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DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU

Year 2009, Volume: 24 Issue: 2, 0 - , 14.02.2013

Yeşim Güçbilmez

Abstract

Çalışma kapsamında silika bazlı Fe-MCM-48 katalizörleri doğrudan hidrotermal sentez (Fe-MCM-48-1) ve yaş
emdirme (Fe-MCM-48-2) metotlarıyla, desteksiz Fe-Mo-O katalizörü ise birlikte çöktürme metodu ile
üretilmiştir. AAS, XRD ve BET sonuçları hidrotermal sentez metodu ile katalizöre yüksek oranda (Fe/Si(katı) =
0,56) demir eklenebildiğini ancak MCM-48 yapısının bozulduğunu, yapıda önemli ölçüde Fe2O3 fazı oluştuğunu
ve BET yüzey alanının düşük olduğunu (214 m2/g) göstermiştir. Yaş emdirme metodu ile MCM-48 yapısına
demir eklendiğinde ise AAS, XRD ve BET sonuçları hidrotermal senteze oranla daha düşük miktarda demir
eklendiğini (Fe/Si(katı) = 0,12) ancak MCM-48’in kübik gözenekli yapısının korunduğunu ve BET yüzey
alanının çok yüksek olduğunu (982 m2/g) göstermiştir. Fe-Mo-O katalizörü için karakterizasyon sonuçları ise
katalizörün düzenli kristal yapıda olduğunu, Fe2(Mo4O)3 ve MoO3 fazlarını içerdiğini ancak silika destekli
katalizörlere oranla çok düşük yüzey alanına (12 m2/g) sahip olduğunu göstermiştir. Fe-MCM-48-1 ve Fe-Mo-O
katalizörlerinin gözenek dağılımlarının homojen olmadığı, Fe-MCM-48-2 katalizörünün ise 2,8 nm civarında
homojen mezo gözenek dağılımına sahip olduğu görülmüştür.

Keywords

MCM-48 Fe-MCM-48 Fe-Mo-O hidrotermal sentez yaş emdirme birlikte çöktürme.

