Seryum, Demir ve Bakır Emdirmenin, Ti-Sütunlu Bentonitlerin Yapısal Özellikleri ve Aktiviteleri Üzerine Etkileri

Yıl 2018, Cilt: 39 Sayı: 2, 477 - 495, 29.06.2018

Funda Turgut Başoğlu

https://doi.org/10.17776/csj.343221

Cited By: 1

Öz

Orta
Anadolu yöresi (Hançılı) bentoniti kullanılarak, Ti-sütunlu bentonit (Ti-SB)
sentezlenmiştir. Ti-SB’e demir ya da bakır, çözeltiden emdirilmiş ve devamında
seryum, ıslak emdirmeyle demirli ve bakırlı Ti-SB’e ilave edilmiştir. Bakırlı
titanyumlu sütunlu bentonitler, Cu/(Cu+Ti) 0,1 ve 0,2 oranlarında hidrotermal
olarak sentezlenmiştir. Bütün numunelerde titanyum dioksit, anataz fazda
görülmüştür. 500 °C de kalsine
edilmiş Ti-SB için 4.41 nm bazal boşluk değeri, 348 m² g^-1
spesifik BET yüzey alanı, 0.093 cm³g^-1 mikrogözenek hacim
değeri elde edilmiştir.  Demir ve bakırın
sonradan ilave edilmesi, elde edilen örneklerin mikrogözenek özelliklerinde
azalmaya sebep olurken, hidrotermal yöntemle sentezlenen bakır titanyumlu örnekler,
Ti-SB ile benzer davranış sergilemişlerdir. 
Enerji dağılımlı X-ışını spektroskopisi (EDS) analizi, bütün örneklerin TiO₂ içeriğinin ağırlıkça yaklaşık % 40 civarında olduğunu ve
Ti-SB’e metal emdirmenin başarılı bir şekilde gerçekleştiğini göstermiştir.
Ti-SB örneklerinde hem Lewis hem de Brønsted asitliği gözlenmiştir. Bakır emdirme, Lewis asitlikte artışa
neden olmuştur. Hidrotermal olarak sentezlenmiş bakır içeren örneklerde, seryum
demir ve seryum bakırlı örneklerde Bronsted asitliğinin arttığı gözlenmiştir.
Seryum ve demir içeren örnekle gerçekleştirilen reaksiyon çalışmalarında
yaklaşık % 90 fenol dönüşümü, 30 °C de 1 saat içinde elde edilmiş ve fotokatalitik oksidasyonun
tamamlanması 2 saatde gerçekleşmiştir. Sıcaklığın artması, fenol dönüşümünü
artırmış ve demir içeren örnekle, 50 °C de 1 saat içinde yaklaşık % 100 dönüşüm elde
edilmiştir. Hidrokinon, benzokinon, katekol ve formic, malik, fumarik asitler
reaksiyon ara ürünleri olarak gözlenmiştir. Düşük değerlerde metal salınımı ve
demirin bakıra göre 6 kat daha fazla kararlılık gösterdiği gözlenmiştir. 

Anahtar Kelimeler

Ti-sütunlu bentonit, yapısal özellikler, yüzey asitliği, fotokatalitik ıslak peroksit oksidasyon

Effects of Cerium, Iron and Copper Incorporation on the Structural Properties and Activities of Ti-Pillared Bentonites

Öz

Ti-pillared
bentonite (Ti-PB) using bentonite from the Middle Anatolia region
(Hançılı) was synthesized. Iron or copper was impregnated to Ti-PB from the solution and subsequent cerium
incorporation was done by wet impregnation. The hydrothermal syntheses were carried out with a Cu/(Cu+Ti)
ratios of 0.1
and 0.2. The anatase phase of titanium dioxide was found for all of
the samples. The Ti-PB calcined at 500
°C gave a basal spacing value of 4.41 nm, a specific BET surface area of 348 m²
g^-1, and a micropore volume of 0.093 cm³g^-1. While the post
incorporation of copper and iron caused decrease in the micropore properties,
the hydrothermally synthesized copper titanium samples reflected the similar
behavior with Ti-PB. Energy dispersive X-ray spectroscopy (EDS) analyses
indicated that TiO₂ content of all PBs was near 40 wt % and metal
incorporation to Ti-PB was succesfully performed by the impregnation method. Ti-PB exhibited both
the Lewis and Brønsted acidities. The copper impregnation resulted in an increase in the Lewis
acidity. The hydrotermally synthesised copper containing
sample and cerium-iron and cerium-copper impregnated samples yielded an
increase in the Brønsted acidity. Approximately 90 % phenol conversion at 30 °C in an hour was achived with the cerium and iron containing sample and the completion of photocatalytic
oxidation was reached at 2 hours. An increase of temperature rised the
conversion of phenol, and the iron
containing sample resulted in approximately 100 % conversion at an hour at 50
°C. Hydroquinone, benzoquinone and catechol and
formic, malic, fumaric acids were observed as the reaction intermediates. The
leaching of metals was observed at low values and the stability of iron was
found six times higher than the copper.

Anahtar Kelimeler

Ti-pillared bentonite, structural properties, surface acidity, photocatalytic wet peroxide oxidation

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