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İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi

Year 2021, Volume: 36 Issue: 2, 1075 - 1088, 05.03.2021
https://doi.org/10.17341/gazimmfd.678990

Abstract

Önemli bir hammadde olan izobütene her geçen gün talebin artması, izobütan dehidrojenasyonunu dikkat çekici bir konuma getirmiştir. Endotermik denge limitasyonlu bu reaksiyon için katalizör sentezi son derece önemlidir. Cr temelli katalizörler için monokromatların en aktif tür olduğu bilinmektedir. Bu çalışmada, Cr içeriğinin Cr@MCM-41 katalizör yapısına, kromat türleri ve miktarları üzerine etkilerinin araştırılması amaçlanmıştır. Bu amaçla, öncelikle katalizör desteği MCM-41 hidrotermal olarak sentezlenmiş, ardından farklı % kütle oranlarında xCr@MCM-41 (x:4,6,8,10) katalizörleri emdirme tekniği ile hazırlanmıştır. Sentezlenen katalizörlerin, XRD, DR-UV vis, XPS, N2 ads./des. analizleri ile karakterizasyon çalışmaları yürütülmüştür. Cr içeriği arttıkça izobütan dehidrojenasyonu için aktivitesi düşük Cr2O3 kristal oluşumların katalizör yapısında arttığı belirlenmiştir. Reaksiyon için aktif monokromat türü en yüksek oranda 4Cr@MCM-41 katalizörü üzerinde elde edilmiş, kristal oluşumların sadece bu katalizör yapısında gözlenmediği tespit edilmiştir. 4Cr@MCM-41 üzerinde yürütülen katalitik testler(600oC, atmosferik) sonucunda 60. dakikaya kadar yüksek izobütan dönüşümleri(%80), 40. dakika sonrası ise yüksek izobüten seçicilikleri(%95) elde edilmiştir. Emdirme tekniği ile sentezlenen xCr@MCM-41 katalizörleri için kütlece %4 Cr içeriğinin, yüksek izobüten seçiciliği ve yüksek miktarda monokromat oluşumu açısından uygun bir oran olduğu görülmektedir.

Supporting Institution

Gazi Üniversitesi Bilimsel Araştırma Projeleri Birimi

Project Number

06/2014-03

Thanks

06 / 2014-03 projesi ile çalışmalarımızı destekleyen Gazi Üniversitesi Bilimsel Araştırma Projeleri Birimi'ne ve fizikorpsiyon analizine yardımcı olduğu için Dr. Dilşad Dolunay Eslek Koyuncu' ya teşekkür ediyoruz.