References

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  • Concentrated Gases”, J. Catal., Cilt 193, No 2,
  • -254, 2000.
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  • Coluccia, S., Frusteri, F., Spadaro, L. ve
  • Parmaliana, A., “Activity pattern of low-loaded
  • FeOx/SiO2 catalysts in the selective oxidation of
  • C1 and C3 alkanes with oxygen”, Catal. Today,
  • Cilt 117, No 1-3, 75-79, 2006.
  • Zhao, W., Luo, Y., Deng, P. ve Li, Q., “Synthesis
  • of Fe-MCM-48 and its catalytic performance in
  • phenol hydroxylation”, Catal. Lett., Cilt 73, No
  • -4, 199-202, 2001.
  • House, M.P., Carley, A.F. ve Bowker, M.,
  • “Selective oxidation of methanol on iron
  • molybdate catalysts effects of surface reduction”,
  • J. Catal., Cilt 252, No 1, 88-96, 2007.
  • Dias, A.P.S., Rozanov, V.V., Waerenborgh,
  • J.C.B. ve Portela, M.F., “New Mo-Fe-O silica
  • supported catalysts for methanol to formaldehyde
  • oxidation”, App. Catal. A: Gen., Cilt 345, No 2,
  • -194, 2008.
  • Soares, A.P.V., Portela, M.F. ve Kiennemann, A.,
  • “Methanol selective oxidation to formaldehyde
  • over iron molybdate catalysts”, Catal. Rev., Cilt
  • , No 1, 2005.
  • Soares, A.P.V., Portela, M.F., Kiennemann, A. ve
  • Hilaire, L., “Mechanism of deactivation of ironmolybdate
  • catalysts prepared by coprecipitation
  • and sol–gel techniques in methanol to
  • formaldehyde oxidation”, Chem. Eng. Sci., Cilt
  • , No 7, 1315-1322, 2003.
  • Soares, A.P.V., Portela, M.F., Kiennemann, A.,
  • Hilaire, L. ve Millet, J.M.M., “Iron molybdate catalysts for methanol to formaldehyde oxidation:
  • Effects of Mo excess on catalytic behaviour”,
  • App. Catal. A: Gen., Cilt 206, No 2, 221-229,
  • -
  • Beck, J.S, Vartuli, J.C., Roth, W.J., Leonowicz,
  • M.E., Kresge, C.T., Schmitt, K.D., Chu, C. T.
  • W., Olson, D.H. ve Sheppard, E. W., “A new
  • family of mesoporous molecular sieves prepared
  • with liquid crystal templates”, J. Am. Chem.
  • Soc., Cilt 114, No 27, 10834–10843, 1992.
  • Oye G., Sjöblom J. ve Stöcker M., “Synthesis,
  • characterization and potential applications of new
  • materials in the mesoporous range”, Adv. Coll.
  • Int. Sci., Cilt 89-90, 439-466, 2001.
  • Zhao, W., Hao, Z. ve Hu, C., “Synthesis of
  • MCM-48 with a high thermal and hydro-thermal
  • stability”, Mater.Res. Bull., Cilt 40, No 10,
  • -1780, 2005.
  • Wang, L., Shao, Y., Zhang, J. ve Masakazu A.,
  • “Synthesis of MCM-48 mesoporous molecular
  • sieve with thermal and hydrothermal stability
  • with the aid of promoter anions”, Micropor.
  • Mesopor. Mater., Cilt 95, No 1-3, 17-25, 2006.
  • Kong, L., Liu,S., Yan, X., Li, Q. ve He H.,
  • “Synthesis of hollow-shell MCM-48 using the
  • ternary surfactant templating method”,
  • Micropor. and Mesopor. Mater., Cilt 81, No 1-
  • , 251-257, 2005.
  • Fröba, M., Köhn, R. ve Bouffaud, G., “Fe2O3
  • nanoparticles within mesoporous MCM-48 silica:
  • In situ formation and characterization”, Chem.
  • Mater., Cilt 11, No 10, 2858-286, 1999.
  • Köhn, R. ve Fröba, M., “Nanoparticles of 3d
  • transition metal oxides in mesoporous MCM-48
