Geopolymers made using organic bases. Part I: Synthesis and atomic structure

Geopolymers can act as a facile forming route to aluminosilicate ceramic composites due to being processed as fluids rather than as powders. However, the compositions available via typical alkali geopolymers are limited by the presence of alkali cations, introduced by the alkali silicate solution precursors. In order to expand the ceramic compositions that are accessible by geopolymer processing, this study explored the use of three strong organic bases (guanidine, tetramethylguanidine [TMG], and tetramethylammonium hydroxide [TMAOH]) as alternatives to inorganic alkali hydroxides in geopolymer synthesis. Silicate solutions were able to be produced with all three bases and favorable silica speciation was identified in the guanidine and TMG silicate solutions. Monolithic bodies were produced using guanidine and TMAOH, while no TMG samples hardened. By ²⁷Al and ²⁹Si nuclear magnetic resonance spectroscopy and powder X-ray diffraction, the guanidine samples were determined to be structurally similar to those made using sodium hydroxide and hence can be called geopolymers, while the solids made with TMAOH were not structurally similar to sodium geopolymers and contained one or more unknown phases. This study has demonstrated that geopolymers can be made using organic bases rather than alkali hydroxides and that the speciation of dissolved silica alone does not indicate that an organic base silicate solution will be reactive.