Isomerization of alpha-pinene over superacidic and heteropolyacidic catalysts
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Tarih
2003
Yazarlar
Dergi Başlığı
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Cilt Başlığı
Yayıncı
Ege Üniversitesi
Erişim Hakkı
info:eu-repo/semantics/closedAccess
Özet
ÖZET SÜPERASİDİK VE HETEROPOLİASÎDİK KATALİZÖRLER ÜZERİNDE a-PINEN İZOMERİZASYONU ATALAY, Burcu Yüksek Lisans Tezi, Kimya Mühendisliği Bölümü Tez Danışmanı: Prof. Dr. Gönül GÜNDÜZ Eylül 2003, 162 sayfa Bu çalışmada, süperasidik ve heteropoliasidik katalizörler ile a-pinen izomerizasyon reaksiyonu incelenmiştir. Bu katalizörlere ek olarak, H2SO4 ile muamele edilmiş taşıyıcılar izomerizasyon reaksiyonunda denenmiştir. Doğal zeolit, silikajel ve y-alumina heteropoliasidik katalizörler için taşıyıcı olarak kullanılmıştır. Katı süperasitler, Z1-O2, TİO7 ve Fe203 H2SO4 ile sülfolandmlarak elde edilmişlerdir. Reaksiyon, kesikli bulamaç reaktörde 100°C'lik sabit sıcaklıkta, a-pinen oksidasyonunu önlemek amacı ile, azot ortamında gerçekleştirilmiştir.Hazırlanan katalizörler a-pinenin izomerizasyonreaksiyonunda test edilmiş ve azot adsorpsiyonu, DSC, İR, XRD ve SEM ölçümleri ile karakterize edilmiştir. Katalizörlerin Lewis ve Broensted asit merkezlerin dağılımları belirlenmiş, a-pinen izomerizasyon reaksiyomındaki katalitik aktiviteleri ve ana ürünler olan kamfen ve limonene seçimlilikleri incelenmiştir. Limonen ikincil reaksiyonlarla terpinen, terpilonen gibi maddelere dönüşerek reaksiyona girmeye devam eder. a-pinen tüketim kinetiğinin 1,5. mertebeden olduğu görülmüştür, a-pinen tüketiminin aktivasyon enerjisi 65,4 kJ/mol olarak hesaplanmıştır. Anahtar Sözcükler: a-pinen, izomerizasyon, kamfen, limonen, heteropoliasidik katalizörler, süperasidik katalizörler, doğal zeolit, silikajel, y-alumina, Z1O2, TİO2, Fe2C>3, katalizör karakterizasyonü, reaksiyon kinetiği
VII ABSTRACT ISOMERIZATION OF a-PINENE OVER SUPERACIDIC AND HETEROPOLYACIDIC CATALYSIS AT ALAY, Burcu MSc Thesis, Chemical Engineering Department Supervisor: Prof. Dr. Gönül GÜNDÜZ September 2003, 162 pages In this study, isomerization reaction of a-pinene was studied over super acidic and heteropoly acidic catalysts. In addition to these catalysts H2SO4 treated supports have been tested in the isomerization reaction. Natural zeolite, silicagel and y-alumina have been used as supports for heteropoly acidic catalysis. The solid superacids were obtained by introducing a sulfur compound, H2SO4, to Z1O2, TİO2 and Fe2Û3. Reaction was carried out in a batch slurry reactor with constant temperature of 100°C and under nitrogen atmosphere to prevent oxidation of a pinene. Prepared catalysts were tested in the isomerization reaction of a-pinene and were characterized by nitrogen adsorption experiments, DSC, IR, XRD and SEM measurements. The distribution of Lewis and Broensted acid sites of the catalyst were determined, their catalytic activies in a-pinene isomerization reaction and selectivities tomain reaction products, camphene and limonene, were investigated. Limonene continues to introduce the reaction by converting to terpinenes and terpinolenes as secondary reactions. It was seen that a-pinene consumption could be described by 1,5th order kinetics. Activation energy of a-pinene consumption was calculated to be 65,4 kJ/mol. Keywords: a-pinene, isomerization, camphene, limonene, heteropolyacidic catalysts, superacidic catalysts, natural zeolite, silicagel, y-alumina, ZrC>2, TİO2, Fe203, catalyst characterization, reaction kinetics.
VII ABSTRACT ISOMERIZATION OF a-PINENE OVER SUPERACIDIC AND HETEROPOLYACIDIC CATALYSIS AT ALAY, Burcu MSc Thesis, Chemical Engineering Department Supervisor: Prof. Dr. Gönül GÜNDÜZ September 2003, 162 pages In this study, isomerization reaction of a-pinene was studied over super acidic and heteropoly acidic catalysts. In addition to these catalysts H2SO4 treated supports have been tested in the isomerization reaction. Natural zeolite, silicagel and y-alumina have been used as supports for heteropoly acidic catalysis. The solid superacids were obtained by introducing a sulfur compound, H2SO4, to Z1O2, TİO2 and Fe2Û3. Reaction was carried out in a batch slurry reactor with constant temperature of 100°C and under nitrogen atmosphere to prevent oxidation of a pinene. Prepared catalysts were tested in the isomerization reaction of a-pinene and were characterized by nitrogen adsorption experiments, DSC, IR, XRD and SEM measurements. The distribution of Lewis and Broensted acid sites of the catalyst were determined, their catalytic activies in a-pinene isomerization reaction and selectivities tomain reaction products, camphene and limonene, were investigated. Limonene continues to introduce the reaction by converting to terpinenes and terpinolenes as secondary reactions. It was seen that a-pinene consumption could be described by 1,5th order kinetics. Activation energy of a-pinene consumption was calculated to be 65,4 kJ/mol. Keywords: a-pinene, isomerization, camphene, limonene, heteropolyacidic catalysts, superacidic catalysts, natural zeolite, silicagel, y-alumina, ZrC>2, TİO2, Fe203, catalyst characterization, reaction kinetics.
Açıklama
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Anahtar Kelimeler
Kimya Mühendisliği, Chemical Engineering, Alfa pinen, Alpha pinene, Katalizörler, Catalysts, Süperasidik, Superacidic, İzomerizasyon, Isomerization