Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites

Rabindran J. Balasamy; Balkrishna B. Tope; Alam Khurshid; Ali A S Al-Ali; Luqman A. Atanda; Kunimasa Sagata; Makiko Asamoto; Hidenori Yahiro; Kiyoshi Nomura; Tsuneji Sano; Katsuomi Takehira; Sulaiman S. Al-Khattaf

doi:10.1016/j.apcata.2011.03.023

Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites

Rabindran J. Balasamy, Balkrishna B. Tope, Alam Khurshid, Ali A S Al-Ali, Luqman A. Atanda, Kunimasa Sagata, Makiko Asamoto, Hidenori Yahiro, Kiyoshi Nomura, Tsuneji Sano, Katsuomi Takehira, Sulaiman S. Al-Khattaf

Research output: Contribution to journal › Article › peer-review

41 Scopus citations

Abstract

A series of Mg3-xZnxFe0.5Al0.5 mixed oxide catalysts derived from hydrotalcites were tested in the ethylbenzene dehydrogenation to styrene in He atmosphere at 550 °C. The catalysts were prepared by coprecipitation from the nitrates of metal components followed by calcination to mixed oxides at 550 °C. A part of Mg2+ in Mg 3Fe0.5Al0.5 mixed oxide was replaced with Zn2+ to test the effect of MgO as the support. The mixed oxides were composed of periclase and spinel-type compounds with a high surface area of 100-180m2gcat-1. Mössbauer and XPS measurements indicated the presence of Fe3+ on the catalysts and H2-TPR measurement suggested that the dehydrogenation reaction is catalyzed by the reduction-oxidation between Fe3+/Fe2+. The activity of Mg3-xZnxFe0.5Al0.5 mixed oxide decreased with increasing x, indicating an important role of MgO on the activity. Both CO2-TPD measurements as well as IR measurements of adsorbed CO2 clearly indicated the presence of basic sites of Mg 2+O2- on the catalysts. It seems that the combination of Mg2+O2- and Fe3+ was essential for the catalytic activity. It is concluded that the surface base sites generated on O2- bound Mg2+ near Fe3+ sites are responsible for H+-abstraction; the dehydrogenation of ethylbenzene was initiated by the H+ abstraction on Mg2+O2- basic sites, and accelerated by the reduction-oxidation of Fe3+/Fe2+ active species. © 2011 Elsevier B.V.

Original language	English (US)
Pages (from-to)	113-122
Number of pages	10
Journal	Applied Catalysis A: General
Volume	398
Issue number	1-2
DOIs	https://doi.org/10.1016/j.apcata.2011.03.023
State	Published - May 2011
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): K-C1-019-12
Acknowledgements: This publication was based on the work supported by Award No. K-C1-019-12 made by King Abdullah University of Science and Technology (KAUST). The support of King Fahd University of Petroleum and Minerals (KFUPM) is also highly appreciated. The authors are grateful to Prof. Emeritus H. Hattori of Hokkaido University for helpful discussions. The authors also acknowledged Japan Cooperation Center, Petroleum (JCCP) for giving an opportunity of this collaborative research.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

Access to Document

10.1016/j.apcata.2011.03.023

Cite this

Balasamy, R. J., Tope, B. B., Khurshid, A., Al-Ali, A. A. S., Atanda, L. A., Sagata, K., Asamoto, M., Yahiro, H., Nomura, K., Sano, T., Takehira, K., & Al-Khattaf, S. S. (2011). Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites. Applied Catalysis A: General, 398(1-2), 113-122. https://doi.org/10.1016/j.apcata.2011.03.023

@article{206c402f73684dc597ddff39f35800db,

title = "Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites",

abstract = "A series of Mg3-xZnxFe0.5Al0.5 mixed oxide catalysts derived from hydrotalcites were tested in the ethylbenzene dehydrogenation to styrene in He atmosphere at 550 °C. The catalysts were prepared by coprecipitation from the nitrates of metal components followed by calcination to mixed oxides at 550 °C. A part of Mg2+ in Mg 3Fe0.5Al0.5 mixed oxide was replaced with Zn2+ to test the effect of MgO as the support. The mixed oxides were composed of periclase and spinel-type compounds with a high surface area of 100-180m2gcat-1. M{\"o}ssbauer and XPS measurements indicated the presence of Fe3+ on the catalysts and H2-TPR measurement suggested that the dehydrogenation reaction is catalyzed by the reduction-oxidation between Fe3+/Fe2+. The activity of Mg3-xZnxFe0.5Al0.5 mixed oxide decreased with increasing x, indicating an important role of MgO on the activity. Both CO2-TPD measurements as well as IR measurements of adsorbed CO2 clearly indicated the presence of basic sites of Mg 2+O2- on the catalysts. It seems that the combination of Mg2+O2- and Fe3+ was essential for the catalytic activity. It is concluded that the surface base sites generated on O2- bound Mg2+ near Fe3+ sites are responsible for H+-abstraction; the dehydrogenation of ethylbenzene was initiated by the H+ abstraction on Mg2+O2- basic sites, and accelerated by the reduction-oxidation of Fe3+/Fe2+ active species. {\textcopyright} 2011 Elsevier B.V.",

author = "Balasamy, {Rabindran J.} and Tope, {Balkrishna B.} and Alam Khurshid and Al-Ali, {Ali A S} and Atanda, {Luqman A.} and Kunimasa Sagata and Makiko Asamoto and Hidenori Yahiro and Kiyoshi Nomura and Tsuneji Sano and Katsuomi Takehira and Al-Khattaf, {Sulaiman S.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): K-C1-019-12 Acknowledgements: This publication was based on the work supported by Award No. K-C1-019-12 made by King Abdullah University of Science and Technology (KAUST). The support of King Fahd University of Petroleum and Minerals (KFUPM) is also highly appreciated. The authors are grateful to Prof. Emeritus H. Hattori of Hokkaido University for helpful discussions. The authors also acknowledged Japan Cooperation Center, Petroleum (JCCP) for giving an opportunity of this collaborative research. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

