A Silicon, Carbon and Deuterium NMR Investigation of Molecular Templating in Amorphous Silicas
The precise pore sizes defined by crystalline zeolite lattices have led to intensive research on zeolite membranes. Unfortunately zeolites have proven to be extremely difficult to prepare in a defect-free thin film form needed for membrane flux and selectivity. We introduce tetrapropylammonium TPA (a structure directing agent for zeolite ZSM-5) into a silica sol and exploit the development of high solvation stresses to create templated amorphous silicas with pore apertures comparable in size to those of ZSM-5. {sup 29}Si and {sup 2}H NMR experiments were performed to evaluate the efficacy of our templating approach. The {sup 29}Si NMR spectrum of the silica matrix was observed by an intermolecular cross-polarization experiment between the {sup 1}H nuclei of TPA and the {sup 29}Si nuclei in the silica matrix. The efficiency of the cross-polarization interaction was used to investigate the degree to which the matrix formed a tight cage surrounding the template molecule. Normally prepared xerogel materials exhibited only weak interactions between the two sets of nuclei. Drying under reduced pressure, where solvation stresses are maximized, resulted in significantly increased interactions. Analogous materials were prepared using fully deuterated TPA. The {sup 2}H NMR wideline spectra consisted of a partially narrowed resonance, corresponding to template molecules which were undergoing restricted rotational motion, and an isotropically narrowed resonance, corresponding to molecules which were undergoing rapid rotational motion. The number of isotropically rotating template molecules decreased for specimens dried under reduced pressure, consistent with improved templating of amorphous silica by TPA.
- Research Organization:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- AC04-94AL85000
- OSTI ID:
- 5676
- Report Number(s):
- SAND98-2497C; TRN: AH200115%%85
- Resource Relation:
- Conference: Materials Research Society Spring Meeting, San Francisco, CA (US), 04/04/1999--04/09/1999; Other Information: PBD: 8 Apr 1999
- Country of Publication:
- United States
- Language:
- English
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