Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH 3 -SCR tests, XRD, BET, SEM, HRTEM, EPR, H 2 -TPR, NH 3 -TPD, NO + O 2 -TPD, in situ DRIFTS, and kinetic tests were performed for the c...
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Veröffentlicht in: | Catalysis science & technology 2016-01, Vol.6 (16), p.6294-634 |
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Sprache: | eng |
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Zusammenfassung: | Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH
3
-SCR tests, XRD, BET, SEM, HRTEM, EPR, H
2
-TPR, NH
3
-TPD, NO + O
2
-TPD,
in situ
DRIFTS, and kinetic tests were performed for the catalytic measurement, bulk characterization and mechanism estimation. The NH
3
-SCR results indicated that Cu-SSZ-13-O showed higher DeNO
x
activity than Cu-SSZ-13-I in the absence or presence of H
2
O across the entire temperature range. The results of EPR, H
2
-TPR and NO + O
2
-TPD showed that more Cu
2+
ions existed in Cu-SSZ-13-O, which mainly accounts for the Lewis acid sites and the majority of the NO
x
adsorption or activation. The DRIFTS results showed that NH
3
on Lewis acid sites was more active than that on Brønsted acid sites in the NH
3
-SCR reaction. Furthermore, the DRIFTS results also indicated that monodentate nitrates are the most active nitrate species. Compared with Cu-SSZ-13-I, Cu-SSZ-13-O showed stronger Lewis acid site strengths and had more abundant monodentate nitrate species. Therefore, the NH
3
-SCR reaction proceeded more easily over Cu-SSZ-13-O in comparison with Cu-SSZ-13-I. This could be the key factor that explains the more excellent low-temperature SCR activity of Cu-SSZ-13-O. In addition, at low reaction temperatures, Cu-SSZ-13-O was less affected by pore (
i.e.
, intracrystalline) diffusion limitations.
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. |
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ISSN: | 2044-4753 2044-4761 |
DOI: | 10.1039/c6cy00737f |