Direct Synthesis of Metal-Chelating Mesoporous Silica:  Effects of Added Organosilanes on Silicate Formation and Adsorption Properties†

Citation

Markowitz, Michael A.; Klaehn, John; Hendel, Robert A.; Qadriq, Syed B.; Golledge, Stephen L.; Castner, David G.; & Gaber, Bruce P. (2000). Direct Synthesis of Metal-Chelating Mesoporous Silica:  Effects of Added Organosilanes on Silicate Formation and Adsorption Properties†. The Journal of Physical Chemistry B, 104(46), 10820-10826.

Abstract

SBA-15 mesoporous silicates with surface functional groups were synthesized by cohydrolysis of tetraethoxyorthosilicate and ethyl-, carboxylate-, and ethylenediaminetriacetic acid-functionalized organosilanes (ETES, CTES, EDATAS, respectively) using the nonionic surfactant poly(ethylene oxide)?poly(propylene oxide)?poly(ethylene oxide) triblock copolymer (PEO20PPO70PEO20, Pluronic P123). X-ray diffraction revealed that silicates synthesized with up to 5% (wt/wt total silica) of added functionalized silane yielded ordered mesoporous materials with P6mm hexagonal symmetry. Further increasing the amount of added functionalized silanes to 20% resulted in a significant decrease in the structural ordering of the resulting silicate. Surface areas, pore volumes, and pore diameters were determined from nitrogen gas adsorption/desorption isotherms. Pore size contraction was observed as the wt % of added ETES was increased but not for the silicates formed with added CTES or EDATAS, with the exception of the silicate formed using 20% added EDATAS. Inclusion of 1,3,5-trimethylbenzene (TMB) during synthesis resulted in silicates with larger pore sizes but a loss of structural order. Appreciable adsorption of copper ions from solution was observed only for the EDATAS-functionalized silicates. X-ray photoelectron spectroscopy of Cu2+-bound EDATAS-functionalized silicates revealed an Cu/N ratio of 0.15, smaller than expected for 1:1 stoichiometry of copper ions and etylenediaminetriacetic acid groups. Adsorption isotherms for Cu2+ binding to EDATAS-functionalized silicates were fit to a double-component Langmuir equation. Binding constants, but not capacity, were dependent on the amount of added EDATAS used in the synthesis and were several orders of magnitude smaller than that reported for structurally similar nonimmobilized HEDTA.

Reference Type

Journal Article

Secondary Title

The Journal of Physical Chemistry B

Author(s)

Markowitz, Michael A.
Klaehn, John
Hendel, Robert A.
Qadriq, Syed B.
Golledge, Stephen L.
Castner, David G.
Gaber, Bruce P.

Year Published

2000

Date Published

973036800

Volume Number

104

Issue Number

46

Pages

10820-10826

ISSN/ISBN

1520-6106

DOI

Direct Synthesis of Metal-Chelating Mesoporous Silica10.1021/jp0008389