期刊
CHEMICAL ENGINEERING JOURNAL
卷 379, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.122376
关键词
Selective catalytic reduction of NOx; Hierarchical pore structure; Cu/SAPO-34; Ion exchanged method; Good resistance to hydrothermal aging
资金
- Harbin Science and Technology Innovation Talent Fund (Outstanding Academic Leader Project) [RC2016XK015004]
- Postdoctoral Science Research Developmental Foundation of Heilongjiang Province of China [LBHZ16176]
- University Nursing Program for Young Scholars with Creative talents [UNPYSCT-2017115]
- State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University
- Youth Science and Technology Innovation Team Project of Heilongjiang Province [RCYJTD201803]
- Heilongjiang Human Resources And Social Security Bureau
SAPO-34 with hierarchical pore structure (SAPO-34-H) was first prepared by a hard-template method using CaCO3 as template. The xCu/SAPO-34-H (x = 1.1 wt%, 1.9 wt%, 2.7 wt% and 3.2 wt%) catalysts were synthesized by ion-exchanged method and applied for selective catalytic reduction (SCR) of NOx with NH3. XRD, XRF, SEM, TEM, UV-vis-DRS, NH3-TPD, XPS, NMR, EPR and in situ DRIFTS were used to characterize the physiochemical properties of the catalysts. The SCR activity results demonstrate that 100% NOx conversion can be achieved over the 2.7 wt%Cu/SAPO-34-H catalyst at about 150 degrees C in the GHSV of 40,000 h(-1). Furthermore, NOx conversion under the testing conditions of H2O and SO2 was slightly influenced over the 2.7 wt%Cu/SAPO-34-H catalyst after high-temperature hydrothermal aging at 700 and 800 degrees C, respectively. NOx convention presents above 90% at 170-480 degrees C even introducing 10% H2O for 10 h, and it can be maintained 90% by introducing 200 ppm SO2 and 12% H2O over 2.7 wt%Cu/SAPO-34-H. In the meantime, 2.7 wt%Cu/SAPO-34-H was investigated through the low-temperature hydration treatment at 80 degrees C, it also displays superior hydration treatment resistance for low-temperature. The outstanding performance is ascribed to the hierarchical pore structure of 2.7 wt%Cu/SAPO-34-H, which can promote the diffusion of reaction gas and generation of active sites. EPR results indicate that the Cu2+ species mainly locates the site I in 2.7 wt%Cu/SAPO-34-H, while the Cu2+ species mainly locates the site III for the conversional 2.7 wt%Cu/SAPO-34. Moreover, the in situ DRIFTS results indicate that the Lewis acid sites are easy to participate in NH3-SCR reaction for 2.7 wt%Cu/SAPO-34-H, which mainly follows the Eley-Rideal (E-R) reaction mechanism at 200 degrees C for 2.7 wt%Cu/SAPO-34-H.
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