Abstract

Dimethyl disulfide (DMDS, CH3SSCH3) is an odorous and harmful air pollutant (volatile organic compound (VOC)) causing nuisance in urban areas. The abatement of DMDS emissions from industrial sources can be realized through catalytic oxidation. However, the development of active and selective catalysts having good resistance toward sulfur poisoning is required. This paper describes an investigation related to improving the performance of Pt and Cu catalysts through the addition of Au to monometallic “parent” catalysts via surface redox reactions. The catalysts were characterized using ICP-OES, N2 physisorption, XRD, XPS, HR-TEM, H2-TPR, NH3-TPD, CO2-TPD, and temperature-programmed 18O2 isotopic exchange. The performance of the catalysts was evaluated in DMDS total oxidation. In addition, the stability of a Pt–Au/Ce–Al catalyst was investigated through 40 h time onstream. Cu–Au catalysts were observed to be more active than corresponding Pt–Au catalysts based on DMDS light-off experiments. However, the reaction led to a higher amount of oxygen-containing byproduct formation, and thus the Pt–Au catalysts were more selective. H2-TPR showed that the higher redox capacity of the Cu-containing catalysts may have been the reason for better DMDS conversion and lower selectivity. The lower amount of reactive oxygen on the surface of Pt-containing catalysts was beneficial for total oxidation. The improved selectivity of ceria-containing catalysts after the Au addition may have resulted from the lowered amount of reactive oxygen as well. The Au addition improved the activity of Al2O3-supported Cu and Pt. The Au addition also had a positive effect on SO2 production in a higher temperature region. A stability test of 40 h showed that the Pt–Au/Ce–Al catalyst, while otherwise promising, was not stable enough, and further development is still needed.

Highlights

  • Volatile organic compounds (VOCs) are major contributors of direct and indirect air pollution [1]

  • These results suggest that oxygen activation at a lower temperature contributed to a lowtolight-off the dimethyl disulfide (DMDS) oxidation, which led to partial oxidation products

  • The aim of the work was to study if the addition of Au to Pt and Cu supported on Al2 O3, CeO2, and Al2 O3 –CeO2 would improve the performance of the catalysts

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Summary

Introduction

Volatile organic compounds (VOCs) are major contributors of direct (toxicity, ground level photochemical ozone formation) and indirect (smog formation, stratospheric ozone depletion, particulate matter formation) air pollution [1]. Sulfur-containing VOCs (SVOCs) originate from the wood industry, such as from pulping processes and chemical production as well as from landfill sites and wastewater treatment plants. Typical examples of SVOCs are methyl mercaptan (CH3 SH), dimethyl sulfide (CH3 SCH3 ), and dimethyl disulfide (CH3 SSCH3 ) [2], which are disturbingly malodorous, even at very low concentrations, and cause discomfort in urban areas. Catalytic treatment is a suitable abatement technology for VOCs, especially when emission streams are complex and when the total VOC concentrations fluctuate. Catalytic oxidation is an environmentally sound destructive method and is highly feasible economically when heat-recovery-allowing processes such as reverse flow reactors (RFRs) are used. Catalytic oxidation of SVOCs is an attractive possibility: due to the presence of sulfur, the selectivity and stability of the catalysts need to be improved [2]

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