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Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi

Yıl 2013, Cilt: 28 Sayı: 3, 0 - , 03.03.2014

Öz

Dizel araçlardan çevreye salınan zararlı NOx gazları, seçici katalitik indirgeme (SCR) reaksiyonları ile N2 gazına dönüştürülebilmektedir. Bu reaksiyonların verimi, kullanılan indirgen maddeye önemli ölçüde bağlıdır. Ürenin hem kendisi hem de bozunma/hidroliz bileşikleri olan izosiyanik asit (HNCO) ve amonyak (NH3) SCR reaksiyonlarında kullanılabilmektedir. Bundan dolayı, üre son zamanlarda ilgi çeken bir indirgen maddedir. NOx indirgenmesinde Ag/Al2O3 katalizörleri önemli bir yere sahiptir. Sol-jel yöntemi kullanılarak hazırlanan %1
Ag/Al2O3 ve %2 Ag/Al2O3 katalizörü üzerinde ürenin bozunma ve hidroliz bileşikleri FTIR cihazı kullanılarak incelenmiştir. Deneysel çalışmalar, helyum ortamında 100–400°C sıcaklık aralığında gerçekleştirilmiştir. FTIR spektrumlarının analizi sonucunda katalizörler üzerinde ürenin bozunma ve hidroliz bileşikleri olarak NH3, NH4+, -CNO, melamin ve CO2 tespit edilmiştir. Bunun yanı sıra OH, CH, NH ve C=O gerilme titreşim bantları da gözlenmiştir. NH4+ bileşiği %2 Ag/Al2O3 katalizörü üzerinde 100 ve 250 °C sıcaklıklarda gözlenirken, %1 Ag/Al2O3 katalizörü üzerinde hiçbir sıcaklıkta tespit edilmemiştir. Ürenin bozunma ve hidroliz bileşiği olan amonyak her iki katalizör üzerinde de çalışılan bütün sıcaklık ve zamanlarda gözlenmiştir. Ürenin bozunma bileşiği olan izosiyanat (-CNO), %1 Ag/Al2O3 katalizörü üzerinde en şiddetli pikini 200°C sıcaklıkta, %2 Ag/Al2O3 katalizörü üzerinde 250°C sıcaklıkta vermiştir.

