a-AluminaCatalyst design Ethylene oxide Particle size effect a b s t r a c t Currently, for the industrial ethylene epoxidation a-alumina supported silver catalysts are the only catalyst of choice. We demonstrate a novel method to produce these catalysts with different silver particle sizes, but without changing other key parameters that may affect the catalytic performance such as support specific surface area or metal precursor. a-Alumina was impregnated with a silver oxalate solution, and was subsequently dried and treated in different gas atmospheres and at different temperatures to tune the silver particle sizes in the range of 20-500 nm. Particles of 20 nm exhibited a lower turnover frequency than particles of 70 nm and larger, which exhibit a constant turnover frequency, in accordance with results in literature. However, the selectivity, when measured at constant conversion, was particle size independent. This is the first time that the effect of the particle size on the selectivity of ethylene epoxidation is reported at constant conversion. This was made possible by a new method of producing supported silver catalysts, which we expect that is also applicable for silver catalysts with other supports and for the preparation of other supported metal catalysts.
Microreactors
present innovative solutions for problems pertaining
to conventional reactors and therefore have seen successful application
in several industrial processes. Yet, its application in heterogeneously
catalyzed gas–liquid reactions has been challenging, mainly
due to the lack of an easy and flexible methodology for catalyst incorporation
inside these reactors. Herein, we report a facile technique for obtaining
small (<2 nm) and well-distributed catalytic nanoparticles on the
walls of silica-coated capillaries, that act as micro(channel) reactors.
These particles are formed in situ on the reactor walls using polyelectrolyte
multilayers (PEMs), built by layer-by-layer self-assembly. Manipulating
the PEMs’ synthesis condition gives easy control over metal
loading, without compromising on particle size. Both monometallic
(Au and Pd) and bimetallic (AuPd) nanoparticles were successfully
obtained using this technique. Finally, these catalytic microreactors
were found to exhibit exceptional activity for the direct synthesis
of hydrogen peroxide from H2 and O2.
Silylation was employed on an active Au/Ti–SiO2 catalyst, in order to enhance catalyst performance for the direct epoxidation of propene to propene oxide (PO) using H2 and O2.
Due to the explosive nature of H 2 , O 2 and CH 4 mixtures, the concept of coupling in situ synthesis of H 2 O 2 with low-temperature single-step methane conversion to methanol has not received sufficient attention.This study aimed to investigate this process using a microchannel reactor, which offers the opportunity to explore the process under a wide range of concentrations. Direct methane activation with in situ generation of H 2 O 2 was successfully demonstrated in a microcapillary containing Au-Pd nanoparticles embedded on its silica-coated walls. The effect of H 2 , O 2 and CH 4 partial pressures, H 2 /O 2 molar ratio, gas-to-liquid (G/L) ratio and liquid phase weight-hourly-space-velocity (WHSV) on the productivity and product distribution was investigated. CH 4 partial pressure had the most significant effect on the productivity, while H 2 and O 2 partial pressures influenced the productivity less. The methane activation rate was found to be correlated with the H 2 O 2 formation rate. With only O 2 or pre-formed stabilized H 2 O 2 methane activation was not found, in situ H 2
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