year = "2011",

month = may,

doi = "10.1016/j.apcata.2011.03.023",

language = "English (US)",

volume = "398",

pages = "113--122",

journal = "Applied Catalysis A: General",

issn = "0926-860X",

publisher = "Elsevier B.V.",

number = "1-2",

}

Balasamy, RJ, Tope, BB, Khurshid, A, Al-Ali, AAS, Atanda, LA, Sagata, K, Asamoto, M, Yahiro, H, Nomura, K, Sano, T, Takehira, K & Al-Khattaf, SS 2011, 'Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites', Applied Catalysis A: General, vol. 398, no. 1-2, pp. 113-122. https://doi.org/10.1016/j.apcata.2011.03.023

TY - JOUR

T1 - Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites

AU - Balasamy, Rabindran J.

AU - Tope, Balkrishna B.

AU - Khurshid, Alam

AU - Al-Ali, Ali A S

AU - Atanda, Luqman A.

AU - Sagata, Kunimasa

AU - Asamoto, Makiko

AU - Yahiro, Hidenori

AU - Nomura, Kiyoshi

AU - Sano, Tsuneji

AU - Takehira, Katsuomi

AU - Al-Khattaf, Sulaiman S.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): K-C1-019-12 Acknowledgements: This publication was based on the work supported by Award No. K-C1-019-12 made by King Abdullah University of Science and Technology (KAUST). The support of King Fahd University of Petroleum and Minerals (KFUPM) is also highly appreciated. The authors are grateful to Prof. Emeritus H. Hattori of Hokkaido University for helpful discussions. The authors also acknowledged Japan Cooperation Center, Petroleum (JCCP) for giving an opportunity of this collaborative research. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

PY - 2011/5

Y1 - 2011/5

N2 - A series of Mg3-xZnxFe0.5Al0.5 mixed oxide catalysts derived from hydrotalcites were tested in the ethylbenzene dehydrogenation to styrene in He atmosphere at 550 °C. The catalysts were prepared by coprecipitation from the nitrates of metal components followed by calcination to mixed oxides at 550 °C. A part of Mg2+ in Mg 3Fe0.5Al0.5 mixed oxide was replaced with Zn2+ to test the effect of MgO as the support. The mixed oxides were composed of periclase and spinel-type compounds with a high surface area of 100-180m2gcat-1. Mössbauer and XPS measurements indicated the presence of Fe3+ on the catalysts and H2-TPR measurement suggested that the dehydrogenation reaction is catalyzed by the reduction-oxidation between Fe3+/Fe2+. The activity of Mg3-xZnxFe0.5Al0.5 mixed oxide decreased with increasing x, indicating an important role of MgO on the activity. Both CO2-TPD measurements as well as IR measurements of adsorbed CO2 clearly indicated the presence of basic sites of Mg 2+O2- on the catalysts. It seems that the combination of Mg2+O2- and Fe3+ was essential for the catalytic activity. It is concluded that the surface base sites generated on O2- bound Mg2+ near Fe3+ sites are responsible for H+-abstraction; the dehydrogenation of ethylbenzene was initiated by the H+ abstraction on Mg2+O2- basic sites, and accelerated by the reduction-oxidation of Fe3+/Fe2+ active species. © 2011 Elsevier B.V.

AB - A series of Mg3-xZnxFe0.5Al0.5 mixed oxide catalysts derived from hydrotalcites were tested in the ethylbenzene dehydrogenation to styrene in He atmosphere at 550 °C. The catalysts were prepared by coprecipitation from the nitrates of metal components followed by calcination to mixed oxides at 550 °C. A part of Mg2+ in Mg 3Fe0.5Al0.5 mixed oxide was replaced with Zn2+ to test the effect of MgO as the support. The mixed oxides were composed of periclase and spinel-type compounds with a high surface area of 100-180m2gcat-1. Mössbauer and XPS measurements indicated the presence of Fe3+ on the catalysts and H2-TPR measurement suggested that the dehydrogenation reaction is catalyzed by the reduction-oxidation between Fe3+/Fe2+. The activity of Mg3-xZnxFe0.5Al0.5 mixed oxide decreased with increasing x, indicating an important role of MgO on the activity. Both CO2-TPD measurements as well as IR measurements of adsorbed CO2 clearly indicated the presence of basic sites of Mg 2+O2- on the catalysts. It seems that the combination of Mg2+O2- and Fe3+ was essential for the catalytic activity. It is concluded that the surface base sites generated on O2- bound Mg2+ near Fe3+ sites are responsible for H+-abstraction; the dehydrogenation of ethylbenzene was initiated by the H+ abstraction on Mg2+O2- basic sites, and accelerated by the reduction-oxidation of Fe3+/Fe2+ active species. © 2011 Elsevier B.V.

UR - http://hdl.handle.net/10754/600103

UR - https://linkinghub.elsevier.com/retrieve/pii/S0926860X11001554

UR - http://www.scopus.com/inward/record.url?scp=79955470536&partnerID=8YFLogxK

U2 - 10.1016/j.apcata.2011.03.023

DO - 10.1016/j.apcata.2011.03.023

M3 - Article

SN - 0926-860X

VL - 398

SP - 113

EP - 122

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

IS - 1-2

ER -

Ethylbenzene dehydrogenation over FeOx/(Mg,Zn)(Al)O catalysts derived from hydrotalcites: Role of MgO as basic sites

Abstract

Bibliographical note

Access to Document

Other files and links

Fingerprint

Cite this