Titanium-silica catalyst derived from defined metallic titanium cluster precursor: Synthesis and catalytic properties in selective oxidations

Claudio Evangelisti, Matteo Guidotti, Cristina Tiozzo, Rinaldo Psaro, Nataliya Maksimchuk, Irina Ivanchikova, Alexandr N. Shmakov, Oxana Kholdeeva

Research output: Contribution to journalArticlepeer-review

5 Citations (Scopus)

Abstract

A class of titanium-grafted mesoporous silica catalysts has been designed and prepared starting from molecularly defined metal clusters. The organosol mixture of zerovalent Ti13 clusters was impregnated onto the surface of ordered mesoporous silica molecular sieves (MCM-41 and MMM-2) and, after high-temperature calcination, an evenly dispersed non-single-site Ti(IV)nOx-like silica-supported catalyst was obtained. The catalytic solids, fully characterized by microscopic, spectroscopic and porosimetric techniques, showed standard performance in the liquid-phase epoxidation of a cyclic alkene, as limonene, but remarkably high selectivity values in the oxidative carboxylation of styrene, with tert-butylhydroperoxide and carbon dioxide in the presence of tetrabutylammonium bromide as a cocatalyst. Unprecedented high yields, up to 67%, in styrene carbonate were achieved after 24 h, under solvent-free conditions. The catalysts displayed also a noteworthy stability of the performance to repeated recovery and reuse cycles.

Original languageEnglish
Pages (from-to)393-401
Number of pages9
JournalInorganica Chimica Acta
Volume470
DOIs
Publication statusPublished - 30 Jan 2018

Keywords

  • Alkene epoxidation
  • Heterogeneous catalysis
  • Mesoporous silica
  • Oxidative carboxylation
  • Titanium clusters
  • ACTIVE-SITES
  • MOLECULAR-SIEVES
  • SILSESQUIOXANE COMPLEXES
  • CYCLOHEXENE EPOXIDATION
  • SITE HETEROGENEOUS CATALYSTS
  • LIQUID-PHASE
  • SINGLE-SITE
  • ALTERNATING COPOLYMERIZATION
  • FINE CHEMICALS
  • MESOPOROUS SILICA

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