Enhanced Catalytic Probe Design for Mapping Radical Density in the Plasma Afterglow.

The electrification of chemical processes using plasma generates an increasing demand for sensors, monitoring concentrations of plasma-activated species such as radicals. Radical probes are a low-cost in situ method for spatially resolved quantification of the radical density in a plasma afterglow using the heat from the exothermal recombination of radicals on a catalytic surface. However, distinguishing recombination heating from other heat fluxes in the system is challenging.

Unraveling NO Production in N-O Plasmas with 0D Kinetic Modeling and Experimental Validation.

This work presents a detailed investigation aimed at understanding the key mechanisms governing nitric oxide (NO) production in N-O discharges by systematically comparing experimental results to modeling data. The experimental phase capitalizes on radiofrequency (13.56 MHz) discharges, sustained at 5 mbar pressure conditions, featuring varying concentrations of oxygen, ranging from pure N plasma to air-like mixtures.

Scaling up BiVO Photoanodes on Porous Ti Transport Layers for Solar Hydrogen Production.

Commercialization of photoelectrochemical (PEC) water-splitting devices requires the development of large-area, low-cost photoanodes with high efficiency and photostability. Herein, we address these challenges by using scalable fabrication techniques and porous transport layer (PTLs) electrode supports. We demonstrate the deposition of W-doped BiVO on Ti PTLs using successive-ionic-layer-adsorption-and-reaction methods followed by boron treatment and chemical bath deposition of NiFeOOH co-catalyst.

Observation and rationalization of nitrogen oxidation enabled only by coupled plasma and catalyst.

Heterogeneous catalysts coupled with non-thermal plasmas (NTP) are known to achieve reaction yields that exceed the contributions of the individual components. Rationalization of the enhancing potential of catalysts, however, remains challenging because the background contributions from NTP or catalysts are often non-negligible. Here, we first demonstrate platinum (Pt)-catalyzed nitrogen (N) oxidation in a radio frequency plasma afterglow at conditions at which neither catalyst nor plasma alone produces significant concentrations of nitric oxide (NO).

High-Throughput Computational Screening of Cubic Perovskites for Solid Oxide Fuel Cell Cathodes.

It is a present-day challenge to design and develop oxygen-permeable solid oxide fuel cell (SOFC) electrode and electrolyte materials that operate at low temperatures. Herein, by performing high-throughput density functional theory calculations, oxygen vacancy formation energy, , data for a pool of all-inorganic ABO and AABO cubic perovskites is generated. Using data of perovskites, the area-specific resistance (ASR) data, which is related to both oxygen reduction reaction activity and selective oxygen ion conductivity of materials, is calculated.

Electrochemical Activation of Atomic Layer-Deposited Cobalt Phosphate Electrocatalysts for Water Oxidation.

The development of efficient and stable earth-abundant water oxidation catalysts is vital for economically feasible water-splitting systems. Cobalt phosphate (CoPi)-based catalysts belong to the relevant class of nonprecious electrocatalysts studied for the oxygen evolution reaction (OER). In this work, an in-depth investigation of the electrochemical activation of CoPi-based electrocatalysts by cyclic voltammetry (CV) is presented.

Charge carrier dynamics and photocatalytic activity of {111} and {100} faceted AgPO particles.

Silver orthophosphate is a highly promising visible light photocatalyst with high quantum yield for solar driven water oxidation. Recently, the performance of this material has been further enhanced using facet-controlled synthesis. The tetrahedral particles with {111} exposed facets demonstrate higher photocatalytic performance than the cubic particles with {100} exposed facets.

Observation of Nanoparticle Exsolution from Perovskite Oxides: From Atomic Scale Mechanistic Insight to Nanostructure Tailoring.

Understanding and controlling the formation of nanoparticles at the surface of functional oxide supports is critical for tuning activity and stability for catalytic and energy conversion applications. Here, we use a latest generation environmental transmission electron microscope to follow the exsolution of individual nanoparticles at the surface of perovskite oxides, with ultrahigh spatial and temporal resolution. Qualitative and quantitative analysis of the data reveals the atomic scale processes that underpin the formation of the socketed, strain-inducing interface that confers exsolved particles their exceptional stability and reactivity.

