Journal
ACS CATALYSIS
Volume 12, Issue 18, Pages 11281-11293Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c03048
Keywords
selective catalytic reduction; core-shell catalysts; Cu-SSZ-13; SO2 poisoning; potassium ion poisoning
Categories
Funding
- National Key Research and Development Plan [2019YFC1907602]
- National Natural Science Foundation of China [22035009, 22002050]
- Postdoctoral Science Foundation of China [2022T150765, 2020M683154]
- Project of Jiangsu University Senior Talents Foundation [20JDG35]
- National Engineering Laboratory for Mobile Source Emission Control Technology [NELMS2020B01]
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A bifunctional core-shell Cu-SSZ-13@CZO catalyst was designed and fabricated, which showed enhanced resistance to sulfur and potassium ion poisoning compared to pristine Cu-SSZ-13. The Cu-SSZ-13 core was protected from poisoning by the CZO shell, resulting in improved catalytic activity for selective catalytic reduction of nitrogen oxides.
The poisoning of sulfur oxides and alkali metals emitted from diesel exhaust to active sites of copper ion-exchanged chabazite (Cu-CHA) catalysts is still present and remains a formidable challenge in practical application. Herein, a bifunctional core-shell structural Cu-SSZ-13@Ce0.75Zr0.25O2 (Cu-SSZ-13@CZO) catalyst was designed and fabricated via a hydrothermally induced self-assembly protocol, and the catalytic activity of Cu-SSZ-13@CZO for selective catalytic reduction (SCR) of nitrogen oxides (NOx) with ammonia was systematically investigated. It unveils that Cu-SSZ-13@CZO features Cu-SSZ-13 as the core and dispersed CZO as the shell and that the CZO shell could not only serve as a sacrificial site protecting the Cu-SSZ-13 active core from SO2 poisoning by the formation of Ce-2(SO4)(3), which could further act as adsorption sites capturing the K+ through the strong interaction between K+ and cerium sulfate, but also render additional Bronsted acid sites functioning as sacrificial sites to trap K+, thereafter inhibiting the adsorption of K+ directly on active Cu species in the Cu-SSZ-13 core. As a result, the as-constructed Cu-SSZ-13@ CZO catalyst, therefore, exhibits perceptibly enhanced coresistance to sulfur and potassium ion poisoning with almost 100% NOx conversion in the temperature window of 275-475 ? as compared to 350-450 ?on pristine Cu-SSZ-13. The finding here may contribute to the fundamental understanding of the coresistance to sulfur oxides and alkali metal poison and thereafter inspire the advancement of a highly efficient NH3-SCR catalyst in the future.
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