Hostname: page-component-586b7cd67f-2brh9 Total loading time: 0 Render date: 2024-11-24T16:46:46.480Z Has data issue: false hasContentIssue false
  • English
  • Français

Nucleation of the Fe3C in reaction of methane with nanocrystalline iron

Published online by Cambridge University Press:  03 March 2011

U. Narkiewicz ,
W. Arabczyk ,
W. Konicki  and
A. Pattek-Janczyk
U. Narkiewicz*
Affiliation:
Institute of Chemical and Environment Engineering, Technical University of Szczecin, 70-322 Szczecin, Poland
W. Arabczyk
Affiliation:
Institute of Chemical and Environment Engineering, Technical University of Szczecin, 70-322 Szczecin, Poland
W. Konicki
Affiliation:
Institute of Chemical and Environment Engineering, Technical University of Szczecin, 70-322 Szczecin, Poland
A. Pattek-Janczyk
Affiliation:
Faculty of Chemistry, Jagiellonian University, 30-060 Krakow, Poland
*
a) Address all correspondence to this author. e-mail: [email protected]
Get access

Abstract

The carburization process of nanocrystalline iron in a flow of CH4/H2 mixture under atmospheric pressure at 580 °C in a differential reactor–thermobalance was studied. The course of reaction was followed by thermogravimetry, and the phase composition of the samples carburized to different degrees was determined by x-ray diffraction (XRD) and Mössbauer spectroscopy techniques. The XRD method was also used for calculating the mean crystallite size of unconverted iron after reaction at different time intervals. An unexpected relation between the average size of iron crystallites and the degree of conversion was found. The nucleation mechanism of the nanocrystalline iron carbide in the kinetic area of the reaction, limited by the dissociative adsorption of methane, has been suggested. According to this mechanism, iron crystallites are carburized successively, from the smallest to the largest.

Keywords

Chemical reactionCrystal growthGrain size
Type
Articles
Information
Journal of Materials Research , Volume 20 , Issue 2 , February 2005 , pp. 386 - 393
Copyright
Copyright © Materials Research Society 2005

