Mesoporous titanosilicate molecular sieves prepared at ambient temperature by electrostatic (S{sup +}I{sup -}, S{sup +}X{sup -}I{sup +}) and neural (S{degree}I{degree}) assembly pathways: A comparison of physical properties and catalytic activity for peroxide oxidations
Journal Article
·
· Journal of the American Chemical Society
- Michigan State Univ., East Lansing, MI (United States)
- Univ. of Hamburg (Germany)
- Lawrence Livermore National Lab., CA (United States)
Hexagonal mesoporous titanosilicates with distinguishable framework charges and textural mesoporosity, namely, Ti-MCM-41 and Ti-HMS, were prepared at ambient temperature by electrostatic and neutral assembly processes, respectively. Titanium incorporation at the 2 mol % level for both materials was accompanied by increases in lattice parameters and wall thicknesses, but the framework pore sizes remained unaffected. Cross-linking of the anionic framework of as-synthesized Ti-substituted MCM-41 prepared by electrostatic S{sup +}I{sup -} and S{sup +}X{sup -}I{sup +} assembly pathways (where S{sup +} is a quaternary ammonium surfactant and I{sup -} and I{sup +} are ionic silicon precursors) was enhanced significantly by Ti substitution, as judged by {sup 29}Si MAS NMR. The neutral framework of as-synthesized Ti-HMS formed by S{degree}I{degree} assembly (where S{degree} is a primary amine and I{degree} is a neutral silicon precursor) exhibited the same high degree of cross-linking as the unsubstituted silica analog. UV-vis and XANES spectra for the calcined forms of Ti-MCM-41 and Ti-HMS indicated (i) the presence of site-isolated Ti species in the framework, (ii) predominantly tetrahedral coordination for Ti, along with some rehydrated five- and six-coordinated sites, and (iii) Ti siting that was virtually independent of the framework assembly pathway. 35 refs., 5 figs., 3 tabs.
- OSTI ID:
- 420824
- Journal Information:
- Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 38 Vol. 118; ISSN JACSAT; ISSN 0002-7863
- Country of Publication:
- United States
- Language:
- English
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