  • silica host structures: Synthesis and characterization”,
  • Catal. Today, Cilt 68, 227–236, 2001.
  • Zhao, W., Kong, L., Luo, Y. ve Li, Q., “Study of
  • the influence factors on the synthesis of Fe-
  • MCM-48 with binary mixed cationic and anionic
  • surfactants”, Micropor. Mesopor. Mater., Cilt
  • , No1-3, 111-117, 2007.
  • Echchahed,B., Moen,A., Nicholson,D. ve
  • Bonneviot, L., “Iron-Modified MCM-48
  • mesoporous molecular sieves”, Chem. Mater.,
  • Cilt 9, No 8, 1716–1719, 1997.
  • Shao,Y., Wang, L., Zhang, J. ve Anpo, M.,
  • “Synthesis of hydrothermally stable and longrange
  • ordered Ce-MCM-48 and Fe-MCM-48
  • materials”, J. Phys. Chem. B, Cilt 109, No 44,
  • -20841, 2005.
  • Kosslick, H., Lischke, G., Landmesser, H.,
  • Parlitza, B., Storek, W. and Fricke, R., “Acidity
  • and catalytic behavior of substituted MCM-48”,
  • J. Catal., Cilt 176, No 1, 102-114, 1998.
  • Subramarian, H. ve Koodali, R.T., “Baeyer-
  • Villiger oxidation of cyclic ketones over ironcontaining
  • mesoporous MCM-48 silica
  • materials”, Reaction Kinetics and Catalysis
  • Letters, Cilt 95, No 2, 239 -245, 2008.
  • Subrahmanyam, H., Viswanathan, B. ve
  • aradarajan, T.K., “Synthesis, characterization and
  • catalytic activity of mesoporous trivalent iron
  • substituted aluminophosphates”, J. Mol. Catal.
  • A Chem., Cilt 223, No 1-2, 149–153, 2004.
  • Trejda, M., Kujawa, J. ve Ziolek, M., “Iron
  • modified MCM-41 materials characterised by
  • methanol oxidation and sulphurisation reactions”,
  • Catal. Lett., Cilt 108, No 3–4, 141-146, 2006.
  • Wang, C.T. ve Ro, S-H, “Nanocluster iron oxidesilica
  • aerogel catalysts for methanol partial
  • oxidation”, App. Cat. A: Gen., Cilt 285, No 1-2,
  • -204, 2005.
  • Wang, C.T. ve Willey, R.J, “Mechanistic aspects
  • of methanol partial oxidation over supported iron
  • oxide aerogels”, J.Catal., Cilt 202, No 2, 211-
  • , 2001.
  • Tsoncheva, T., Rosenholm, J., Linden, M.,
  • Kleitz, F., Tiemann, M., Ivanova, L., Dimitrova,
  • M., Paneva, D., Mitov, I. ve Mincheva, C.,
  • “Critical evaluation of the state of iron oxide
  • nanoparticles on different mesoporous silicas
  • prepared by an impregnation method”,
  • Micropor. Mesopor. Mater., Cilt 112, No 1-3,
  • -337, 2008.
  • Michal Kruk, Mietek Jaroniec, Ryoo, R. ve Joo,
  • S.H., “Characterization of ordered mesoporous
  • carbons synthesized using MCM-48 silicas as
  • templates”, J. Phys. Chem. B, Cilt 104, 7960-
  • , 2000.
  • Ravikovitch, P. I. ve Neimark, A. V., Langmuir,
  • Cilt 16, No 6, 2419-2423, 2000.
  • Wang X., Jia, J., Zhao, L. ve Sun, T.,
  • “Mesoporous SBA-15 supported iron oxide: A
  • potent catalyst for Hydrogen Sulfide Removal”,
  • Water, Air and Soil Pollution, Cilt 193, No 1,
  • -257, 2008.
  • Sun-Kou, M.R., Mendioroz, S., Fierro, J.L.G.,
  • Palacios, J.M. ve Guerrero-Ruiz, R.A., “Influence
  • of the preparation method on the behaviour of Fe-
  • Mo catalysts for the oxidation of methanol”, J.
  • Mater. Sci., Cilt 30, No 2, 496-503, 1995.
  • Lowell, S. ve Shields J.E., Powder Surface Area
  • and Porosity, Second Edition, Chapman and Hall,
  • London,GreatBritian,1984.

