The reaction of [(≡SiO)Zr(CH2tBu)3] with H 2 at 150 °C leads to the hydrogenolysis of the zirconium-carbon bonds to form a very reactive hydride intermediate(s), which further reacts with the surrounding siloxane ligands present at the surface of this support to form mainly two different zirconium hydrides: [(≡SiO)3Zr-H] (1a, 70-80%) and [(≡SiO)2ZrH2] (1b, 20-30%) along with silicon hydrides, [(≡SiO)3SiH] and [(≡SiO) 2SiH2]. Their structural identities were identified by 1H DQ solid-state NMR spectroscopy as well as reactivity studies. These two species react with CO2 and N2O to give, respectively, the corresponding formate [(≡SiO)4-xZr(O-C(=O)H) x] (2) and hydroxide complexes [(≡SiO)4-xZr(OH) x] (x = 1 or 2 for 3a and 3b, respectively) as major surface complexes.
|Original language||English (US)|
|Number of pages||10|
|Journal||Journal of the American Chemical Society|
|State||Published - Oct 6 2004|
ASJC Scopus subject areas
- Colloid and Surface Chemistry