Unified Formation Mechanism of Disordered Mesoporous Silica, Structured by Means of Nontemplating Organic Additives

作者:Wang Jia*; Groen Johan C; Coppens Marc Olivier
来源:Journal of Physical Chemistry C, 2008, 112(49): 19336-19345.
DOI:10.1021/jp805276j

摘要

TUD-C and TUD-M are two novel mesoporous zeolite composites. Tetrapropyl ammonium hydroxide (TPAOH) plays the well-known templating role in the formation of the zeolite micropores. The role of TPAOH in the formation of the disordered mesopores of a controlled size can be described as "nontemplating structure-directing". For the first time, this type of structure-directing is systematically investigated and compared with templating. Supra-molecular templates are not involved. The nontemplating structure-directing mechanism in the TEOS-TPAOH-H(2)O system consists of three steps: (1) formation of silica nanoparticles in the presence of TPAOH during homogenization of the solution; (2) development of a gel with extended silica framework during the mild evaporation of ethanol and water; and (3) drying of the gel. TPAOH plays an important role in each of these steps. The key parameters for a successful synthesis are pH, solution composition, and temperature. It is shown that this type of structure-directing is a rather general phenomenon, since many organic molecules can play a role similar to TPAOH. However, the required synthesis conditions vary between different molecules. The mechanism is investigated by means of ATR-IR, TEM, N(2) sorption, and NMR experiments.

  • 出版日期2008-12-11