Enhanced Catalytic Performance of a Ce/V Oxo Cluster through Confinement in Mesoporous SBA-15

Xingjie Wang, Zoha H. Syed, Zhihengyu Chen, J. David Bazak, Xinyi Gong, Megan C. Wasson, Nancy M. Washton, Karena W. Chapman, Justin M. Notestein, Omar K. Farha*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

To increase catalytic efficiency, mesoporous supports have been widely applied to immobilize well-defined metal oxide clusters due to their ability to stabilize highly dispersed clusters. Herein, a redox-active heterometallic Ce12V6-oxo cluster (CeV) was first presynthesized and then incorporated into mesoporous silica, SBA-15, via a straightforward impregnation method. Scanning transmission electron microscopy (STEM) and Fourier transform infrared spectroscopy (FTIR), in concert with scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDS), verified the successful introduction of the CeV cluster inside the pore of SBA-15. The 51V magic angle spinning solid-state nuclear magnetic resonance (51V MAS NMR) spectroscopy and differential pair distribution function (dPDF) analysis confirmed the structural integrity of the CeV cluster inside the SBA-15. The composite was then benchmarked for liquid-phase oxidation of 2-chloroethyl ethyl sulfide (CEES) under mild conditions and gas-phase oxidative dehydrogenation (ODH) of propane under high temperatures (up to 550 °C). The catalytic reactivity results demonstrated 8- and 14-fold increase in turnover frequency (TOF) values of the composite (CeV@10SBA-2) than the bulk CeV cluster under the same conditions for CEES oxidation and ODH, respectively. These results highlight the improved reactivity of the catalytically active CeV cluster as attributed to the higher dispersion of the discrete cluster upon immobilization within the SBA-15 support.

Original languageEnglish (US)
Pages (from-to)52886-52893
Number of pages8
JournalACS Applied Materials and Interfaces
Volume14
Issue number47
DOIs
StatePublished - Nov 30 2022

Keywords

  • CEES oxidation
  • SBA-15
  • cerium vanadium oxo cluster
  • propane oxidative dehydrogenation
  • solid state NMR

ASJC Scopus subject areas

  • General Materials Science

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