References

  • 1. Chen, M., Zhao H., Yang J., Zhao J., Chou L., The catalytic dehydrogenation of isobutane and the stability enhancement over Fe incorporated SBA-15, Microporous and Mesoporous Materials, 266, 117-125, 2018. 2. Tian Y., Liu X., Rood M. J., Yan Z., Study of coke deposited on a VOx-K2O/γ-Al2O3 catalyst in the non-oxidative dehydrogenation of isobutane, Applied Catalysis A: General, 545, 1-9, 2017. 3. Dong A., Wang K., Zhu S. Yang G., Wan, X., Facile Preparation of PtSn-La/Al2O3 Catalyst with large pore size and its improved catalytic performance for isobutane dehydrogenation, Fuel Processing Technology, 158, 218-225, 2017. 4. Kraemer S., Rondinone A. J., Tsai Y., Schwartz V., Wu Z., Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes, Catalysis Today, 263, 84-90, 2016. 5. Fridman V.Z, Xing R., Investigating the CrOx/Al2O3 dehydrogenation catalyst model: II. Relative activity of the chromium species on the catalyst surface, Applied Catalysis A: General, 530, 154-165, 2017. 6. Fridman V.Z, Xing R., Severance M., Investigating the CrOx/Al2O3 dehydrogenation catalyst model: I. identification and stability evaluation of the Cr species on the fresh and equilibrated catalysts, Applied Catalysis A: General, 523, 39-53, 2016. 7. Li P., Lang W., Xia K., Luan L. Guo Y., The promotion effects of Ni on the properties of Cr/Al catalysts for propane dehydrogenation reaction, Applied Catalysis A: General, 522, 172-179, 2016. 8. Salaeva A.A., Salaev M.A., Vodyankina O. V., Mamontov G. V., Synergistic effect of Cu and Zn modifiers on the activity of CrOx/Al2O3 catalysts in isobutane dehydrogenation, Applied Catalysis A: General, 581, 82-90, 2019. 9. Kim T. H., Kang K. H., Baek M., Song J. H., Hong U.G., Park Choi W.C., Park Y., Song I.K., Dehydrogenation of propane to propylene eith lattice oxygen over CrOy/Al2O3-ZrO2 Catalysts. Molecular Catalysis, 433, 1-7, 2017. 10. Gao X., Lu W., Hu S., Li W., Lu A., Rod-shaped porous alumina-supported Cr2O3 catalyst with low acidity for propane dehydrogenation, Chinese Journal of Catalysis, 40(2), 184-191, 2019. 11. Zhao H., Song H., Miao Z., Chou L., Isobutane dehydrogenation over chromia alumina catalysts prepared from MIL-101: Insight into chromium species on activity and selectivity, Journal of Energy Chemistry, 23(6),708-716, 2014. 12. Nemykina E.I., Pakhomov N.A., Danilevich V.V., Rogov V.A., Zaikovskii V.I., Larina T.V., Molchanov V.V., Effect of chromium content on the properties of a microspherical alümina-chromium catalyst for ısobutane dehydrogenation prepared with the use of a centrifugal thermal activation product of gibbsite, Kinetics and Catalysis, 51 (6), 898-906, 2010. 13. Baronskiy M.G., Kostyukov A.I., Larina T.V., Snytnikov V.N., Zhuzhgov, A.V., Photoluminescence of surface chromium centers in the Cr/Al2O3 system that is active in isobutane dehydrogenation, Materials Chemistry and Physics, 234, 403-410, 2019. 14. Li L., Zhu W., Shi L., Liu Y., Liu H., Ni Y., Liu S., Zhau H., Liu Z., The effect of ethanol on the performance of CrOx/SiO2 catalysts during propane dehydrogenation, Chinese Journal of Catalysis, 37, 3, 359-366, 2016. 15. Deng J., Zhang L., Liu C., Xia Y., Dai H., Single-crystalline mesoporous CaO supported Cr–V binary oxides: Highly active catalysts for the oxidative dehydrogenation of isobutane, Catalysis Today, 164(1), 347-352, 2011. 16. Asghari E., Haghighi M., Rahmani F, CO2- Oxidative dehydrogenation of ethane to ethylene over Cr/MCM-41 nanocatalyst synthesized via hydrothermal/impregnation methods: Influence of chromium content on catalytic properties and performance, Journal of Molecular Catalysis A: Chemical, 418-419, 115-124, 2016. 17.Ajayi B.P., Jermy B.R., Ogunronbi K.E., Abussaud B.A., Al-Khattaf S., N-butane dehydrogenation over mono and bimetallic MCM-41 catalysts under oxygen free atmosphere, Catalysis Today, 204, 189-196, 2013. 18. Kilicarslan S., Dogan M., Dogu, T., Cr Incorporated MCM-41 Type Catalysts for Isobutane Dehydrogenation and Deactivation Mechanism, Industrial & Engineering Chemistry Research, 52 (10), 3674-3682, 2013. 19. Kilicarslan S., Dogan M., Dogu T., Synthesis and characterization of Ca-Cr-MCM-41 catalysts for isobutane dehydrogenation, Journal of The Faculty of Engineering and Architecture of Gazi University,, 29 (3), 459-467, 2014. 20. Cheng Y., Zhou L., Xu J., Miao C., Gao Z., Chromium-based catalysts for ethane dehydrogenation: Effect of SBA-15 support, Microporous and Mesoporous Materials, 234, 370-376, 2016. 21. Al-Awadi A.. S., El-Toni A. M., Al-Zahrani S. M., Abasaeed A. E., Al-Fatesh A., Role of TiO2 nanoparticle modification of Cr/MCM41 catalyst to enhance Cr-support interaction for oxidative dehydrogenation of ethane with carbon dioxide, Applied Catalysis A: General, 584, 117114, 2019.
Year 2021, Volume: 36 Issue: 2, 1075 - 1088, 05.03.2021
https://doi.org/10.17341/gazimmfd.678990