Solar Hydrogen Generation from Ambient Humidity Using Functionalized Porous Photoanodes.

Solar hydrogen is a promising sustainable energy vector, and steady progress has been made in the development of photoelectrochemical (PEC) cells. Most research in this field has focused on using acidic or alkaline liquid electrolytes for ionic transfer. However, the performance is limited by (i) scattering of light and blocking of catalytic sites by gas bubbles and (ii) mass transport limitations.

Electrochemistry of Sputtered Hematite Photoanodes: A Comparison of Metallic DC versus Reactive RF Sputtering.

The water splitting activity of hematite is sensitive to the film processing parameters due to limiting factors such as a short hole diffusion length, slow oxygen evolution kinetics, and poor light absorptivity. In this work, we use direct current (DC) magnetron sputtering as a fast and cost-effective route to deposit metallic iron thin films, which are annealed in air to obtain well-adhering hematite thin films on F:SnO-coated glass substrates. These films are compared to annealed hematite films, which are deposited by reactive radio frequency (RF) magnetron sputtering, which is usually used for depositing metal oxide thin films, but displays an order of magnitude lower deposition rate.

Vibrational Kinetics in Plasma as a Functional Problem: A Flux-Matching Approach.

A new approach to calculate the vibrational distribution function of molecules in a medium providing energy for vibrational excitation is proposed and demonstrated. The approach is an improvement of solution methods based on the drift-diffusion Fokker-Planck (FP) equation for a double differentiable function representing the vibrational populations on a continuum internal energy scale. A self-consistent numerical solution avoids approximations used in previous analytical solutions.

Zeolites for CO-CO-O Separation to Obtain CO-Neutral Fuels.

Carbon dioxide release has become an important global issue due to the significant and continuous rise in atmospheric CO concentrations and the depletion of carbon-based energy resources. Plasmolysis is a very energy-efficient process for reintroducing CO into energy and chemical cycles by converting CO into CO and O utilizing renewable electricity. The bottleneck of the process is that CO remains mixed with O and residual CO.

Analysis of temporal evolution of quantum dot surface chemistry by surface-enhanced Raman scattering.

Temporal evolution of surface chemistry during oxidation of silicon quantum dot (Si-QD) surfaces were probed using surface-enhanced Raman scattering (SERS). A monolayer of hydrogen and chlorine terminated plasma-synthesized Si-QDs were spin-coated on silver oxide thin films. A clearly enhanced signal of surface modes, including Si-Clx and Si-Hx modes were observed from as-synthesized Si-QDs as a result of the plasmonic enhancement of the Raman signal at Si-QD/silver oxide interface.

Characterization of Nanocrystal Size Distribution using Raman Spectroscopy with a Multi-particle Phonon Confinement Model.

Analysis of the size distribution of nanocrystals is a critical requirement for the processing and optimization of their size-dependent properties. The common techniques used for the size analysis are transmission electron microscopy (TEM), X-ray diffraction (XRD) and photoluminescence spectroscopy (PL). These techniques, however, are not suitable for analyzing the nanocrystal size distribution in a fast, non-destructive and a reliable manner at the same time.

Surface modifications induced by high fluxes of low energy helium ions.

Several metal surfaces, such as titanium, aluminum and copper, were exposed to high fluxes (in the range of 10(23) m(-2) s(-1)) of low energy (<100 eV) Helium (He) ions. The surfaces were analyzed by scanning electron microscopy and to get a better understanding on morphology changes both top view and cross sectional images were taken. Different surface modifications, such as voids and nano pillars, are observed on these metals.

Nanostructuring of iron surfaces by low-energy helium ions.

The behavior of iron surfaces under helium plasma exposure is investigated as a function of surface temperature, plasma exposure time, and He ion flux. Different surface morphologies are observed for a large process parameter range and discussed in terms of temperature-related surface mechanisms. Surface modification is observed under low-He ion flux (in the range of 10(20) m(-2) s(-1)) irradiation, whereas fiberlike iron nanostructures are formed by exposing the surface to a high flux (in the range of 10(23) m(-2) s(-1)) of low-energy He ions at surface temperatures of 450-700 °C.