Surface organometallic chemistry of zirconium: Chemical reactivity of the ≡Si-O-ZrNp3 surface complex synthesized on dehydroxylated silica and application to the modification of mordenite

Mariko Adachi, Christophe Nédez, Xu Xu Wang, François Bayard, Véronique Dufaud, Frédéric Lefebvre*, Jean-Marie Maurice Basset

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

The organometallic complex ≡Si-O-Zr(CH2C(CH 3)3)3 was synthesized on the surface of silica dehydroxylated at 500 °C and its reactivity towards oxygenated molecules was studied. The materials were characterized by IR, 13C CP-MAS NMR, analysis of evolved gases and elemental analysis. Reaction with neopentyl alcohol ((CH3)3CCH2OH) leads to the quantitative formation of ≡Si-O-Zr(OCH2C(CH3) 3)3. Similarly, reaction with pivalic acid ((CH 3)3CCOOH) leads to the quantitative formation of ≡Si-O-Zr(OCOC(CH3)3)3. Addition of dry oxygen at 25 °C to ≡Si-O-Zr(CH2C(CH3) 3)3 leads to the formation of ≡Si-O-Zr(OCH 2C(CH3)3)3. When heated at 200 °C under oxygen, the alkoxy ligands transform into carboxylate species ((CH3)3CCOO)- probably coordinated to zirconium. These results, together with molecular modelling studies of the adsorption of hydrocarbons on mordenite modified by such complexes, explain the different behaviours observed in presence of air or inert gases.

Original languageEnglish (US)
Pages (from-to)443-455
Number of pages13
JournalJournal of Molecular Catalysis A: Chemical
Volume204-205
DOIs
StatePublished - Sep 15 2003

Keywords

  • Mordenite
  • Organometallic
  • Oxidation
  • Solid-state NMR
  • Zirconium

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

Fingerprint

Dive into the research topics of 'Surface organometallic chemistry of zirconium: Chemical reactivity of the ≡Si-O-ZrNp<sub>3</sub> surface complex synthesized on dehydroxylated silica and application to the modification of mordenite'. Together they form a unique fingerprint.

Cite this