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

Year 2018, , 477 - 495, 29.06.2018

Funda Turgut Başoğlu

https://doi.org/10.17776/csj.343221
Cited By: 1

Abstract

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. 

Keywords

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

References

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

Year 2018, , 477 - 495, 29.06.2018

Funda Turgut Başoğlu

https://doi.org/10.17776/csj.343221
Cited By: 1

Abstract

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.

Keywords

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

References

  • [1] Gil A., Korili S.A., Trujillano R. and Vicente M.A., A review on characterization of pillared clays by specific techniques, Appl. Clay Sci., 53 (2011) 97-105.
  • [2] Bergaya F., Aouad A., Mandalia T., Pillared clays and clay minerals, In: Bergaya F., Theng B.K.G., Lagaly G. (Eds.). Development in Clay Science: Handbook of Clay Science. vol. 1, 2nd ed., Amsterdam: Elsevier, 2011; pp 393–421.
  • [3] Vicente M.A., Gil A., Bergaya F., Pillared clays and clay minerals, In: Bergaya F., Lagaly G. (Eds.), Development in Clay Science: Handbook of Clay Science, Part A: Fundamentals, vol. 5, 2nd ed., Amsterdam: Elsevier, 2013; pp 523–557.
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  • [5] Centi G. and Perathoner S., Catalysis by layered materials: a review, Microporous Mesoporous. Mater., 107 (2008) 3-15.
  • [6] Turgut Basoglu F. and Balci S., Catalytic properties and activity of copper and silver containing Al-pillared layered bentonite for CO oxidation, J. Molecular Struct., 1106 (2016) 382-389.
  • [7] Turgut Basoglu F., Effect of the titanium source on the structural properties and acidity of Ti-pillared bentonite, Chem. Pap., 70-7 (2016) 933-945.
  • [8] Tomul F., Turgut Basoglu F. and Canbay H., Determination of adsorptive and catalytic properties of copper, silver and iron containing titanium-pillared bentonite for the removal bisphenol A from aqueous solution, Appl. Surf. Sci., 360 Part B (2016) 579-593.
  • [9] Bineesh K.V., Kim D., Kim M. and Park D., Selective catalytic oxidation of H2S over V2O5 supported on TiO2-pillared clay catalysts in the presence of water and ammonia, Appl. Clay Sci., 53 (2011) 204-211.
  • [10] Carriazo J.G., Moreno-Forero M., Molina R.A. and Moreno S., Incorporation of titanium and titanium iron species inside a smectite type mineral for photocatalysis, Appl. Clay Sci., 50 (2010) 401-408.
  • [11] Chen K., Li J., Li J., Zhang Y. and Wang W., Synthesis and Characterization of TiO2 montmorillonites doped with vanadium and/or carbon and their application for the photodegredation of sulphorbodamine B under UV-vis irradiation, Colloids Surf. A, 360 (2010) 47-56.
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  • [18] Mnasri-Ghnimi S. and Frini-Srasra N., Catalytic wet peroxide oxidation of phenol over Ce-Zr-modified clays: Effect of the pillaring method, Korean J. Chem. Eng., 32-1 (2015) 68-73.
  • [19] Yan Y., Jiang S., Zhang H. and Zhang X., Preparation of novel Fe-ZSM-5 zeolite membrane catalysts for catalytic wet peroxide oxidation of phenol in a membrane reactor, Chem. Eng. J., 259 (2015) 243-251.
  • [20] Luca C., Massa P., Fenoglio R. and Cabello F.M., Improved Fe2O3/Al2O3 as heteregeneous Fenton catalysts for the oxidation of phenol solutions in a continuous reactor, J. Chem. Technol. Biotechnol., 89 (2014) 1121-1128.
