Water Formation Kinetics on Co(0001) at Low and Near-Ambient Hydrogen Pressures in the Context of Fischer-Tropsch Synthesis

Understanding the kinetics of oxygen removal from catalytically active metal surfaces by hydrogen is important for several catalytic reactions such as Fischer-Tropsch synthesis, methanation of CO or CO2, and the reverse-water-gas-shift reaction. Motivated by FTS, a Co(0001) single crystal model catalyst was used to study the kinetics of oxygen removal through reaction with hydrogen. Kinetic studies in the 10-7 - 10-4 mbar H2 pressure regime show that water formation is first order in the surface hydrogen concentration while the order in oxygen concentration changes from one at low oxygen coverage to zero at high oxygen coverage. In situ XPS shows that the hydrogen surface concentration saturates around 10-1 mbar and on this basis the typical temperature of 450K needed for water formation in this pressure regime can be considered as typical for high pressures as well. The absence of OH buildup during the reaction points to O + H as the rate-limiting step, with a barrier of -120 kJ mol-1. Such a high barrier shows that slow removal of adsorbed oxygen from the surface of reactive metal catalysts such as cobalt may be rate-limiting for the overall reaction

Overview of tokamak turbulence stabilization by fast ions

Tokamak experiments and modelling have in recent years increasingly indicated that the interaction between suprathermal (fast) ions and thermal plasma can lead to a reduction of turbulence and improvement of confinement. The regimes in which this stabilization occurs are of relevance to burning plasmas, and their understanding will inform reactor scenario optimization. This review summarizes observations, simulations, theoretical understanding, and open questions on this emerging topic

Post-plasma Quenching to Improve Conversion and Energy Efficiency in a CO2 Microwave Plasma

Transforming CO2 into value-added chemicals is crucial to realizing a carbon–neutral economy, and plasma-based conversion, a Power-2-X technology, offers a promising route to realizing an efficient and scalable process. This paper investigates the effects of post-plasma placement of a converging–diverging nozzle in a vortex-stabilized 2.45 GHz CO2 microwave plasma reactor to increase energy efficiency and conversion. The CDN leads to a 21% relative increase in energy efficiency (31%) and CO2 conversion (13%) at high flow rates and near-atmospheric conditions. The most significant performance improvement was seen at low flow rates and sub-atmospheric pressure (300 mbar), where energy efficiency was 23% and conversion was 28%, a 71% relative increase over conditions without the CDN. Using CFD simulations, we found that the CDN produces a change in the flow geometry, leading to a confined temperature profile at the height of the plasma, and forced extraction of CO to the post-CDN region

Reducing tin droplet ejection from capillary porous structures under hydrogen plasma exposure in Magnum-PSI

Liquid metal based divertors could be a more robust alternative to a solid tungsten design for DEMO. The liquid is confined in a sponge-like tungsten layer, called a capillary porous structure (CPS). It has been found previously that under certain conditions, many tin droplets eject from a CPS when it is brought into contact with a hydrogen plasma. These would present a contamination issue for the plasma core. Stability analysis suggests that droplet ejection can be suppressed by reduction of the pore size. To test this, stainless-steel CPS targets with pore size ranging from 0.5-100um filled with tin were exposed to identical loading conditions. This was done in the linear plasma device Magnum-PSI, capable of reaching divertor relevant plasma conditions. Furthermore, the influence of the CPS manufacturing techniques is considered by comparing the performance of a 3D printed, a mesh felts and a sintered CPS, all made from tungsten. Each target was surrounded by four witness plates, which were analysed post-mortem for Sn content by Rutherford backscattering. During plasma exposure, tin droplets were observed using a fast visible camera and plasma light emission via survey optical emission spectroscopy. The results imply that Sn erosion can be reduced by a factor of 50 when reducing the pore size. Moreover, it highlights the importance of avoiding overfilling of CPS targets with Sn

A Modified Fokker–Planck Approach for a Complete Description of Vibrational Kinetics in a N2 Plasma Chemistry Model