Kaynakça

  • Miyadera, T., ”Alumina-Supported Silver
  • Catalysts for the Selective Reduction of Nitric
  • Oxide with Propene and Oxygen-Containing
  • Organic Compounds”, Applied Catalysis B:
  • Environmental, Cilt 2, No 2-3, 199-205, (993.
  • Bethke, K.A., and Kung, H. H.”Supported Ag
  • Catalysts for the Lean Reduction of NO with
  • C3H6”, Journal of Catalysis, Cilt 72, 93-102,
  • -
  • Ueda, A., Oshima, T., and Haruta, M.,”
  • Reduction of Nitrogen Monoxide with Propene in
  • the Presence of Oxygen and Moisture over Gold
  • Supported on Metal Oxides”, Applied Catalysis
  • B: Environmental , Cilt12, No 2-3, 81-93,
  • -
  • Kramlich, J.C and Linak, W.P. ”Nitrous Oxide
  • Behavior in the Atmosphere, and in Combustion
  • and Industrial Systems”, Progress in Energy
  • and Combustion Science, Cilt 20, No 2, 149–
  • , 1994.
  • Van Kooten, W.E.J, Krijnsen, H.C, Van Den
  • Bleek, C.M, Calis, H.P.A, “Deactivation of
  • Zeolite Catalysts Used for NOx Removal”,
  • Applied Catalysis B: Environmental, Cilt 25,
  • No 2–3, 125–135, 2000.
  • Long, R.Q., Yang, R.T, “Characterization of Fe-
  • ZSM5 Catalyst for Selective Catalytic Reduction
  • Nitric Oxide by Ammonia”, Journal of
  • Catalysis, Cilt 194, 80-90, 2000.
  • Richter, M., Trunschke, A., Bentrup, U.,
  • Brzezinka, K., Schreier, E., Schneider M. , Pohl,
  • M. , Fricke, R. “Selective Catalytic Reduction of
  • NO by Ammonia over Egg-shell MnOx/NaY
  • Composite Catalysts”, Journal of Catalysis, Cilt
  • , 98-113, 2002.
  • Seker, E. , Yasyerli, N. , Gulari, E. , Lambert, C. ,
  • Hammerle, R.H , “NO Reduction by Urea under
  • Lean Conditions over Single Sol-Gel Cu/Alumina
  • Catalyst” , Journal of Catalysis, Cilt 208, 15–20,
  • -
  • He, H., Li, Y., Zhang, X., Yu, Y., Zhang, C., “
  • Precipitable Silver Compound Catalysts for
  • Selective Catalytic Reduction of NOx by
  • Ethanol”, Applied Catalysis A: General, Cilt
  • , 258-264,2010.
  • Dong, H., Shuai, S., Li, R., Wang, J., Shi, X., He,
  • H., “ Study of NOx Selective Catalytic Reduction
  • by Ethanol over Ag/Al2O3 Catalyst on a HD
  • Diesel Engine”, Chemical Engineering Journal,
  • Cilt 135, 195-201,2008.
  • Breen, J.P., Burch, R., Hill, C.J., “ NOx Storage
  • During H2 Assisted Selective Catalytic Reduction
  • of NOx Reaction over a Ag/Al2O3 Catalyst”,
  • Catalysis Today, Cilt 145, 34-37, 2009.
  • Shimizu, K., Satsuma, A., “Hydrogen Assisted
  • Urea-SCR and NH3-SCR with Silver-Alumina as
  • Highly Active and SO2- Tolerant De-NOx
  • Catalysis”, Applied Catalysis B:
  • Environmental, Cilt77, 202-205, 2007.
  • Richter, M., Bentrup, U., Eckelt, R., Schneider
  • M. , Pohl, M.M. , Fricke, R., “ The Effect of
  • Hydrogen on the Selective Catalytic Reduction of
  • NO in Excess Oxygen over Ag/Al2O3”, Applied
  • Catalysis B: Environmental, Cilt 51, 261-274,
  • -
  • Seker, E., Cavataio, J., Gulari, E.,
  • Lorpongpaiboon, P., Osuwan, S., “Nitric Oxide
  • Reduction by Propene over Silver/Alumina and
  • Silver-Gold/Alumina Catalysts: Effect of
  • Preparation Methods”, Applied Catalysis A:
  • General, Cilt 183, 121-134, 1999.
  • Zhang, C., He, H., Shuai, S., Wang, J., “Catalytic
  • Performance of Ag/Al2O3-C2H5OH-Cu/Al2O3
  • System for the Removal of NOx from Diesel
  • Engine Exhaust”, Environmental Pollution, Cilt
  • , 415-421, 2007.
  • Liu, Z., Li, J., Hao, J., “Selective Catalytic
  • Reduction of NOx with Propene over SnO2/Al2O3
