Insight into deactivation of commercial SCR catalyst by arsenic: an experiment and DFT study.
Fresh and arsenic-poisoned V2O5–WO3/TiO2 catalysts are investigated by experiments and DFT calculations for SCR activity and the deactivation mechanism. Poisoned catalyst (1.40% of arsenic) presents lower NO conversion and more N2O formation than fresh. Stream (5%) could further decrease the activity of poisoned catalyst above 350 °C. The deactivation is not attributed to the loss of surface area or phase transformation of TiO2 at a certain arsenic content, but due to the coverage of the V2O5 cluster and the decrease in the surface acidity: the number of Lewis acid sites and the stability of Brønsted acid sites. Large amounts of surface hydroxyl induced by H2O molecules provide more unreactive As–OH groups and give rise to a further decrease in the SCR activity. N2O is mainly from NH3 unselective oxidation at high temperatures since the reducibility of catalysts and the number of surface-active oxygens are improved by As2O5. Finally, the reaction pathway seems unchanged after poisoning: NH3 adsorbed on both Lewis and Brønsted acid sites is reactive.
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing, 100084, China.
Yue
Y
Peng
Junhua
J
Li
Wenzhe
W
Si
Jinming
J
Luo
Qizhou
Q
Dai
Xubiao
X
Luo
Xin
X
Liu
Jiming
J
Hao
D000143:Acids; D000327:Adsorption; D001151:Arsenic / Q000737:chemistry*; D002384:Catalysis; D004785:Environmental Pollutants / Q000737:chemistry; D004787:Environmental Pollution / Q000517:prevention & control; D058116:Lewis Acids; D009569:Nitric Oxide; D010084:Oxidation-Reduction; D014025:Titanium / Q000737:chemistry*; D017968:Vanadium Compounds / Q000737:chemistry*
D000143:Acids; D004785:Environmental Pollutants; D058116:Lewis Acids; D017968:Vanadium Compounds; C009495:titanium dioxide; D009569:Nitric Oxide; D014025:Titanium; D001151:Arsenic