TY - JOUR
T1 - Characterization of Silica-Supported Tungsten Bis- and Tris-hydrides by Advanced Solid-State NMR
AU - Wackerow, Wiebke
AU - Thiam, Zeynabou
AU - Abou-Hamad, Edy
AU - Almaksoud, Walid
AU - Hedhili, Mohamed N.
AU - Basset, Jean-Marie
N1 - KAUST Repository Item: Exported on 2021-06-07
Acknowledged KAUST grant number(s): BAS/1/1326-01-01.
Acknowledgements: We would like to acknowledge King Abdullah University of Science and Technology for funding. We also acknowledge KAUST NMR core lab for their continuous help. We acknowledge as well the KAUST Imaging Core Lab, particularly Dr. Alessandro Genovese.
PY - 2021/6/3
Y1 - 2021/6/3
N2 - Tungsten-hydrides supported on oxide supports are unique catalysts regarding the direct transformation of ethylene to propylene, alkane metathesis, and the low-temperature hydrogenolysis of waxes to lower molecular paraffins. The number of hydrides coordinated to the tungsten center and their structure on the siliceous support with very high surface silica (KCC-1) is unknown. KCC-1(700) silica of extremely high surface area allows for a high tungsten metal loading of 14 wt %. We show here the full characterization of supported tungsten bis- and tris-hydrides, which, after reaction with N2O gas, yield well-defined tungsten bis- and tris-hydroxide species on KCC-1(700). The obtained tungsten-hydroxide species are perfectly suitable for a detailed NMR study. The obtained tungsten hydroxo complexes are proven to be a tungsten bis-hydroxo and tungsten tris-hydroxo species. This analysis supports the conclusion that supported tungsten-hydride complexes coexist on the support as bis-hydride and tris-hydride species. They are, respectively, in close proximity to the silicon bis-hydride and the silicon mono-hydride. This proximity is explained by the mechanism of the formation of tungsten-hydride on the silica surface.
AB - Tungsten-hydrides supported on oxide supports are unique catalysts regarding the direct transformation of ethylene to propylene, alkane metathesis, and the low-temperature hydrogenolysis of waxes to lower molecular paraffins. The number of hydrides coordinated to the tungsten center and their structure on the siliceous support with very high surface silica (KCC-1) is unknown. KCC-1(700) silica of extremely high surface area allows for a high tungsten metal loading of 14 wt %. We show here the full characterization of supported tungsten bis- and tris-hydrides, which, after reaction with N2O gas, yield well-defined tungsten bis- and tris-hydroxide species on KCC-1(700). The obtained tungsten-hydroxide species are perfectly suitable for a detailed NMR study. The obtained tungsten hydroxo complexes are proven to be a tungsten bis-hydroxo and tungsten tris-hydroxo species. This analysis supports the conclusion that supported tungsten-hydride complexes coexist on the support as bis-hydride and tris-hydride species. They are, respectively, in close proximity to the silicon bis-hydride and the silicon mono-hydride. This proximity is explained by the mechanism of the formation of tungsten-hydride on the silica surface.
UR - http://hdl.handle.net/10754/669399
UR - https://pubs.acs.org/doi/10.1021/acs.jpcc.1c03625
U2 - 10.1021/acs.jpcc.1c03625
DO - 10.1021/acs.jpcc.1c03625
M3 - Article
SN - 1932-7447
JO - The Journal of Physical Chemistry C
JF - The Journal of Physical Chemistry C
ER -