Year 2009, Volume: 24 Issue: 2, 0 - , 14.02.2013

Yeşim Güçbilmez

Abstract

References

  • Wingen A., Anastasievic N., Hollnagel A.,
  • Werner D. ve Schuth F., “Fe-MCM-41 as a
  • Catalyst for Sulfur Dioxide Oxidation in Highly
  • Concentrated Gases”, J. Catal., Cilt 193, No 2,
  • -254, 2000.
  • Arena, A., Gatti, G., Stievano, L., Martra, G.,
  • Coluccia, S., Frusteri, F., Spadaro, L. ve
  • Parmaliana, A., “Activity pattern of low-loaded
  • FeOx/SiO2 catalysts in the selective oxidation of
  • C1 and C3 alkanes with oxygen”, Catal. Today,
  • Cilt 117, No 1-3, 75-79, 2006.
  • Zhao, W., Luo, Y., Deng, P. ve Li, Q., “Synthesis
  • of Fe-MCM-48 and its catalytic performance in
  • phenol hydroxylation”, Catal. Lett., Cilt 73, No
  • -4, 199-202, 2001.
  • House, M.P., Carley, A.F. ve Bowker, M.,
  • “Selective oxidation of methanol on iron
  • molybdate catalysts effects of surface reduction”,
  • J. Catal., Cilt 252, No 1, 88-96, 2007.
  • Dias, A.P.S., Rozanov, V.V., Waerenborgh,
  • J.C.B. ve Portela, M.F., “New Mo-Fe-O silica
  • supported catalysts for methanol to formaldehyde
  • oxidation”, App. Catal. A: Gen., Cilt 345, No 2,
  • -194, 2008.
  • Soares, A.P.V., Portela, M.F. ve Kiennemann, A.,
  • “Methanol selective oxidation to formaldehyde
  • over iron molybdate catalysts”, Catal. Rev., Cilt
  • , No 1, 2005.
  • Soares, A.P.V., Portela, M.F., Kiennemann, A. ve
  • Hilaire, L., “Mechanism of deactivation of ironmolybdate
  • catalysts prepared by coprecipitation
  • and sol–gel techniques in methanol to
  • formaldehyde oxidation”, Chem. Eng. Sci., Cilt
  • , No 7, 1315-1322, 2003.
  • Soares, A.P.V., Portela, M.F., Kiennemann, A.,
  • Hilaire, L. ve Millet, J.M.M., “Iron molybdate catalysts for methanol to formaldehyde oxidation:
  • Effects of Mo excess on catalytic behaviour”,
  • App. Catal. A: Gen., Cilt 206, No 2, 221-229,
  • -
  • Beck, J.S, Vartuli, J.C., Roth, W.J., Leonowicz,
  • M.E., Kresge, C.T., Schmitt, K.D., Chu, C. T.
  • W., Olson, D.H. ve Sheppard, E. W., “A new
  • family of mesoporous molecular sieves prepared
  • with liquid crystal templates”, J. Am. Chem.
  • Soc., Cilt 114, No 27, 10834–10843, 1992.
  • Oye G., Sjöblom J. ve Stöcker M., “Synthesis,
  • characterization and potential applications of new
  • materials in the mesoporous range”, Adv. Coll.
  • Int. Sci., Cilt 89-90, 439-466, 2001.
  • Zhao, W., Hao, Z. ve Hu, C., “Synthesis of
  • MCM-48 with a high thermal and hydro-thermal
  • stability”, Mater.Res. Bull., Cilt 40, No 10,
  • -1780, 2005.
  • Wang, L., Shao, Y., Zhang, J. ve Masakazu A.,
  • “Synthesis of MCM-48 mesoporous molecular
  • sieve with thermal and hydrothermal stability
  • with the aid of promoter anions”, Micropor.
  • Mesopor. Mater., Cilt 95, No 1-3, 17-25, 2006.
  • Kong, L., Liu,S., Yan, X., Li, Q. ve He H.,
  • “Synthesis of hollow-shell MCM-48 using the
  • ternary surfactant templating method”,
  • Micropor. and Mesopor. Mater., Cilt 81, No 1-
  • , 251-257, 2005.
  • Fröba, M., Köhn, R. ve Bouffaud, G., “Fe2O3
  • nanoparticles within mesoporous MCM-48 silica:
  • In situ formation and characterization”, Chem.
  • Mater., Cilt 11, No 10, 2858-286, 1999.
  • Köhn, R. ve Fröba, M., “Nanoparticles of 3d
  • transition metal oxides in mesoporous MCM-48
  • silica host structures: Synthesis and characterization”,
  • Catal. Today, Cilt 68, 227–236, 2001.
  • Zhao, W., Kong, L., Luo, Y. ve Li, Q., “Study of
  • the influence factors on the synthesis of Fe-
  • MCM-48 with binary mixed cationic and anionic
  • surfactants”, Micropor. Mesopor. Mater., Cilt
  • , No1-3, 111-117, 2007.
  • Echchahed,B., Moen,A., Nicholson,D. ve
  • Bonneviot, L., “Iron-Modified MCM-48
  • mesoporous molecular sieves”, Chem. Mater.,
  • Cilt 9, No 8, 1716–1719, 1997.
