A promising catalyst for catalytic oxidation of chlorobenzene and slipped ammonia in SCR exhaust gas: Investigating the simultaneous removal mechanism
[Display omitted] •The competition adsorption mechanism of NH3 and CB at low temperature is revealed.•Byproduct of NH3-SCO promotes deep oxidation of intermediates in CBCO reaction.•The forms of N and Cl species in simultaneous catalytic oxidation are unveiled. As the emission limits for NOx become...
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Veröffentlicht in: | Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2023-10, Vol.473, p.145106, Article 145106 |
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Sprache: | eng |
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•The competition adsorption mechanism of NH3 and CB at low temperature is revealed.•Byproduct of NH3-SCO promotes deep oxidation of intermediates in CBCO reaction.•The forms of N and Cl species in simultaneous catalytic oxidation are unveiled.
As the emission limits for NOx become further stringent, development of a synergistic control technology to prevent emissions of slipped ammonia (NH3) and chlorinated organics from steel production and waste incineration is both a prospect and a challenge for the environmental issues. In this work, the designed ruthenium-based catalyst (RuNb/ST) showed the excellent chlorobenzene (CB)/NH3 synergistic removal performance and N2/CO2 selectivity above 300 ℃. The activity of NH3 and CB were suppressed at relatively low temperature due to the competitive adsorption of CB and NH3. Whereas, there was a significant improvement in the N2/CO2 selectivity at relatively high temperature. The removal mechanism was studied by experiments, in which the accumulation of chlorine species, the role of NO2 and the oxidation of CB were considerable. In contrast to the carrier, the vast majority of the chloride ions adsorbed onto the active sites after dissociating from CB could be efficiently removed in form of Cl2 via the Deacon Reaction catalyzed by RuO2. CB was predominantly converted into CO2 and H2O with a fraction persisting as organics. Partial of organics were attacked by Cl ions to generate organic chlorine-containing by-products. The presence of NO2 molecule was found to promote the cleavage of the benzene ring within CB, and expedited the carbon migration towards the ultimate product of CO2, resulting in a notable reduction of byproducts. |
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ISSN: | 1385-8947 1873-3212 |
DOI: | 10.1016/j.cej.2023.145106 |