Elsevier

Applied Surface Science

Volume 349, 15 September 2015, Pages 21-26
Applied Surface Science

CO oxidation over fiberglasses with doped Cu-Ce-O catalytic layer prepared by surface combustion synthesis

https://doi.org/10.1016/j.apsusc.2015.04.185Get rights and content

Highlights

  • The doped CuO–CeO2 systems supported on fiberglass were prepared by surface combustion synthesis.

  • The preparation method allows one to disperse the additive in the form of crystals with the size less than 20 nm.

  • The dopant interaction with CuO phase plays a key role in catalytic behavior.

Abstract

Surface combustion synthesis was applied as a coating technique to prepare the fiberglass systems with supported oxide layer. Effect of the dopant's nature (Co3O4, Mn3O4) on catalytic activity of the supported copper-ceria samples was studied. Catalyst samples were characterized by various physicochemical methods. Active components exist on surface of support in three different states: large agglomerates; small particles and thin oxide film. The additive is found to be in highly disperse state. Catalytic activity of modified CuO–CeO2 samples has been tested in CO oxidation. It was established that the catalytic performance is to be directly determined by the nature of dopant and the way it interacts with CuO phase.

Introduction

An intensive industrial progress of the last decades has led to the significant increase in volume of gas emissions released in atmosphere. Besides dust and particulate matter, industrial emissions normally comprise carbon monoxide (CO) that causes a particular interest of researchers in the field of search and development of new catalytic technologies for its effective neutralization. Use of the gas-permeable system with supported catalytic layer to be the basic element of the complex equipment could serve as an example of novel approach allowing one to achieve high purification efficiency [1], [2], [3], [4], [5].

The technologies based on ceramic composite membranes have been successfully developing for the market in recent years. As a rule, such membranes are made of a substrate on the basis of alumina (with pore sizes of 10–15 μm and the total porosity of about 0.45) and catalytically active layer [6]. A striking example of effective utilization of such technologies can be found in catalytic soot filters used as a part of neutralization system for diesel engine exhausts. A deposited layer bears the function of the catalyst providing necessary conditions for burning of the collected soot out. The mentioned approach is also successfully applied at the industrial enterprises for oxidation of the CO and hydrocarbons present in gas emissions. Along with membranes, the fiberglass materials and glass fabrics can be used as a permeable substrate. Thus, development of methods to deposit and anchor the nanostructured layer on a surface of a permeable substrate to function as active catalyst in CO oxidation represents practical interest.

It is known that the catalysts on the basis of precious metals (Au, Pt, Pd) possess highest catalytic activity in CO oxidation reaction. However, owing to their high cost and susceptibility to poisons, the scan of alternative systems still remains topical. On the other hand, the catalysts based on mix of certain metal oxides (Co, Cu, Cr, Mn) are characterized with similar catalytic activity and higher resistance to poisoning if compared with those based on precious metals [7], [8], [9], [10].

Distinctive feature of considered CuO–CeO2 system consists in its high activity and selectivity in CO oxidation in comparison with conventional CuO [10], [11]. Redox characteristics are enhanced due to high oxygen conductivity in ceria (ability to keep oxygen atoms and transfer them to the interphase boundary) [11], [12], [13]. Drawback of this system is related to drop of catalytic activity at raised temperatures, which is explained by sintering of active component in supported catalyst. High stability toward CO2 and H2O vapors [13], [14] should be referred to the main advantages of CuO–CeO2 catalysts.

Catalytic performance of CuO–CeO2 system might be improved by its modification with certain component, which is also active in CO oxidation. Various metal oxides could act as such modifying agents. According to literature, high catalytic activity is shown by cobalt oxide [15].

Here we report the results of study on catalytic performance of CuO–CeO2 system doped with cobalt and manganese oxides. Surface combustion synthesis (SCS) was applied to deposit a catalytic layer on a surface of fiberglass substrate [16]. The morphology and phase composition of obtained catalysts were characterized by chemical analysis, XRD, and methods of electronic microscopy (SEM, TEM).

Section snippets

Experimental

Zr-containing siliceous fiberglass fabric (KZT-2) was taken as a substrate due to its high thermal stability (up to 1200 °C), structure and chemical composition close to ceramic membranes used in industry. Prior to SCS procedure, the strips of fiberglass fabric (1.5 cm × 8 cm) were washed out in acetone, dried at 120 °C and calcined at 600 °C (1 h). Catalytic layer was deposited via SCS method using water solutions of precursor salts (Cu(NO3)2, Co(NO3)2, Mn(NO3)3 and Ce(CH3COO)3) and lemon acid as a

Results and discussion

At the initial stage of research the two-component systems were synthesized in order to elucidate the promoting effect of cobalt and manganese oxides. Catalytic performance of synthesized samples in CO oxidation is presented in Fig. 1. It is seen that the activity of sample Co-Ce-O/FG exceeds that corresponding to Cu-Ce system (T50 is 10 °C lower). Light-off curve for the Co-containing sample is characterized by more rapid conversion growth along with temperature. The Mn-containing sample was

Conclusion

The catalytic performance of supported oxide Cu-Ce systems modified with Co and Mn oxides has been studied. It was shown that using SCS procedure to deposit the catalytic layers on a surface of fiberglass fabric permits one to obtain high-disperse oxide particles. When the Cu-Ce system is modified by cobalt oxide, the formation of solid solution with spinel structure (CuxCo3–xO4) takes place. Cerium oxide was found not to form any joint phase in all considered cases; it is represented on a

Acknowledgements

This work was supported by Russian Academy of Sciences and Federal Agency of Scientific Organizations (project #V.45.3.2).

The authors are grateful to T.A. Komnik for her assistance in catalyst testing.

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