The Fokker–Planck (FP) approach for the description of vibrational kinetics is extended in order to include multiquanta transitions and time dependent solutions. Due to the importance of vibrational ladder climbing for the optimization of plasma-assisted nitrogen fixation, nitrogen is used as a test case with a comprehensive set of elementary processes affecting the vibrational distribution function (VDF). The inclusion of the vibrational energy equation is shown to be the best way to model transient conditions in a plasma reactor using the FP approach. Results are benchmarked against results from the widely employed state-to-state (STS) approach for a wide parameters range. STS and FP solutions agree within ∼10% for the lowest vibrational levels, while time dependent VDFs are in agreement with the STS solution within a ∼ 5% error. Using the FP approach offers the possibility to parametrize drift and diffusion coefficients in energy space as a function of vibrational and gas temperature, providing intuitive and immediate insights into energy transport within the vibrational manifold.</p

First-principles study of the magnetic exchange forces between the RuO2(110) surface and Fe tip

Magnetic exchange force microscopy (MExFM) is an important experimental technique for mapping the magnetic structure of surfaces with atomic resolution relying on the spin-dependent short-range exchange interaction between a magnetic tip and a magnetic surface. RuO2 is a significant compound with applications in heterogeneous catalysis and electrocatalysis. It has been characterized recently as an antiferromagnetic (AFM) material, and its magnetism has been predicted somewhat surprisingly to play an important role in its catalytic properties. In the current study, we explore theoretically whether MExFM can visualize the magnetic surface structure of RuO2. We use density functional theory (DFT) calculations to extract the exchange interactions between a ferromagnetic Fe tip interacting with an AFM RuO2(110) surface, as a function of tip-surface distance and the position of the tip over the surface. Mimicking the MExFM experiment, these data are then used to calculate the normalized frequency shift of an oscillating cantilever tip versus the minimum tip-surface distance, and construct corrugation height line profiles. It is found that the exchange interaction between tip and surface is strongest for a parallel configuration of the spins of the tip and of the surface; it is weakest for an anti-parallel orientation. In a corrugation profile, this gives rise to a sizable height difference of 25 pm between the spin-up and spin-down Ru atoms in the RuO2(110) surface at a normalized frequency shift y=−10.12 fNm1/2. The O atoms in the surface are not or hardly visible in the corrugation profile

The X-Point radiating regime at ASDEX Upgrade and TCV

Future fusion reactors require a safe, steady-state divertor operation. With deep divertor detachment, which is typically induced by impurity seeding, the radiation concentrates in a small region at the X-point or on closed flux surfaces above the X-point. This so-called X-point radiator (XPR) moves further inside the confined region with increasing seeding and the location can be actively controlled. At AUG, the parameter space for operation with an XPR was significantly extended, using active feedback on the XPR location. The XPR is observed in nearly the whole operational space of AUG in the high-densities or high collisionality regime. ELM suppression is consistently observed in all cases where the XPR was moved to a significant height above the X-point. Direct measurements of density and temperature from the region around the XPR using the new divertor Thomson scattering system at AUG indicate that the temperature at the location of the XPR remains high (>30eV) and only the region towards the X-point cools down further. In this cold XPR core, the temperature reduces to about 1eV. An XPR is also observed in TCV by the injection of nitrogen as extrinsic impurity. This highlights that the wall material (W for AUG, C for TCV) or machine size does not play a significant role for the existence of the regime. However, the scenario appears to be less stable in TCV. First experiments show the necessity of an active control for the XPR: Depending on the wall conditions and the nitrogen wall storage, the required nitrogen seeding level to achieve an XPR changes. Both, the low temperatures measured radially outside of the radiation zone at AUG, and the lower stability of the XPR regime at TCV with the presence of carbon are consistent with the predictions of a one-dimensional model of the XPR. However, the model would predict the development of the cold XPR core, and significant radiation at the X-point might already exist before reaching this cold temperature solution

Fast simultaneous estimation of nD transport coefficients and source function in perturbation experiments

In the calculation of transport coefficients from experimental data precise knowledge of the source is usually assumed, while the identification of the coefficients focuses on specific geometries and one spatial variable. This paper presents a method for the simultaneous estimation of both the distributions of transport coefficients as well as the source profile. A convex solution of the inverse problem is retained which makes the calculations highly computational efficient. Moreover, this allows for the estimation of multi-dimensional transport coefficients, source terms, and the analysis of the effect of regularization on experimental data and transport coefficient distributions. &nbsp;</p