Molecular understanding of the formation of surface zirconium hydrides upon thermal treatment under hydrogen of [(≡SiO)Zr(CH2tBu) 3] by using advanced solid-state NMR techniques

Franck Rataboul, Anne Baudouin, Chloé Thieuleux, Laurent Veyre, Christophe Copéret*, Jean Thivolle-Cazat, Jean-Marie Maurice Basset, Anne Lesage, Lyndon Emsley

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

108 Scopus citations

Abstract

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 languageEnglish (US)
Pages (from-to)12541-12550
Number of pages10
JournalJournal of the American Chemical Society
Volume126
Issue number39
DOIs
StatePublished - Oct 6 2004

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Fingerprint

Dive into the research topics of 'Molecular understanding of the formation of surface zirconium hydrides upon thermal treatment under hydrogen of [(≡SiO)Zr(CH<sub>2</sub>tBu) <sub>3</sub>] by using advanced solid-state NMR techniques'. Together they form a unique fingerprint.

Cite this