期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 207, 期 -, 页码 60-71出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2017.02.001
关键词
Ag/Al2O3; HC-SCR; Water vapor; H-2; DFT
资金
- National Natural Science Foundation of China [21373261, 21673277, 21637005]
Water vapor is typically present in diesel engine exhausts, and thus the design of catalysts with high water-tolerance is highly desired. The addition of water vapor was shown to have quite different influences on the activity of Ag/Al2O3 catalysts with different Ag loadings during the H-2-assistedC(3)H(6)-SCR of NOx (H-2-C3H6-SCR). The 2 wt% Ag/Al2O3 catalyst showed the best activity for H2-C3H6-SCR, with excellent water resistance over the whole temperature range. An enhancement in NOx conversion was observed after water vapor was introduced, particularly at low temperatures. Over this catalyst, kinetic studies confirmed that H2O addition did not change the apparent activation energy for NOx reduction, while it increased the reaction order of C3 H-6 from -0.62 to 0.73. This result indicated that the reaction pathway for NOx reduction was hardly changed by the introduction of water vapor, while a poisoning effect related to C3H6 oxidation was decreased. In situ DRIFTS studies and DFT calculations revealed that water vapor significantly inhibits the formation of inert formate during the H2-C3H6-SCR process, and thus more sites are available for the formation of active enolic species and acetates, finally leading to increased activity for 2 wt% Ag/Al2O3 in NOx reduction. (C) 2017 Elsevier B.V. All rights reserved.
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