Surface functionalization of mesoporous silica SBA-15 by liquid-phase grafting of zirconium phosphate

Jianan Zhang; Zhen Ma; Jian Jiao; Hongfeng Yin; Wenfu Yan; Edward W. Hagaman; Jihong Yu; Sheng Dai

doi:10.1016/j.micromeso.2009.09.016

Surface functionalization of mesoporous silica SBA-15 by liquid-phase grafting of zirconium phosphate

Jianan Zhang, Zhen Ma, Jian Jiao, Hongfeng Yin, Wenfu Yan, Edward W. Hagaman, Jihong Yu, Sheng Dai

Chemical Sciences Division

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

39 Scopus citations

Abstract

The introduction of mesoporous silicas in the 1990s has offered new opportunities for the engineering of ordered catalytic nanoreactors, but the acid properties of mesoporous silicas are rather poor. Herein, mesoporous silica (SBA-15) surfaces were functionalized by zirconium phosphate via two methods recently developed in our group. Zr(OPr)₄ and POCl₃ were used as appropriate precursors in both methods. The main difference between these methods lies in whether Zr(OPr)₄ is grafted onto SBA-15 first and POCl₃ second (method 1) or the grafting process takes place in one pot, with SBA-15, Zr(OPr)₄, and POCl₃ altogether (method 2). More zirconium phosphate could be grafted by repeating the above procedures. The materials were characterized by ICP-OES, XRD, N₂ adsorption-desorption, TEM, ³¹P and ²⁹Si MAS NMR, and NH₃-TPD, and their applications in catalytic isopropanol dehydration, cumene cracking, and metal-ion adsorption were demonstrated. Aluminum phosphate-modified SBA-15 samples could be obtained via these two methods as well. This work enriches the family of metal phosphate-functionalized mesoporous silicas as new solid acid catalysts.

Original language	English
Pages (from-to)	200-209
Number of pages	10
Journal	Microporous and Mesoporous Materials
Volume	129
Issue number	1-2
DOIs	https://doi.org/10.1016/j.micromeso.2009.09.016
State	Published - Apr 1 2010

Funding

S. Dai thanks the Division of Chemical Sciences, Office of Basic Energy Sciences, US Department of Energy under contract DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. J.H. Yu thanks the grants provided by National Natural Science Foundation of China and the State Basic Research Project (973) of China. This research was also supported by the appointment for Z. Ma, J. Jiao, and H.F. Yin to the ORNL Research Associates Program, administered by Oak Ridge Associated Universities.

Funders	Funder number
Division of Chemical Sciences
State Basic Research Project (973) of China
U.S. Department of Energy	DE-AC05-00OR22725
Basic Energy Sciences
Oak Ridge Associated Universities
Oak Ridge National Laboratory
National Natural Science Foundation of China

Keywords

Aluminum phosphate
Grafting
Mesoporous silica
SBA-15
Solid acid
Surface functionalization
Zirconium phosphate

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title = "Surface functionalization of mesoporous silica SBA-15 by liquid-phase grafting of zirconium phosphate",

abstract = "The introduction of mesoporous silicas in the 1990s has offered new opportunities for the engineering of ordered catalytic nanoreactors, but the acid properties of mesoporous silicas are rather poor. Herein, mesoporous silica (SBA-15) surfaces were functionalized by zirconium phosphate via two methods recently developed in our group. Zr(OPr)4 and POCl3 were used as appropriate precursors in both methods. The main difference between these methods lies in whether Zr(OPr)4 is grafted onto SBA-15 first and POCl3 second (method 1) or the grafting process takes place in one pot, with SBA-15, Zr(OPr)4, and POCl3 altogether (method 2). More zirconium phosphate could be grafted by repeating the above procedures. The materials were characterized by ICP-OES, XRD, N2 adsorption-desorption, TEM, 31P and 29Si MAS NMR, and NH3-TPD, and their applications in catalytic isopropanol dehydration, cumene cracking, and metal-ion adsorption were demonstrated. Aluminum phosphate-modified SBA-15 samples could be obtained via these two methods as well. This work enriches the family of metal phosphate-functionalized mesoporous silicas as new solid acid catalysts.",

keywords = "Aluminum phosphate, Grafting, Mesoporous silica, SBA-15, Solid acid, Surface functionalization, Zirconium phosphate",

author = "Jianan Zhang and Zhen Ma and Jian Jiao and Hongfeng Yin and Wenfu Yan and Hagaman, {Edward W.} and Jihong Yu and Sheng Dai",

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AU - Zhang, Jianan

AU - Ma, Zhen

AU - Jiao, Jian

AU - Yin, Hongfeng

AU - Yan, Wenfu

AU - Hagaman, Edward W.

AU - Yu, Jihong

AU - Dai, Sheng

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N2 - The introduction of mesoporous silicas in the 1990s has offered new opportunities for the engineering of ordered catalytic nanoreactors, but the acid properties of mesoporous silicas are rather poor. Herein, mesoporous silica (SBA-15) surfaces were functionalized by zirconium phosphate via two methods recently developed in our group. Zr(OPr)4 and POCl3 were used as appropriate precursors in both methods. The main difference between these methods lies in whether Zr(OPr)4 is grafted onto SBA-15 first and POCl3 second (method 1) or the grafting process takes place in one pot, with SBA-15, Zr(OPr)4, and POCl3 altogether (method 2). More zirconium phosphate could be grafted by repeating the above procedures. The materials were characterized by ICP-OES, XRD, N2 adsorption-desorption, TEM, 31P and 29Si MAS NMR, and NH3-TPD, and their applications in catalytic isopropanol dehydration, cumene cracking, and metal-ion adsorption were demonstrated. Aluminum phosphate-modified SBA-15 samples could be obtained via these two methods as well. This work enriches the family of metal phosphate-functionalized mesoporous silicas as new solid acid catalysts.

AB - The introduction of mesoporous silicas in the 1990s has offered new opportunities for the engineering of ordered catalytic nanoreactors, but the acid properties of mesoporous silicas are rather poor. Herein, mesoporous silica (SBA-15) surfaces were functionalized by zirconium phosphate via two methods recently developed in our group. Zr(OPr)4 and POCl3 were used as appropriate precursors in both methods. The main difference between these methods lies in whether Zr(OPr)4 is grafted onto SBA-15 first and POCl3 second (method 1) or the grafting process takes place in one pot, with SBA-15, Zr(OPr)4, and POCl3 altogether (method 2). More zirconium phosphate could be grafted by repeating the above procedures. The materials were characterized by ICP-OES, XRD, N2 adsorption-desorption, TEM, 31P and 29Si MAS NMR, and NH3-TPD, and their applications in catalytic isopropanol dehydration, cumene cracking, and metal-ion adsorption were demonstrated. Aluminum phosphate-modified SBA-15 samples could be obtained via these two methods as well. This work enriches the family of metal phosphate-functionalized mesoporous silicas as new solid acid catalysts.

KW - Aluminum phosphate

KW - Grafting

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KW - SBA-15

KW - Solid acid

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Surface functionalization of mesoporous silica SBA-15 by liquid-phase grafting of zirconium phosphate

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