Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH3.) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C2 and C1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.
Surface oxygen vacancy
can greatly affect the properties of transition-metal
oxides. However, engineering oxygen vacancy-abundant transition-metal
oxides with high specific surface area (SSA) remains challenging.
At present, the generation of oxygen vacancies in metal oxides is
time-consuming and less environmentally friendly by chemical leaching
methods that usually require additional waste treatment. Herein, a
series of oxygen vacancy-abundant transition-metal oxides with high
SSA are constructed via a lattice refining strategy. This strategy
is realized by urea-assisted ball milling pyrolysis and is green,
efficient, and universal. The oxygen vacancies promote the mobility
of oxygen, leading to a boosted catalytic oxidation performance of
aromatic sulfides. Such a strategy provides an efficient approach
to manufacturing oxygen vacancies on transition-metal oxides, which
may be beneficial for various related applications as an effective
catalytic material.
Efficient metal-free
carbon-based catalysts are of particular interest
due to their unique electronic structure and compositional variability.
Herein, petroleum-coke-based N,O-doped porous graphene (PG) was prepared
as a preferred alternative to metal catalysts for catalytic oxidative
reaction. Such a high specific surface area and heteroatom-rich structure
promote high exposure of active sites, regulating the electron delocalization
of materials effectively. In addition, the synergistic effect between
N-doped and oxygen-containing functional groups is beneficial for
the catalytic performance. As such, when employing the active PG as
catalyst for the catalytic oxidative desulfurization (ODS), aromatic
sulfur-containing compounds would be oxidized effectively and the
sulfur removal in real diesel reached 84%. This work develops a facile
approach for preparing heteroatoms co-doped porous graphene for aerobic
catalytic ODS as well as an effective design idea for high value-added
utilization of petroleum coke.
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