Plasma catalysis is gaining increasing interest for various gas conversion applications, such as CO2 conversion into value-added chemicals and fuels, CH4 activation into hydrogen, higher hydrocarbons or oxygenates, and NH3 synthesis. Other applications are already more established, such as for air pollution control, e.g. volatile organic compound remediation, particulate matter and NOx removal. In addition, plasma is also very promising for catalyst synthesis and treatment. Plasma catalysis clearly has benefits over ‘conventional’ catalysis, as outlined in the Introduction. However, a better insight into the underlying physical and chemical processes is crucial. This can be obtained by experiments applying diagnostics, studying both the chemical processes at the catalyst surface and the physicochemical mechanisms of plasma-catalyst interactions, as well as by computer modeling. The key challenge is to design cost-effective, highly active and stable catalysts tailored to the plasma environment. Therefore, insight from thermal catalysis as well as electro- and photocatalysis is crucial. All these aspects are covered in this Roadmap paper, written by specialists in their field, presenting the state-of-the-art, the current and future challenges, as well as the advances in science and technology needed to meet these challenges.
Plasma-enhanced catalytic
ammonia synthesis has been proposed as
an alternative pathway for green nitrogen fixation in the case of
medium- and small-scale operation. Recently, Mehta et al. [Nat. Catal.20181269275] postulated that plasma-induced vibrational
excitations of N2 decrease the dissociation barrier, without
influencing the subsequent hydrogenation reactions and ammonia desorption
at atmospheric conditions. In this paper, this postulation is substantiated
with experimental data of unpromoted and promoted, alumina-supported
ruthenium ammonia synthesis catalysts. Within the temperature regime
for plasma-enhanced catalytic ammonia synthesis over ruthenium-based
catalysts (>200 °C), synergy is experimentally observed between
the catalyst and the plasma by a lowered apparent activation energy.
While the apparent activation energy for thermal-catalytic ammonia
synthesis typically ranges from ∼60 to ∼115 kJ mol–1 depending on the promoters, the apparent activation
energy for plasma-enhanced catalytic ammonia synthesis ranges from
∼20 to ∼40 kJ mol–1, consistent with
the hypothesis that ammonia synthesis is enhanced via plasma-induced
vibrational excitations of N2. Further support follows
from the observation that the effects of promoters and supports on
activity are similar for thermal catalysis and plasma-enhanced catalysis.
As promoter and support influence activity via enhancing dissociation
of N2, it follows that breaking the N–N bond is
still relevant in plasma-enhanced catalytic ammonia synthesis.
We experimentally investigate drop impact dynamics onto different superhydrophobic surfaces, consisting of regular polymeric micropatterns and rough carbon nanofibers, with similar static contact angles. The main control parameters are the Weber number We and the roughness of the surface. At small We, i.e., small impact velocity, the impact evolutions are similar for both types of substrates, exhibiting Fakir state, complete bouncing, partial rebouncing, trapping of an air bubble, jetting, and sticky vibrating water balls. At large We, splashing impacts emerge forming several satellite droplets, which are more pronounced for the multiscale rough carbon nanofiber jungles. The results imply that the multiscale surface roughness at nanoscale plays a minor role in the impact events for small We less than or approximately equal 120 but an important one for large We greater than or approximately equal 120. Finally, we find the effect of ambient air pressure to be negligible in the explored parameter regime We less than or approximately equal 150.
IR spectroscopy has been an important tool for studying detailed interactions of reactants and reaction-intermediates with catalyst surfaces. Studying reactions in water is, however, far from trivial, due to the excessive absorption of infrared light by water. One way to deal with this is the use of Attenuated Total Reflection spectroscopy (ATR-IR) minimizing the path length of infrared light through the water. Moreover, ATR-IR allows for a direct comparison of reactions in gas and water on the same sample, which bridges the gap between separate catalyst investigations in gas and liquid phase. This tutorial review describes recent progress in using ATR-IR for studying heterogeneous catalysts in water. An overview is given of the important aspects to be taken into account when using ATR-IR to study heterogeneous catalysts in liquid phase, like the procedure to prepare stable catalyst layers on the internal reflection element. As a case study, CO adsorption and oxidation on noble metal catalysts is investigated with ATR-IR in gas and water. The results show a large effect of water and pH on the adsorption and oxidation of CO on Pt/Al(2)O(3) and Pd/Al(2)O(3). From the results it is concluded that water affects the metal particle potential as well as the adsorbed CO molecule directly, resulting in higher oxidation rates in water compared to gas phase. Moreover, also pH influences the metal particle potential with a clear effect on the observed oxidation rates. Finally, the future outlook illustrates that ATR-IR spectroscopy holds great promise in the field of liquid phase heterogeneous catalysis.
Ammonia is one of the most produced chemicals, mainly synthesized from fossil fuels for fertilizer applications. Furthermore, ammonia may be one of the energy carriers of the future, when it...
Evaporation of water droplets on a superhydrophobic substrate, on which the contact line is pinned, is investigated. While previous studies mainly focused on droplets with contact angles smaller than 90 • , here we analyze almost the full range of possible contact angles (10 • -150 • ). The greater contact angles and pinned contact lines can be achieved by the use of superhydrophobic Carbon Nanofiber substrates. The time-evolutions of the contact angle and the droplet mass are examined. The experimental data is in good quantitative agreement with the model presented by Popov (Physical Review E 71, 2005), demonstrating that the evaporation process is quasi-static, diffusion-driven, and that thermal effects play no role. Furthermore, we show that the experimental data for the evolution of both the contact angle and the droplet mass can be collapsed onto one respective universal curve for all droplet sizes and initial contact angles.
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