https://www.lehigh.edu/operando/Publications/2005%20Recent%20Conceptual%20Advances%20in%20Catalysis.pdf

Recent conceptual advances in the catalysis science of mixed metal oxide catalytic materials

Heterogeneous metal oxide catalysts are widely studied for the aerobic oxidations of C1–C4 alkanes to form olefins and oxygenates. In this review, we outline the properties of supported metal oxides, mixed-metal oxides, and zeolites and detail their most common applications as catalysts for partial oxidations of light alkanes. By doing this we establish similarities between different classes of metal oxides and identify common themes in reaction mechanisms and research strategies for catalyst improvement. For example, almost all partial alkane oxidations, regardless of the metal oxide, follow Mars–van Krevelen reaction kinetics, which utilize lattice oxygen atoms to reoxidize the reduced metal centers while the gaseous O2 reactant replenishes these lattice oxygen vacancies. Many of the most-promising metal oxide catalysts include V5+ surface species as a necessary constituent to convert the alkane. Transformations involving sequential oxidation steps (i.e., propane to acrylic acid) require specific reacti...

Aerobic Oxidations of Light Alkanes over Solid Metal Oxide Catalysts

The molecular aspect of the Raman vibrational selection rules allows for the molecular structural and reactivity determinations of metal oxide catalytic active sites in all types of oxide catalyst systems (supported metal oxides, zeolites, layered hydroxides, polyoxometalates (POMs), bulk pure metal oxides, bulk mixed oxides and mixed oxide solid solutions). The molecular structural and reactivity determinations of metal oxide catalytic active sites are greatly facilitated by the use of isotopically labeled molecules. The ability of Raman spectroscopy to (1) operate in all phases (liquid, solid, gas and their mixtures), (2) operate over a very wide temperature (−273 to >1000 °C) and pressure (UHV to ≫100 atm) range, and (3) provide molecular level information about metal oxides makes Raman spectroscopy the most informative characterization technique for understanding the molecular structure and surface chemistry of the catalytic active sites present in metal oxide heterogeneous catalysts. The recent use of hyphenated Raman spectroscopy instrumentation (e.g., Raman–IR, Raman–UV-vis, Raman–EPR) and the operando Raman spectroscopy methodology (e.g., Raman–MS and Raman–GC) is allowing for the establishment of direct structure–activity/selectivity relationships that will have a significant impact on catalysis science in this decade. Consequently, this critical review will show the growth in the use of Raman spectroscopy in heterogeneous catalysis research, for metal oxides as well as metals, is poised to continue to exponentially grow in the coming years (173 references).

Monitoring surface metal oxide catalytic active sites with Raman spectroscopy

Selective oxidation of light alkanes: interaction between the catalyst and the gas phase on different classes of catalytic materials

Bulk mixed oxide catalysts are widely used for various applications (selective oxidation catalysts, electrocatalysts for solid oxide fuel cells, and solid oxide electrolyzers for the production of hydrogen), but fundamental understanding of their structure–performance relationships have lagged in the literature. The absence of suitable surface composition and surface structural characterization techniques and methods to determine the number of catalytic active sites, with the latter needed for determination of specific reaction rates (e.g., turnover frequency (1/s)), have hampered the development of sound fundamental concepts in this area of heterogeneous catalysis. This Perspective reviews the traditional concepts that have been employed to explain catalysis by bulk mixed oxides (molybdates, vanadates, spinels, perovskites, and several other specific mixed oxide systems) and introduces a modern perspective to the fundamental surface structure–activity/selectivity relationships for bulk mixed oxide cataly...

Catalysis Science of Bulk Mixed Oxides

Bulk crystallinity of vanadyl(IV) pyrophosphate catalysts forn-butane partial oxidation increased up to 23 days on stream as determined by XRD and Raman spectroscopy, while selectivity reached steady state after 8–10 days. Electron microscopy detected a 15 A amorphous layer terminating the (200) planes of (VO)2P2O7 in fresh catalysts that was not observed in the equilibrated catalysts. It is suggested that ordering of (200) planes at the surface of (VO)2P2O7 is responsible for selective oxidation.

/pdf/evolution-of-the-active-surface-of-the-vanadyl-pyrophosphate-43mbo49rby.pdf

Evolution of the active surface of the vanadyl pyrophosphate catalysts

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Evolution of the active surface of the vanadyl pyrophosphate catalysts