  • [21] Martinez F., Pariente M.I., Botas J.A., Melero J.A. and Rubalcaba A., Influence of preoxidizing treatments on the preparation of iron-containing activated carbons for catalytic wet peroxide oxidation of phenol, J. Chem. Technol. Biotechnol., 87 (2012) 880-886.
  • [22] Satishkumar G., Landau M.V., Buzaglo T., Frimet L., Ferentz M., Vidruk R., Wagner F., Gal Y. and Herskowitz M., Fe/SiO2 heteregeneous Fenton catalyst for continuous catalytic wet peroxide oxidation prepared in situ by grafting of iron released from LaFeO3, Appl. Catal. B Environ., 138-139 (2013) 276-284.
  • [23] Zhong X., Barbier J., Duprez D., Zhang H. and Royer S., Modulating the copper oxide morphology and accessibility by using micro-/mesoporous SBA-15 structures as host support: effect on the activity for the CWPO of phenol reaction, Appl. Catal. B Environ., 121-122 (2012) 123-134.
  • [24] Dougna A.A., Gombert B., Kodom T., Djaneye-Boundjou G., Boukari S.O.B., Vel Leitner N.K. and Bawa L.M., Photocatalytic removal of phenol using titanium dioxide deposited on different substrates: Effect of inorganic oxidants, J. Photochem. Photobio. A Chem., 305 (2015) 67-77.
  • [25] Khraisheh M., Wu L., Al-Muhtaseb A.H., Albadarin A.B. and Walker G.M., Phenol degradation by powdered metal ion modified titanium dioxide photocatalysts, Chem. Eng. J., 213 (2012) 125-134.
  • [26] Lopes R.J.G., Perdigoto M.L.N. and Quinta-Ferreira R.M., Tailored investigation and characterization of heteregeneous {Mn, Cu}/TiO2 catalysts embedded within a ceria-based framework for the wet peroxide oxidation of hazardous pollutants, Appl. Catal. B Environ., 117-118 (2012) 292-301.
  • [27] Menesi J., Körösi L., Bazso E., Zöllmer V., Richardt A. and Dekany I., Photocatalytic oxidation of organic pollutants on titania-clay composites, Chemosphere, 70 (2008) 538-542.
  • [28] Turki A., Guillard C., Dappozze F., Ksibi Z., Berhault G. and Kochkar H., Phenol photocatalytic degradation over anisotropic TiO2 nanomaterials: Kinetic study, adsorption isotherms and formal mechanisms, Appl. Catal. B Environ., 163 (2015) 404-414.
  • [29] Li Z., Sheng J., Zhang Y., Li X. and Xu Y., Role of CeO2 as oxygen promoter in the accelerated photocatalytic degradation of phenol over rutile TiO2, Appl. Catal. B Environ., 166-167 (2015) 313-319.
  • [30] Mnasri-Ghnimi S. and Frini-Srasra N., Effect of Al and Ce on Zr-pillared bentonite and their performance in catalytic oxidation of phenol, Russian J. Phys. Chem. A, 90-9 (2016) 1766-1773.
  • [31] Timofeeva M.N., Khankhasaeva S.Ts., Talsi E P., Panchenko V.N., Golovin A.V., Dashinamzhilova E.Ts. and Tsybulya S.V., The effect of Fe/Cu ratio in the synthesis of mixed Fe, Cu, Al-clays used as catalysts in phenol peroxide oxidation, Appl. Catal. B Environ., 90 (2009) 618-627.
  • [32] Tomul F., The effect of ultrasonic treatment on iron-chromium pillared bentonite synthesis and catalytic wet peroxide oxidation of phenol, Appl. Clay Sci., 120 (2016) 121-134.
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There are 60 citations in total.

Details

Primary Language English
Journal Section Engineering Sciences
Authors

Funda Turgut Başoğlu

Publication Date June 29, 2018
Submission Date October 13, 2017
Acceptance Date April 27, 2018
Published in Issue Year 2018

Cite

APA Turgut Başoğlu, F. (2018). Effects of Cerium, Iron and Copper Incorporation on the Structural Properties and Activities of Ti-Pillared Bentonites. Cumhuriyet Science Journal, 39(2), 477-495. https://doi.org/10.17776/csj.343221

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