Tapia, Antonio [2 ]
Hazemann, Jean-Louis [2 ,3 ]
Hedhili, Mohamed Nejib [4 ]
Wen, Fei [5 ]
Ruiz-Martinez, Javier [1 ]
机构
[1] King Abdullah Univ Sci & Technol, KAUST Catalysis Ctr, Catalysis Nanomat & Spect CNS, Thuwal 23955, Saudi Arabia
[2] Univ Grenoble Alpes, Inst Chim Mole Grenoble, UAR2607 CNRS, F-38000 Grenoble, France
[3] UPR 2940 CNRS, Inst Neel, F-38042 Grenoble, France
[4] King Abdullah Univ Sci & Technol, KAUST Core Labs, Thuwal 23955, Saudi Arabia
[5] Umicore AG & Co KG, Rodenbachen Chaussee 4, D-63457 Hanau, Germany
关键词
LOW-TEMPERATURE SCR; MANGANESE OXIDE CATALYSTS; MIXED OXIDES; NITRIC-OXIDE; NH3; REMOVAL; PERFORMANCE; CERIUM; REDOX; MECHANISM;
D O I
10.1038/s41467-022-30679-9
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Mn-based oxides are promising for the selective catalytic reduction (SCR) of NOx with NH3 at temperatures below 200 degrees C. There is a general agreement that combining Mn with another metal oxide, such as CeOx improves catalytic activity. However, to date, there is an unsettling debate on the effect of Ce. To solve this, here we have systematically investigated a large number of catalysts. Our results show that, at low-temperature, the intrinsic SCR activity of the Mn active sites is not positively affected by Ce species in intimate contact. To confirm our findings, activities reported in literature were surface-area normalized and the analysis do not support an increase in activity by Ce addition. Therefore, we can unequivocally conclude that the beneficial effect of Ce is textural. Besides, addition of Ce suppresses second-step oxidation reactions and thus N2O formation by structurally diluting MnOx. Therefore, Ce is still an interesting catalyst additive. The role of Ce one Mn-based catalysts for the selective catalytic reduction of NOx at low temperature is an ongoing debate. Here the authors demonstrate that Ce has a structural promoting effect but impacts negatively on the intrinsic catalytic activity of Mn.
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页数:10
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