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1.Adamson, A.W. and Gast, A.P.: Physical Chemistry of Surfaces, 6th ed. (Wiley, New York, 1997).Google Scholar
2.Buckley, H.E.: Crystal Growth (Wiley, New York, 1951).Google Scholar
3.Hurth, J.P. and Pound, G.M.: Condensation and Evaporation, Nucleation and Growth Kinetics (McMillan, New York, 1963).Google Scholar
4.Mutaftschiev, B.: The Atomistic Nature of Crystal Growth (Springer-Verlag, Berlin, Heidelberg, New York, 2002).Google Scholar
5.Volmer, M. and Weber, A.: Nucleus formation in supersaturated systems. Z. Phys. Chem. 119, 227 (1926).Google Scholar
6.Becker, R. and Döring, W.: Kinetic treatment of nuclear formation in supersaturated vapors. Ann. Phys. 24, 719 (1935).CrossRefGoogle Scholar
7.Frenkel, I.Ya.: Theory of condensation phenomena. J. Chem. Phys. 1, 200 (1939).CrossRefGoogle Scholar
8.Christian, J.W.: The Theory of Transformations in Metals and Alloys (Pergamon, Amsterdam, Boston, London, New York, Oxford, Paris, San Diego, San Francisco, Singapore, Sydney, Tokyo, 2002).Google Scholar
9.Barret, P.: Heterogeneous kinetics (Gauthier-Villars, Paris, France, 1973), (in French).Google Scholar
10.Orr, W.H.: Oxide Nucleation and Growth. Thesis, Cornell University, Ithaca, NY (1962), Rep. 5.Google Scholar
11.Rhodin, T.N., Orr, W.H. and Walton, D.: Nucleation and Growth of Oxide on Metals. Mémoires Scientifiques Rev. Métallurg. LXII, 67 (1965).Google Scholar
12.Kunze, J.: Nitrogen and carbon in iron and steel-thermodynamics (Akademie-Verlag, Berlin, Germany, 1990).Google Scholar
13.Grabke, H.J. and Martin, E.: Kinetik und Thermodynamik der Aufkohlung von a-Eisen in CH4-H2-Gemischen. Arch Eisenhüttenwes 44, 837 (1973).CrossRefGoogle Scholar
14.Grabke, H.J.: Evidence of the surface concentration of carbon on gamma iron from the kinetics of the carburization in CH4-H2. Metall. Trans. 1, 2972 (1970).CrossRefGoogle Scholar
15.Grabke, H.J.: Kinetics and mechanizm of surface reactions of carburization and decarburization and of nitriding and denitriding of iron in gases. Arch Eisenhüttenwes. 46, 75 1975, (in German).Google Scholar
16.Grabke, H.J., Müller, E.M., Speck, H.V. and Konczos, G.: Kinetics of the carburization of iron alloys in methane-hydrogen mixtures. Steel Res. 56, 275 (1985).CrossRefGoogle Scholar
17.Hirano, S-I. and Tajima, S.: Synthesis and magnetic properties of Fe5C2 by reaction of iron oxide and carbon monoxide. J. Mater. Sci. 25, 4457 (1990).CrossRefGoogle Scholar
18.Tajima, S. and Hirano, S-I.: Synthesis and magnetic properties of Fe7C3 particles with high saturation magnetization. Jpn. J. Appl. Phys. 29, 662 (1990).CrossRefGoogle Scholar
19.Pilipenko, P.S. and Veselov, V.V.: About the possibility of a low-temperature synthesis of the iron-, cobalt-, nickel -carbides by carburization of metals using methane. Poroshkovaia Metallurgija. 6, 9 1975, (in Russian).Google Scholar
20.Mellor, J.W.: A comprehensive treatise on inorganic and theoretical chemistry, Vol. XIII, (Longmans, Green and Co., London, U.K., 1957).Google Scholar
21.Buyanov, R.A., Babenko, V.S., Afanasjev, A.D. and Ostankovich, A.A.: About the mechanism of the cauterization of carbonized precipitates during the regeneration of coke-covered). iron-catalysts. Kinet. Katal. 18, 927 1977, (in Russian).Google Scholar
22.Buyanov, R.A., Chesnokov, V.V., Afanasjev, A.D. and Babenko, V.S.: The carbide mechanism of formation of carbon deposits and their properties on the iron-chromium dehydrogenation catalysts. Kinet. Katal. 18, 1021 1977, (in Russian).Google Scholar
23.Chesnokov, V.V., Buyanov, R.A. and Afanasjev, A.D.: About the carbide-cycle mechanism of the catalysts carburization. Kinet. Katal. 20, 477 1979, (in Russian).Google Scholar
24.Chesnokov, V.V., Buyanov, R.A. and Afanasjev, A.D.: Mechanism of the carbon deposits formation from benzene on iron and nickel. Kinet. Katal. 28, 403 1987, (in Russian).Google Scholar
25.Masaru, T. and Takayuki, I.: Magnetic recording medium. Japanese Patent No. JP1994000152793.Google Scholar
26.Takashi, I. and Kiminori, T.: Magnetic recording medium and its production. Japanese Patent No. JP1993000001872.Google Scholar
27.Arabczyk, W., Ziebro, J., Kałucki, K., Świerkowski, R. and Jakrzewska, M.: Laboratory equipment for continuous fusion of iron catalysts. Chemik. 1, 22 1996, (in Polish).Google Scholar
28.Perego, C. and Peratello, S.: Experimental methods in catalytic kinetics. Catal. Today 52, 133R (1999).CrossRefGoogle Scholar
29.Farrauto, J. and Bartholomew, C.H.: Fundamentals of Industrial Catalytic Processes (Chapman & Hall, London, Weinheim, New York, Tokyo, Victoria, Madras, 1997).Google Scholar
30.Arabczyk, W., Konicki, W., Narkiewicz, U., Jasińska, I. and Kałucki, K.: Kinetics of the Fe3C formation in the reaction of methane with nanocrystalline iron catalyst. Appl. Catal. A: General 266, 135 (2004).CrossRefGoogle Scholar
31.Arabczyk, W., Narkiewicz, U., Konicki, W. and Grzmil, B.: Studies of the kinetics of CH4 decomposition to Fe3C on the promoted iron catalysts. Pol. J. Chem. Technol. 4, 1 (2002).Google Scholar
32.Niemantsverdiet, J.W. and van der Kraan, A.M.: Behavior of metallic iron catalysts during Fischer-Tropsch synthesis studies with Moessbauer spectroscopy, x-ray diffraction, carbon content determination, and reaction kinetic measurements. J. Phys. Chem. 84, 3363 (1980).CrossRefGoogle Scholar
33.Tau, L.M., Borcar, S., Bianchi, D. and Bennett, C.O.: The chemisorption of carbon monoxide on iron/alumina. J. Catal. 87, 36 (1984).CrossRefGoogle Scholar
34.Seth, B.B.L. and Ross, H.U.: The mechanism of iron oxide reduction. Trans. Met. Soc. AIME 233, 180 (1965).Google Scholar
35.Park, J.Y. and Levenspiel, O.: The crackling core model for the reaction on solid particles. Chem. Eng. Sci. 30, 1207 (1975).CrossRefGoogle Scholar
36.Arabczyk, W., Wróbel, R.: A new method of the determination of the crystallites size in the iron catalyst for ammonia synthesis, in EUROPACAT-V, Abstracts, Book 1, 6-P-59 (Limerick, Ireland, 2001).Google Scholar
37.du Plessis, J.: Surface Segregation (Sci-Tech Publications, Brookfield, 1990).CrossRefGoogle Scholar
38.Grabke, H.J.: Adsorption, segregation and reactions of nonmetal atoms on iron surfaces. Mater. Sci. Eng. 42, 91 (1980).CrossRefGoogle Scholar
39.Arabczyk, W. and Narkiewicz, U.: Segregation of carbon in iron and molybdenum. Surf. Sci. 352–354, 223 (1996).CrossRefGoogle Scholar