The prepared bifunctional Nb-OMS-2 catalysts are promising candidate in partial oxidation of methanol into dimethoxymethane at a lower temperature suggesting that there is an important temperature regime when forming active sites for DMM production.
A mesoporous
crystalline niobium oxide with tunable pore sizes
was synthesized via the sol–gel-based inverse micelle method.
The material shows a surface area of 127 m2/g, which is
the highest surface area reported so far for crystalline niobium oxide
synthesized by soft template methods. The material also has a monomodal
pore size distribution with an average pore diameter of 5.6 nm. A
comprehensive characterization of niobium oxide was performed using
powder X-ray diffraction, Brunauer–Emmett–Teller, thermogravimetric
analysis, scanning electron microscopy, transmission electron microscopy,
UV–vis, and X-ray photoelectron spectroscopy. The material
acts as an environmentally friendly, solid acid catalyst toward hydration
of alkynes under with excellent catalytic activity (99% conversion,
99% selectivity, and 4.39 h–1 TOF). Brønsted
acid sites present in the catalyst were found to be responsible for
the high catalytic activity. The catalyst was reusable up to five
cycles without a significant loss of the activity.
High-temperature oxidation mechanisms
of metallic nanoparticles
have been extensively investigated; however, it is challenging to
determine whether the kinetic modeling is applicable at the nanoscale
and how the differences in nanoparticle size influence the oxidation
mechanisms. In this work, we study thermal oxidation of pristine Ni
nanoparticles ranging from 4 to 50 nm in 1 bar 1%O2/N2 at 600 °C using in situ gas-cell environmental
transmission electron microscopy. Real-space in situ oxidation videos revealed an unexpected nanoparticle surface refacetting
before oxidation and a strong Ni nanoparticle size dependence, leading
to distinct structural development during the oxidation and different
final NiO morphology. By quantifying the NiO thickness/volume change
in real space, individual nanoparticle-level oxidation kinetics was
established and directly correlated with nanoparticle microstructural
evolution with specified fast and slow oxidation directions. Thus,
for the size-dependent Ni nanoparticle oxidation, we propose a unified
oxidation theory with a two-stage oxidation process: stage 1: dominated
by the early NiO nucleation (Avrami–Erofeev model) and stage
2: the Wagner diffusion-balanced NiO shell thickening (Wanger model).
In particular, to what extent the oxidation would proceed into stage
2 dictates the final NiO morphology, which depends on the Ni starting
radius with respect to the critical thickness under given oxidation
conditions. The overall oxidation duration is controlled by both the
diffusivity of Ni2+ in NiO and the Ni in Ni self-diffusion.
We also compare the single-particle kinetic curve with the collective
one and discuss the effects of nanoparticle size differences on kinetic
model analysis.
High‐valent molybdenum ions were substituted into the cobalt oxide lattice through a one step, sol‐gel method and investigated for selective synthesis of 2‐substituted benzimidazoles. Catalyst synthesis involves surfactant assisted soft templating inverse micelle method, which forms mesopores by interconnected intraparticle voids. Substitutional doping of Mo6+ resulted in materials with modified structural, morphological, surface, and redox properties. The catalytic activity increased with Mo concentration until an optimum amount (3 % Mo incorporation). Modified material shows lattice expansion, increased surface oxygen vacancies, and high surface area, which are responsible for the higher catalytic activity in selective benzimidazole synthesis reaction. A strong correlation between surface properties of the catalyst and the product selectivity was observed and plausible mechanistic and kinetic data are proposed and collected, respectively.
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