  • Catalyst”, Chemical Engineering Journal, Cilt
  • , No 1, 420-425, 2010.
  • Eichelbaum, M., Farrauto, R. J., Castaldi, M.J.,”
  • The Impact of Urea on the Performance of Metal
  • Exchanged Zeolite for the Selective Catalytic
  • Reduction of NOx Part I. Pyrolysis and
  • Hydrolysis of Urea over Zeolite Catalysts”,
  • Applied Catalysis B: Environmental, Cilt 97,
  • No 1, 90-97, 2010.
  • Lundström, A., Snelling, T., Morsing, P.,
  • Gabrielson, P., Senar, E., Olsson, L., “Urea
  • Decomposition and HNCO Hydrolysis Studied
  • over Titanium Oxide, Fe-Beta and γ-Alumina”,
  • Applied Catalysis B: Environmental, Cilt 106,
  • -279, 2011.
  • Bernhard, A.M., Peitz, D., Elsener, M., Wokaun,
  • A., Kröcher, O., “Hydrolysis and Thermolysis of Urea and Its Decomposition Byproducts Biuret,
  • Cyanuric Acid and Melamine over Anatase
  • TiO2”, Applied Catalysis B: Environmental,
  • Cilt 115-116, 129-137, 2012.
  • Şahin, A., Aktan, H., Balbaşı, M., Ar, İ.,
  • “Synthesis and Characterization of Phosphonated
  • Poly(Vinyl Alcohol) Based Membrane with
  • Silica Support” , J. Fac. Eng. Archit. Gazi
  • Univ., Cilt 25, No 4, 693-699, 2010.
  • Şahin, A., Balbaşı, M., Ar, İ., “Synthesis and
  • Characterization of Sulphonated
  • Polystyrene/Polyvinyl Alcohol Composite
  • Membrane with Boric Acid and Boron Phosphate
  • Support” , J. Fac. Eng. Archit. Gazi Univ., Cilt
  • , No 1, 137-144, 2009.
  • Yaşyerli, S., Aktaş, Ö., “MCF Supported V-Mo-
  • Nb Catalysts Prepared by Dırect Hydrothermal
  • Synthesıs and Impregnatıon Methods for
  • Oxıdatıve Dehydrogenatıon of Propane”, J. Fac.
  • Eng. Archit. Gazi Univ., Cilt 27, No 1, 49-58,
  • -
  • Yasyerli, N., Tasdemir, M., “ FTIR Studies of
  • Urea Decomposition over Pt-Alumina and Cu-
  • Alumina Catalysts”, International Journal of
  • Chemical Reactor Engineering, Cilt 8, No 1,
  • A162, 2010.
  • Park, P.W., Boyer, C.L, “Effect of SO2 on the
  • Activity of Ag/γ-Al2O3 Catalysts for NOx
  • Reduction in Lean Conditions”, Applied
  • Catalysis B: Environmental, Cilt 59, No 1-2,
  • -34, 2005.
  • Lowell, S., Shield,J. “Powder Surface Area and
  • Porosity”, Chapman and Hall, New York, A.B.D,
  • -
  • Sing, K.S.W, Haul, R.A.W, Pierotti, R.A.,
  • Siemieniewska, T., “Reporting Physisorption
  • Data for Gas/Solid Systems with Special
  • Reference to the Determination of Surface Area
  • and Porosity”, Pure & App. Chem., Cilt 57, No
  • , 603-619, 1985.
  • Chen, L.F., Gonzalez, G., Wang, J.A, Norena,
  • L.E., Toledo, A., Castillo, S., Pineda, M.M.,
  • “Surfactant Control Synthesis of Pd/Ce0.6Zr0.4O2
  • Catalyst for NO Reduction by CO with Excess
  • Oxygen”, Applied Surface Science, Cilt 243,
  • -328, 2005.
  • Li, Q., Zhao, N., Wei, W., Sun, Y., “Catalytic
  • Performance of Metal Oxide for the Synthesis of
  • Propylene Carbonate from Urea and 1,2
  • Propanediol”, Journal of Moleculer Catalysis
  • A: Chemical, Cilt 270, No 1-2, 44-49, 2007.
  • Li, G., Jones, C.A, Grassian, V.H, Larsen, S.C.,
  • “Selective Catalytic Reduction of NO2 with Urea
  • in Nanocrystalline NaY Zeolite”, Journal of
  • Catalysis, Cilt 234, No 2, 401-413, 2005
  • Seker, E. , Yasyerli, N. , Gulari, E. , Lambert, C. ,
  • Hammerle, R.H , “NOx Reduction by Urea under
  • Lean Conditions over Single Sol-Gel Pt/Alumina
  • Catalyst” , Applied Catalysis B:
  • Environmental, Cilt 37, No 1, 27–35, 2002.
Yıl 2013, Cilt: 28 Sayı: 3, 0 - , 03.03.2014