Abstract

Project Number

06/2014-03

References

  • 1. Chen, M., Zhao H., Yang J., Zhao J., Chou L., The catalytic dehydrogenation of isobutane and the stability enhancement over Fe incorporated SBA-15, Microporous and Mesoporous Materials, 266, 117-125, 2018. 2. Tian Y., Liu X., Rood M. J., Yan Z., Study of coke deposited on a VOx-K2O/γ-Al2O3 catalyst in the non-oxidative dehydrogenation of isobutane, Applied Catalysis A: General, 545, 1-9, 2017. 3. Dong A., Wang K., Zhu S. Yang G., Wan, X., Facile Preparation of PtSn-La/Al2O3 Catalyst with large pore size and its improved catalytic performance for isobutane dehydrogenation, Fuel Processing Technology, 158, 218-225, 2017. 4. Kraemer S., Rondinone A. J., Tsai Y., Schwartz V., Wu Z., Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes, Catalysis Today, 263, 84-90, 2016. 5. Fridman V.Z, Xing R., Investigating the CrOx/Al2O3 dehydrogenation catalyst model: II. Relative activity of the chromium species on the catalyst surface, Applied Catalysis A: General, 530, 154-165, 2017. 6. Fridman V.Z, Xing R., Severance M., Investigating the CrOx/Al2O3 dehydrogenation catalyst model: I. identification and stability evaluation of the Cr species on the fresh and equilibrated catalysts, Applied Catalysis A: General, 523, 39-53, 2016. 7. Li P., Lang W., Xia K., Luan L. Guo Y., The promotion effects of Ni on the properties of Cr/Al catalysts for propane dehydrogenation reaction, Applied Catalysis A: General, 522, 172-179, 2016. 8. Salaeva A.A., Salaev M.A., Vodyankina O. V., Mamontov G. V., Synergistic effect of Cu and Zn modifiers on the activity of CrOx/Al2O3 catalysts in isobutane dehydrogenation, Applied Catalysis A: General, 581, 82-90, 2019. 9. Kim T. H., Kang K. H., Baek M., Song J. H., Hong U.G., Park Choi W.C., Park Y., Song I.K., Dehydrogenation of propane to propylene eith lattice oxygen over CrOy/Al2O3-ZrO2 Catalysts. Molecular Catalysis, 433, 1-7, 2017. 10. Gao X., Lu W., Hu S., Li W., Lu A., Rod-shaped porous alumina-supported Cr2O3 catalyst with low acidity for propane dehydrogenation, Chinese Journal of Catalysis, 40(2), 184-191, 2019. 11. Zhao H., Song H., Miao Z., Chou L., Isobutane dehydrogenation over chromia alumina catalysts prepared from MIL-101: Insight into chromium species on activity and selectivity, Journal of Energy Chemistry, 23(6),708-716, 2014. 12. Nemykina E.I., Pakhomov N.A., Danilevich V.V., Rogov V.A., Zaikovskii V.I., Larina T.V., Molchanov V.V., Effect of chromium content on the properties of a microspherical alümina-chromium catalyst for ısobutane dehydrogenation prepared with the use of a centrifugal thermal activation product of gibbsite, Kinetics and Catalysis, 51 (6), 898-906, 2010. 13. Baronskiy M.G., Kostyukov A.I., Larina T.V., Snytnikov V.N., Zhuzhgov, A.V., Photoluminescence of surface chromium centers in the Cr/Al2O3 system that is active in isobutane dehydrogenation, Materials Chemistry and Physics, 234, 403-410, 2019. 14. Li L., Zhu W., Shi L., Liu Y., Liu H., Ni Y., Liu S., Zhau H., Liu Z., The effect of ethanol on the performance of CrOx/SiO2 catalysts during propane dehydrogenation, Chinese Journal of Catalysis, 37, 3, 359-366, 2016. 15. Deng J., Zhang L., Liu C., Xia Y., Dai H., Single-crystalline mesoporous CaO supported Cr–V binary oxides: Highly active catalysts for the oxidative dehydrogenation of isobutane, Catalysis Today, 164(1), 347-352, 2011. 16. Asghari E., Haghighi M., Rahmani F, CO2- Oxidative dehydrogenation of ethane to ethylene over Cr/MCM-41 nanocatalyst synthesized via hydrothermal/impregnation methods: Influence of chromium content on catalytic properties and performance, Journal of Molecular Catalysis A: Chemical, 418-419, 115-124, 2016. 17.Ajayi B.P., Jermy B.R., Ogunronbi K.E., Abussaud B.A., Al-Khattaf S., N-butane dehydrogenation over mono and bimetallic MCM-41 catalysts under oxygen free atmosphere, Catalysis Today, 204, 189-196, 2013. 18. Kilicarslan S., Dogan M., Dogu, T., Cr Incorporated MCM-41 Type Catalysts for Isobutane Dehydrogenation and Deactivation Mechanism, Industrial & Engineering Chemistry Research, 52 (10), 3674-3682, 2013. 19. Kilicarslan S., Dogan M., Dogu T., Synthesis and characterization of Ca-Cr-MCM-41 catalysts for isobutane dehydrogenation, Journal of The Faculty of Engineering and Architecture of Gazi University,, 29 (3), 459-467, 2014. 20. Cheng Y., Zhou L., Xu J., Miao C., Gao Z., Chromium-based catalysts for ethane dehydrogenation: Effect of SBA-15 support, Microporous and Mesoporous Materials, 234, 370-376, 2016. 21. Al-Awadi A.. S., El-Toni A. M., Al-Zahrani S. M., Abasaeed A. E., Al-Fatesh A., Role of TiO2 nanoparticle modification of Cr/MCM41 catalyst to enhance Cr-support interaction for oxidative dehydrogenation of ethane with carbon dioxide, Applied Catalysis A: General, 584, 117114, 2019.
There are 1 citations in total.

