Zhong-yi Wang,Rui-tang Guo,Zhen-zhen Guan,Xu Shi,Wei-guo Pan,Zai-guo Fu,Hao Qin,Xing-yu Liu
A sequence of Cr-modified CeZr 2 O x catalysts were synthesized through the co-precipitation way and applied in selective catalytic reduction (SCR) of NO x with ammonia. The optimal catalyst (Cr 1 CeZr 2 O x ) exhibited the excellent NH 3 -SCR activity and high SO 2 resistance. From the characterization results, Cr species in Cr 1 CeZr 2 O x could suppress the formation of ZrO 2 crystals, which could also contribute to stronger surface acidity and reducibility . Besides, more Ce 3+ and surface adsorbed oxygen species were observed on Cr 1 CeZr 2 O x catalyst. On the basis of in situ DRIFT experiments, it could be confirmed that the NH 3 -SCR process on Cr 1 CeZr 2 O x was promoted through Langmuir-Hinshelwood (L-H) mechanism. Besides, the improved NO oxidation and more ad-NO x and ad-NH 3 also played a vital role for the superior low-temperature SCR activity of Cr 1 CeZr 2 O x .
In this paper, a series of Sb modified CeZr 2 O x mixed oxides (Sb y CZ) were synthesized by citrate method for the selective catalytic reduction of NO with ammonia (NH 3 -SCR). Experimental results exhibited that the Sb addition could bring a great improvement of SCR activity at 200–360 °C owing to the enhancement in surface area , redox ability and surface acidity . More importantly, the sulfur tolerance of the catalyst with proper Sb loading contents was dramatically improved. For instance, above 85% deNO x efficiency was retained over Sb 0.5 CZ catalyst after 24 h reaction in the presence of 100 ppm SO 2 and 5 vol.% H 2 O. As for pure CeZr 2 O x and the catalysts with low Sb loading contents, the serious accumulation of ammonium sulfates resulted in the deactivation after SO 2 exposure. However, with excessive Sb addition, more labile oxygen readily reacted with SO 2 and the redox cycle was then disrupted, leading to the decrease of SCR activity. With an appropriate Sb loading contents, the sulfate species preferentially formed around Sb cations could restrain the further consumption of oxygen species in Ce-O-Ce or Ce-O-Zr mode by SO 2 via a space confinement effect. Thus, a certain amount of labile oxygen was preserved to drive the SCR reaction, thereby enhancing the sulfur tolerance of the catalyst.
Sun Xiao,Guo Rui-tang,Li Ming-yuan,Sun Peng,Pan Wei-guo,Liu Shu-ming,Liu Jian,Liu Shuai-wei
Fe was used as the modifier to improve the performance of CeZr 2 O
x
catalyst for the selective catalytic reduction (SCR) reaction with ammonia. Experimental results revealed that proper Fe species (Fe/Ce molar ratio = 2) could effectively improve the SCR activity of CeZr 2 O
x
, along with the elevated resistance to SO 2 and H 2 O. The characterization results including BET, XRD, H 2 -TPR and NH 3 -TPD confirmed that Fe species in Fe 2 CeZr 2 O
x
catalyst could inhibit the formation of ZrO 2 crystals and lead to higher reducibility and surface acidity. In addition, more Ce 3+ and surface active oxygen species could be detected on Fe 2 CeZr 2 O
x
compared with CeZr 2 O
x
. By means of in situ DRIFT technique, it could be deduced that the SCR reaction process over Fe 2 CeZr 2 O
x
was accelerated mainly through theL–H pathway due to the advanced adsorption of NH 3 and NO
x
species, along with the promoted NO conversion to NO 2 . Therefore, the modification of CeZrO
x
catalyst by Fe had a significant stimulation effect on its low-temperature SCR performance.
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