Öz

Kaynakça

  • Miyadera, T., ”Alumina-Supported Silver
  • Catalysts for the Selective Reduction of Nitric
  • Oxide with Propene and Oxygen-Containing
  • Organic Compounds”, Applied Catalysis B:
  • Environmental, Cilt 2, No 2-3, 199-205, (993.
  • Bethke, K.A., and Kung, H. H.”Supported Ag
  • Catalysts for the Lean Reduction of NO with
  • C3H6”, Journal of Catalysis, Cilt 72, 93-102,
  • -
  • Ueda, A., Oshima, T., and Haruta, M.,”
  • Reduction of Nitrogen Monoxide with Propene in
  • the Presence of Oxygen and Moisture over Gold
  • Supported on Metal Oxides”, Applied Catalysis
  • B: Environmental , Cilt12, No 2-3, 81-93,
  • -
  • Kramlich, J.C and Linak, W.P. ”Nitrous Oxide
  • Behavior in the Atmosphere, and in Combustion
  • and Industrial Systems”, Progress in Energy
  • and Combustion Science, Cilt 20, No 2, 149–
  • , 1994.
  • Van Kooten, W.E.J, Krijnsen, H.C, Van Den
  • Bleek, C.M, Calis, H.P.A, “Deactivation of
  • Zeolite Catalysts Used for NOx Removal”,
  • Applied Catalysis B: Environmental, Cilt 25,
  • No 2–3, 125–135, 2000.
  • Long, R.Q., Yang, R.T, “Characterization of Fe-
  • ZSM5 Catalyst for Selective Catalytic Reduction
  • Nitric Oxide by Ammonia”, Journal of
  • Catalysis, Cilt 194, 80-90, 2000.
  • Richter, M., Trunschke, A., Bentrup, U.,
  • Brzezinka, K., Schreier, E., Schneider M. , Pohl,
  • M. , Fricke, R. “Selective Catalytic Reduction of
  • NO by Ammonia over Egg-shell MnOx/NaY
  • Composite Catalysts”, Journal of Catalysis, Cilt
  • , 98-113, 2002.
  • Seker, E. , Yasyerli, N. , Gulari, E. , Lambert, C. ,
  • Hammerle, R.H , “NO Reduction by Urea under
  • Lean Conditions over Single Sol-Gel Cu/Alumina
  • Catalyst” , Journal of Catalysis, Cilt 208, 15–20,
  • -
  • He, H., Li, Y., Zhang, X., Yu, Y., Zhang, C., “
  • Precipitable Silver Compound Catalysts for
  • Selective Catalytic Reduction of NOx by
  • Ethanol”, Applied Catalysis A: General, Cilt
  • , 258-264,2010.
  • Dong, H., Shuai, S., Li, R., Wang, J., Shi, X., He,
  • H., “ Study of NOx Selective Catalytic Reduction
  • by Ethanol over Ag/Al2O3 Catalyst on a HD
  • Diesel Engine”, Chemical Engineering Journal,
  • Cilt 135, 195-201,2008.
  • Breen, J.P., Burch, R., Hill, C.J., “ NOx Storage
  • During H2 Assisted Selective Catalytic Reduction
  • of NOx Reaction over a Ag/Al2O3 Catalyst”,
  • Catalysis Today, Cilt 145, 34-37, 2009.
  • Shimizu, K., Satsuma, A., “Hydrogen Assisted
  • Urea-SCR and NH3-SCR with Silver-Alumina as
  • Highly Active and SO2- Tolerant De-NOx
  • Catalysis”, Applied Catalysis B:
  • Environmental, Cilt77, 202-205, 2007.
  • Richter, M., Bentrup, U., Eckelt, R., Schneider
  • M. , Pohl, M.M. , Fricke, R., “ The Effect of
  • Hydrogen on the Selective Catalytic Reduction of
  • NO in Excess Oxygen over Ag/Al2O3”, Applied
  • Catalysis B: Environmental, Cilt 51, 261-274,
  • -
  • Seker, E., Cavataio, J., Gulari, E.,
  • Lorpongpaiboon, P., Osuwan, S., “Nitric Oxide
  • Reduction by Propene over Silver/Alumina and
  • Silver-Gold/Alumina Catalysts: Effect of
  • Preparation Methods”, Applied Catalysis A:
  • General, Cilt 183, 121-134, 1999.
  • Zhang, C., He, H., Shuai, S., Wang, J., “Catalytic
  • Performance of Ag/Al2O3-C2H5OH-Cu/Al2O3
  • System for the Removal of NOx from Diesel
  • Engine Exhaust”, Environmental Pollution, Cilt
  • , 415-421, 2007.
  • Liu, Z., Li, J., Hao, J., “Selective Catalytic
  • Reduction of NOx with Propene over SnO2/Al2O3
  • Catalyst”, Chemical Engineering Journal, Cilt
  • , No 1, 420-425, 2010.
  • Eichelbaum, M., Farrauto, R. J., Castaldi, M.J.,”
  • The Impact of Urea on the Performance of Metal
  • Exchanged Zeolite for the Selective Catalytic
  • Reduction of NOx Part I. Pyrolysis and
  • Hydrolysis of Urea over Zeolite Catalysts”,
  • Applied Catalysis B: Environmental, Cilt 97,
  • No 1, 90-97, 2010.
  • Lundström, A., Snelling, T., Morsing, P.,
  • Gabrielson, P., Senar, E., Olsson, L., “Urea
  • Decomposition and HNCO Hydrolysis Studied
  • over Titanium Oxide, Fe-Beta and γ-Alumina”,
  • Applied Catalysis B: Environmental, Cilt 106,
  • -279, 2011.
  • Bernhard, A.M., Peitz, D., Elsener, M., Wokaun,
  • A., Kröcher, O., “Hydrolysis and Thermolysis of Urea and Its Decomposition Byproducts Biuret,
  • Cyanuric Acid and Melamine over Anatase
  • TiO2”, Applied Catalysis B: Environmental,
  • Cilt 115-116, 129-137, 2012.
  • Şahin, A., Aktan, H., Balbaşı, M., Ar, İ.,
  • “Synthesis and Characterization of Phosphonated
  • Poly(Vinyl Alcohol) Based Membrane with
  • Silica Support” , J. Fac. Eng. Archit. Gazi
  • Univ., Cilt 25, No 4, 693-699, 2010.
  • Şahin, A., Balbaşı, M., Ar, İ., “Synthesis and
  • Characterization of Sulphonated
  • Polystyrene/Polyvinyl Alcohol Composite
  • Membrane with Boric Acid and Boron Phosphate
  • Support” , J. Fac. Eng. Archit. Gazi Univ., Cilt
  • , No 1, 137-144, 2009.
  • Yaşyerli, S., Aktaş, Ö., “MCF Supported V-Mo-
  • Nb Catalysts Prepared by Dırect Hydrothermal
  • Synthesıs and Impregnatıon Methods for
  • Oxıdatıve Dehydrogenatıon of Propane”, J. Fac.
  • Eng. Archit. Gazi Univ., Cilt 27, No 1, 49-58,
  • -
  • Yasyerli, N., Tasdemir, M., “ FTIR Studies of
  • Urea Decomposition over Pt-Alumina and Cu-
  • Alumina Catalysts”, International Journal of
  • Chemical Reactor Engineering, Cilt 8, No 1,
  • A162, 2010.
  • Park, P.W., Boyer, C.L, “Effect of SO2 on the
  • Activity of Ag/γ-Al2O3 Catalysts for NOx
  • Reduction in Lean Conditions”, Applied
  • Catalysis B: Environmental, Cilt 59, No 1-2,
  • -34, 2005.
  • Lowell, S., Shield,J. “Powder Surface Area and
  • Porosity”, Chapman and Hall, New York, A.B.D,
  • -
  • Sing, K.S.W, Haul, R.A.W, Pierotti, R.A.,
  • Siemieniewska, T., “Reporting Physisorption
  • Data for Gas/Solid Systems with Special
  • Reference to the Determination of Surface Area
  • and Porosity”, Pure & App. Chem., Cilt 57, No
  • , 603-619, 1985.
  • Chen, L.F., Gonzalez, G., Wang, J.A, Norena,
  • L.E., Toledo, A., Castillo, S., Pineda, M.M.,
  • “Surfactant Control Synthesis of Pd/Ce0.6Zr0.4O2
  • Catalyst for NO Reduction by CO with Excess
  • Oxygen”, Applied Surface Science, Cilt 243,
  • -328, 2005.
  • Li, Q., Zhao, N., Wei, W., Sun, Y., “Catalytic
  • Performance of Metal Oxide for the Synthesis of
  • Propylene Carbonate from Urea and 1,2
  • Propanediol”, Journal of Moleculer Catalysis
  • A: Chemical, Cilt 270, No 1-2, 44-49, 2007.
  • Li, G., Jones, C.A, Grassian, V.H, Larsen, S.C.,
  • “Selective Catalytic Reduction of NO2 with Urea
  • in Nanocrystalline NaY Zeolite”, Journal of
  • Catalysis, Cilt 234, No 2, 401-413, 2005
  • Seker, E. , Yasyerli, N. , Gulari, E. , Lambert, C. ,
  • Hammerle, R.H , “NOx Reduction by Urea under
  • Lean Conditions over Single Sol-Gel Pt/Alumina
  • Catalyst” , Applied Catalysis B:
  • Environmental, Cilt 37, No 1, 27–35, 2002.
Toplam 154 adet kaynakça vardır.

