DRIFTS/MS/Isotopic Labeling Study on the NO-Moderated Decomposition of a Silica-Supported Nickel Nitrate Catalyst Precursor

M. Wolters, H. Daly, A. Goguet, F. C. Meunier, C. Hardacre, J. H. Bitter, P. E. de Jongh, K. P. de Jong*

*Corresponding author for this work

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

In the preparation of silica-supported nickel oxide from nickel nitrate impregnation and drying, the replacement of the traditional air calcination step by a thermal treatment in 1% NO/Ar prevents agglomeration, resulting in highly dispersed NiO. The mechanism by which NO prevents agglomeration was investigated by using combined in situ diffuse reflectance infrared fourier transform (DRIFT) spectroscopy and mass spectrometry (MS). After impregnation and drying, a supported nickel hydroxynitrate phase with composition Ni(3)(NO(3))(2)(OH)(4) had been formed. Comparison of the evolution of the decomposition gases during the thermal decomposition of Ni(3)(NO(3))(2)(OH)(4) in labeled and unlabeled NO and O(2) revealed that NO scavenges oxygen radicals, forming NO(2). The DRIFT spectra revealed that the surface speciation evolved differently in the presence of NO as compared with in O(2) or Ar. It is proposed that oxygen scavenging by NO depletes the Ni(3)(NO(3))(2)(OH)(4) phase of nitrate groups, creating nucleation sites for the formation of NiO, which leads to very small (similar to 4 nm) NiO particles and prevents agglomeration.

Original languageEnglish
Pages (from-to)7839-7845
Number of pages7
JournalJournal of Physical Chemistry C
Volume114
Issue number17
DOIs
Publication statusPublished - 06 May 2010

Keywords

  • HYDROGENATION
  • SPECTROSCOPY
  • METAL NITRATES
  • FISCHER-TROPSCH SYNTHESIS
  • THERMAL-DECOMPOSITION
  • COADSORPTION
  • DRYING STEP
  • CO
  • IMPREGNATION
  • PARTICLE-SIZE

Cite this

Wolters, M., Daly, H., Goguet, A., Meunier, F. C., Hardacre, C., Bitter, J. H., de Jongh, P. E., & de Jong, K. P. (2010). DRIFTS/MS/Isotopic Labeling Study on the NO-Moderated Decomposition of a Silica-Supported Nickel Nitrate Catalyst Precursor. Journal of Physical Chemistry C, 114(17), 7839-7845. https://doi.org/10.1021/jp910840k