Physical effects, such as electromagnetic waves, plasma, electric potential, electric/magnetic fields and mechanical strain, can efficiently promote heterogeneous catalysis beyond catalyst design.
The acceleration
of Faradaic reactions by oscillating electric
potentials has emerged as a viable tool to enhance electrocatalysis,
but the non-Faradaic dynamic promotion of thermal catalytic processes
remains to be proven. Here, we present experimental evidence showing
that oscillating potentials are capable of enhancing the rate of ethylene
hydrogenation despite no promotion effect being observed under static
potentials. The non-Faradaic dynamic enhancement reaches up to 553%
on a Pd/C electrode when cycling between −0.25 and 0.55 V
NHE
under optimized conditions with a frequency of around 0.1
Hz and a duty cycle of 99%. Under those conditions, the catalytic
reaction rates were promoted beyond the rate of charge transfer to
the electrode surface, confirming the non-Faradaic nature of the process.
Experiments in different electrolytes reveal a good correlation between
the catalytic enhancement and the double-layer capacitance, a measure
for the interfacial electric field strength. Preliminary kinetic data
is consistent with cyclic removal of adsorbates from the surface at
negative potential and the subsequent adsorption of H
2
and
C
2
H
4
and hydrogenation reaction at the positively
polarized surface.
The electrocatalytic reductive amination (ERA) offers an attractive way to make organonitrogen chemicals from renewable feedstock. Here, we report carbon nanotube (CNT) as an effective catalyst for the ERA of...
The acceleration of Faradaic reactions by oscillating electric potentials has emerged as a viable tool to enhance
electrocatalysis, but the non-Faradaic dynamic promotion of thermal catalytic processes remains to be proven.
Here, we present experimental evidence showing that oscillating potentials are capable of enhancing the rate of
ethylene hydrogenation despite no promotion effect was observed under static potentials. The non-Faradaic
dynamic enhancement reaches up to 553% on a Pd/C electrode when cycling between –0.25 VNHE and 0.55 VNHE
under optimized conditions with a frequency of around 0.1 Hz and a duty cycle of 99%. Under those conditions,
no stoichiometric electron transfer to ethylene can be observed, confirming the non-Faradaic nature of the process.
Experiments in different electrolytes reveal a good correlation between the catalytic enhancement and the doublelayer capacitance – a measure for the interfacial electric field strength. Preliminary kinetic data suggests that
cycling to a low potential increases the hydrogen adsorption on the catalyst surface while at higher potential, the
ethylene adsorption and hydrogenation becomes relatively more favorable<br>
We report a methodology based on applying oscillating potentials to various electrocatalytically active metal surfaces during the formic acid oxidation reaction. Moderate frequency oscillations (0.1 to 10 Hz) allow us to control the coverage of intermediates on the surface, thus enable quantifying the transient effects (on the time scale of up to 10−4 s) of coverage on the reaction rate. We determined different coverage-dependences of turnover frequencies for Pt metal plate and various carbon-supported metal nanoparticle catalysts (Pt/C, Pd/C and Rh/C). This method therefore constitutes a valuable and simple tool for the elucidation of adsorbate coverages on metal surfaces and their resulting catalytic performance. We also demonstrate that dynamic catalytic processes can be analyzed semi-quantitatively with this new approach allowing the design of catalytic processes under optimized conditions.<br>
Spheronization of cylindrical extrudates on a rotating friction plate involves breakage and rounding. Little attention has been given to the breakage stage and quantitative modeling of this process is scarce. Two simple models are compared with experimental data obtained for the early stages of spheronization of microcrystalline cellulose/water extrudates. Tests were conducted for different times (t), rotational speeds (ω), initial loadings, and on pyramidal friction plates with different dimensions. The first model, describing the number of pellets, validated ω 3 t as a characteristic time scale for the breakage stage. The kinetic parameters obtained by fitting showed a systematic dependence on plate dimensions expressed as a scaled gap width. The second model, a simple population balance, described the evolution of the number and length of pellets. The pseudo rate constants provided insights into the kinetics: extrudates tended to break near the middle, while breakage of smaller pellets was slowed down by more pellet-pellet collisions.
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