Alkali metal poisoning of a CeO2-WO3 catalyst used in the selective catalytic reduction of NOx with NH3: an experimental and theoretical study.
The alkali metal-induced deactivation of a novel CeO(2)-WO(3) (CeW) catalyst used for selective catalytic reduction (SCR) was investigated. The CeW catalyst could resist greater amounts of alkali metals than V(2)O(5)-WO(3)/TiO(2). At the same molar concentration, the K-poisoned catalyst exhibited a greater loss in activity compared with the Na-poisoned catalyst below 200 °C. A combination of experimental and theoretical methods, including NH(3)-TPD, DRIFTS, H(2)-TPR, and density functional theory (DFT) calculations, were used to elucidate the mechanism of the alkali metal deactivation of the CeW catalyst in SCR reaction. Experiments results indicated that decreases in the reduction activity and the quantity of Brønsted acid sites rather than the acid strength were responsible for the catalyst deactivation. The DFT calculations revealed that Na and K could easily adsorb on the CeW (110) surface and that the surface oxygen could migrate to cover the active tungsten, and then inhibit the SCR of NO(x) with ammonia. Hot water washing is a convenient and effective method to regenerate alkali metal-poisoned CeW catalysts, and the catalytic activity could be recovered 90% of the fresh catalyst.
School of Environment, Tsinghua University, Beijing 100084, China.
Yue
Y
Peng
Junhua
J
Li
Liang
L
Chen
Jinghuan
J
Chen
Jian
J
Han
He
H
Zhang
Wei
W
Han
D000327:Adsorption; D000468:Alkalies / Q000737:chemistry*; D000641:Ammonia / Q000737:chemistry*; D002384:Catalysis; D002563:Cerium / Q000737:chemistry*; D058116:Lewis Acids / Q000737:chemistry; D008670:Metals / Q000737:chemistry*; D008956:Models, Chemical; D009566:Nitrates / Q000737:chemistry*; D009573:Nitrites / Q000737:chemistry*; D010084:Oxidation-Reduction; D010087:Oxides / Q000737:chemistry*; D014414:Tungsten / Q000737:chemistry*; D014867:Water / Q000737:chemistry; D014961:X-Ray Diffraction
D000468:Alkalies; D058116:Lewis Acids; D008670:Metals; D009566:Nitrates; D009573:Nitrites; D010087:Oxides; D014867:Water; D002563:Cerium; C030583:ceric oxide; D000641:Ammonia; C511604:tungsten oxide; D014414:Tungsten