Investigation of Silica-Supported Vanadium Oxide Catalysts by High-Field 51 V Magic-Angle Spinning NMR

Jaegers, Nicholas R.; Wan, Chuan; Hu, Mary Y.; Vasiliu, Monica; Dixon, David A.; Walter, Eric; Wachs, Israel E.; Wang, Yong; Hu, Jian Zhi

doi:10.1021/acs.jpcc.7b01658

Title: Investigation of Silica-Supported Vanadium Oxide Catalysts by High-Field ⁵¹ V Magic-Angle Spinning NMR

Journal Article · Tue Mar 14 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b01658· OSTI ID:1399179

Jaegers, Nicholas R.; Wan, Chuan; Hu, Mary Y.; Vasiliu, Monica;

; Walter, Eric; Wachs, Israel E.; Wang, Yong;

Supported V2O5/SiO2 catalysts were studied using solid state 51V MAS NMR at a sample spinning rate of 36 kHz and at a magnetic field of 19.975 T for a better understanding of the coordination of the vanadium oxide as a function of environmental conditions . Structural transformations of the supported vanadium oxide species between the catalyst in the dehydrated state and hydrated state under an ambient environment were revisited to examine the degree of oligomerization and the effect of water. The experimental results indicate the existence of a single dehydrated surface vanadium oxide species that resonates at -675 ppm and two vanadium oxide species under ambient conditions that resonate at -566 and -610 ppm, respectively. No detectable structural difference was found as a function of vanadium oxide loading on SiO2 (3% V2O5/SiO2 and 8% V2O5/SiO2). Quantum chemistry simulations of the 51V NMR chemical shifts on predicted surface structures were used as an aide in understanding potential surface vanadium oxide species on the silica support. The results suggest the formation of isolated surface VO4 units for the dehydrated catalysts with the possibility of dimer and cyclic trimer presence. The absence of bridging V-O-V vibrations (~200-300 cm-1) in the Raman spectra [Gao et al. J. Phys. Chem. B 1998, 102, 10842-10852], however, indicates that the isolated surface VO4 sites are the dominant dehydrated surface vanadia species on silica. Upon exposure to water, hydrolysis of the bridging V-O-Si bonds is most likely responsible for the decreased electron shielding experienced by vanadium. No indicators for the presence of hydrated decavanadate clusters or hydrated vanadia gels previously proposed in the literature were detected in this study.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1399179

Report Number(s):: PNNL-SA-124184; 49339; KC0302010

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 11; ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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