  • Shao,Y., Wang, L., Zhang, J. ve Anpo, M.,
  • “Synthesis of hydrothermally stable and longrange
  • ordered Ce-MCM-48 and Fe-MCM-48
  • materials”, J. Phys. Chem. B, Cilt 109, No 44,
  • -20841, 2005.
  • Kosslick, H., Lischke, G., Landmesser, H.,
  • Parlitza, B., Storek, W. and Fricke, R., “Acidity
  • and catalytic behavior of substituted MCM-48”,
  • J. Catal., Cilt 176, No 1, 102-114, 1998.
  • Subramarian, H. ve Koodali, R.T., “Baeyer-
  • Villiger oxidation of cyclic ketones over ironcontaining
  • mesoporous MCM-48 silica
  • materials”, Reaction Kinetics and Catalysis
  • Letters, Cilt 95, No 2, 239 -245, 2008.
  • Subrahmanyam, H., Viswanathan, B. ve
  • aradarajan, T.K., “Synthesis, characterization and
  • catalytic activity of mesoporous trivalent iron
  • substituted aluminophosphates”, J. Mol. Catal.
  • A Chem., Cilt 223, No 1-2, 149–153, 2004.
  • Trejda, M., Kujawa, J. ve Ziolek, M., “Iron
  • modified MCM-41 materials characterised by
  • methanol oxidation and sulphurisation reactions”,
  • Catal. Lett., Cilt 108, No 3–4, 141-146, 2006.
  • Wang, C.T. ve Ro, S-H, “Nanocluster iron oxidesilica
  • aerogel catalysts for methanol partial
  • oxidation”, App. Cat. A: Gen., Cilt 285, No 1-2,
  • -204, 2005.
  • Wang, C.T. ve Willey, R.J, “Mechanistic aspects
  • of methanol partial oxidation over supported iron
  • oxide aerogels”, J.Catal., Cilt 202, No 2, 211-
  • , 2001.
  • Tsoncheva, T., Rosenholm, J., Linden, M.,
  • Kleitz, F., Tiemann, M., Ivanova, L., Dimitrova,
  • M., Paneva, D., Mitov, I. ve Mincheva, C.,
  • “Critical evaluation of the state of iron oxide
  • nanoparticles on different mesoporous silicas
  • prepared by an impregnation method”,
  • Micropor. Mesopor. Mater., Cilt 112, No 1-3,
  • -337, 2008.
  • Michal Kruk, Mietek Jaroniec, Ryoo, R. ve Joo,
  • S.H., “Characterization of ordered mesoporous
  • carbons synthesized using MCM-48 silicas as
  • templates”, J. Phys. Chem. B, Cilt 104, 7960-
  • , 2000.
  • Ravikovitch, P. I. ve Neimark, A. V., Langmuir,
  • Cilt 16, No 6, 2419-2423, 2000.
  • Wang X., Jia, J., Zhao, L. ve Sun, T.,
  • “Mesoporous SBA-15 supported iron oxide: A
  • potent catalyst for Hydrogen Sulfide Removal”,
  • Water, Air and Soil Pollution, Cilt 193, No 1,
  • -257, 2008.
  • Sun-Kou, M.R., Mendioroz, S., Fierro, J.L.G.,
  • Palacios, J.M. ve Guerrero-Ruiz, R.A., “Influence
  • of the preparation method on the behaviour of Fe-
  • Mo catalysts for the oxidation of methanol”, J.
  • Mater. Sci., Cilt 30, No 2, 496-503, 1995.
  • Lowell, S. ve Shields J.E., Powder Surface Area
  • and Porosity, Second Edition, Chapman and Hall,
  • London,GreatBritian,1984.
There are 139 citations in total.

Details

Primary Language Turkish
Journal Section Makaleler
Authors

Yeşim Güçbilmez This is me

Publication Date February 14, 2013
Submission Date February 14, 2013
Published in Issue Year 2009 Volume: 24 Issue: 2

Cite

APA Güçbilmez, Y. (2013). DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, 24(2).
AMA Güçbilmez Y. DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU. GUMMFD. March 2013;24(2).
Chicago Güçbilmez, Yeşim. “DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 24, no. 2 (March 2013).
EndNote Güçbilmez Y (March 1, 2013) DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 24 2
IEEE Y. Güçbilmez, “DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU”, GUMMFD, vol. 24, no. 2, 2013.
ISNAD Güçbilmez, Yeşim. “DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 24/2 (March 2013).
JAMA Güçbilmez Y. DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU. GUMMFD. 2013;24.
MLA Güçbilmez, Yeşim. “DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, vol. 24, no. 2, 2013.
Vancouver Güçbilmez Y. DEMİR İÇERİKLİ DESTEKLİ VE DESTEKSİZ KATALİZÖR SENTEZİ VE KARAKTERİZASYONU. GUMMFD. 2013;24(2).