Ayrıntılar

Birincil Dil Türkçe
Bölüm Makaleler
Yazarlar

H. Mehmet Taşdemir Bu kişi benim

Nail Yaşyerli Bu kişi benim

Yayımlanma Tarihi 3 Mart 2014
Gönderilme Tarihi 3 Mart 2014
Yayımlandığı Sayı Yıl 2013 Cilt: 28 Sayı: 3

Kaynak Göster

APA Taşdemir, H. M., & Yaşyerli, N. (2014). Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, 28(3).
AMA Taşdemir HM, Yaşyerli N. Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi. GUMMFD. Mart 2014;28(3).
Chicago Taşdemir, H. Mehmet, ve Nail Yaşyerli. “Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 28, sy. 3 (Mart 2014).
EndNote Taşdemir HM, Yaşyerli N (01 Mart 2014) Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 28 3
IEEE H. M. Taşdemir ve N. Yaşyerli, “Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi”, GUMMFD, c. 28, sy. 3, 2014.
ISNAD Taşdemir, H. Mehmet - Yaşyerli, Nail. “Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 28/3 (Mart 2014).
JAMA Taşdemir HM, Yaşyerli N. Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi. GUMMFD. 2014;28.
MLA Taşdemir, H. Mehmet ve Nail Yaşyerli. “Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, c. 28, sy. 3, 2014.
Vancouver Taşdemir HM, Yaşyerli N. Ag/Alumina Katalizörleri Üzerinde Ürenin Bozunmasının İncelenmesi. GUMMFD. 2014;28(3).