期刊
CHEMICAL ENGINEERING JOURNAL
卷 417, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.129013
关键词
Water effect; VOX/TiO2; NH3-SCR; 1,2-dichlorobenzene; Vanadium species; Deactivation
资金
- MINECO/FEDER [CTQ2015-64616-P, BES-2016-077849]
- MINECO [PID2019-107503RB-I00]
- Basque Government [IT657-13, IT1297-19]
- University of the Basque Country, UPV/EHU [INF12/37, UFI 11/39]
- ERDF
- ESF
The study found that water has different effects on the NO reduction and o-DCB oxidation reactions under different conditions, mainly depending on the vanadium species and temperature. At high temperatures, water inhibits side reactions, increasing selectivity towards N2; at low temperatures, water helps to reduce the adsorption of harmful species, improving activity.
VOX/TiO2 catalysts with different vanadium loading were prepared in order to study the influence of vanadium species on the effect of water in the simultaneous NO reduction through NH3-SCR and o-DCB oxidation reactions. The presence of isolated, polymeric and crystalline species and their redox and acid properties were evaluated by N-2-Adsorption, XRD, Raman, H-2-TPR, XPS and NH3-TPD. Water has a bimodal and reversible effect in both NO reduction and o-DCB oxidation depending on vanadium species and temperature. In SCR, water has a detrimental effect at low temperature due to competitive adsorption with NO and NH3, while at high temperature it promotes an increase of NO conversion associated to the suppression of side-reactions, which increase the selectivity towards N-2. In o-DCB oxidation, the effect of water is the sum of two contributions: one positive, related to the removal of surface adsorbed detrimental species; and one negative, associated to the competitive adsorption with o-DCB. Thus, at high temperature water acts as inhibitor, while at low temperature water has a promotional effect in the highly dispersed vanadium catalysts due to their tendency to suffer deactivation, mainly by carbonaceous materials. The presence of water also favors total oxidation and decreases the formation of chlorinated by products.
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