Details

Primary Language Turkish
Subjects Architecture
Journal Section Makaleler
Authors

Saliha Çetinyokuş 0000-0001-9955-6428

Meltem Dogan 0000-0002-5903-2600

Project Number 06/2014-03
Publication Date March 5, 2021
Submission Date January 23, 2020
Acceptance Date November 23, 2020
Published in Issue Year 2021 Volume: 36 Issue: 2

Cite

APA Çetinyokuş, S., & Dogan, M. (2021). İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, 36(2), 1075-1088. https://doi.org/10.17341/gazimmfd.678990
AMA Çetinyokuş S, Dogan M. İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi. GUMMFD. March 2021;36(2):1075-1088. doi:10.17341/gazimmfd.678990
Chicago Çetinyokuş, Saliha, and Meltem Dogan. “İzobütan Dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin Incelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 36, no. 2 (March 2021): 1075-88. https://doi.org/10.17341/gazimmfd.678990.
EndNote Çetinyokuş S, Dogan M (March 1, 2021) İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 36 2 1075–1088.
IEEE S. Çetinyokuş and M. Dogan, “İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi”, GUMMFD, vol. 36, no. 2, pp. 1075–1088, 2021, doi: 10.17341/gazimmfd.678990.
ISNAD Çetinyokuş, Saliha - Dogan, Meltem. “İzobütan Dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin Incelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi 36/2 (March 2021), 1075-1088. https://doi.org/10.17341/gazimmfd.678990.
JAMA Çetinyokuş S, Dogan M. İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi. GUMMFD. 2021;36:1075–1088.
MLA Çetinyokuş, Saliha and Meltem Dogan. “İzobütan Dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin Incelenmesi”. Gazi Üniversitesi Mühendislik Mimarlık Fakültesi Dergisi, vol. 36, no. 2, 2021, pp. 1075-88, doi:10.17341/gazimmfd.678990.
Vancouver Çetinyokuş S, Dogan M. İzobütan dehidrojenasyonunda Cr@MCM-41 katalizörlerinin etkinliğinin incelenmesi. GUMMFD. 2021;36(2):1075-88.