Johan Zetterberg

Simultaneous PIV/PH-PLIF, Rayleigh thermometry/OH-PLIF and stereo PIV measurements in a low-swirl-flame

The diagnostic techniques for simultaneous velocity and relative OH distribution, simultaneous temperature and relative OH distribution, and three component velocity mapping are described. The data extracted from the measurements include statistical moments for inflow fluid dynamics, temperature, conditional velocities, and scalar flux. The work is a first step in the development of a detailed large eddy simulation (LES) validation database for a turbulent, premixed flame. The low-swirl burner used in this investigation has many of the necessary attributes for LES model validation, including a simplified interior geometry; it operates well into the thin reaction zone for turbulent premixed flames, and flame stabilization is based entirely on the flow field and not on hardware or pilot flames.

Applications of a single-longitudinal-mode alexandrite laser for diagnostics of parameters of combustion interest

We report on the applications of a single-longitudinal-mode (SLM) pulsed alexandrite laser system for diagnostics of parameters of flow/combustion interest. The laser system is characterized by its narrow linewidth, high peak power, and broad tunablity. The absolute frequency of the laser output was monitored by a wavelength diagnostic system, which included a high-resolution confocal etalon and a molecular iodine laser-induced fluorescence (LIF) detection system. Different nonlinear frequency conversion schemes were used to cover a large frequency range from the infrared to the deep UV. The versatility of the laser system for flow/combustion diagnostics is demonstrated in three applications, namely filtered Rayleigh scattering, high-resolution Doppler-free two-photon LIF of CO, and infrared LIF and polarization spectroscopy of CO2. The potential impacts of using this SLM laser system in laser flow/combustion diagnostic applications are discussed.

Midinfrared polarization spectroscopy of OH and hot water in low pressure lean premixed flames

The application of midinfrared polarization spectroscopy (mid-IRPS) is demonstrated for sensitive detection of minor molecular species in combustion environments by probing rovibrational transitions. High resolution mid-IRPS spectra of low pressure flames were obtained in the spectral range around 3 microm. Rotational lines of the fundamental vibrational band of the hydroxyl radical (OH) were fully resolved and properly assigned among the abundant hot water lines in the flame mid-IRPS spectra. The high signal-to-noise ratio of the recorded OH lines indicates the feasibility of sensitive mid-IRPS OH detection. This constitutes, to the best of our knowledge, the first reported OH flame detection in the midinfrared spectral range. A simulation of hot water mid-IRPS lines with molecular parameters extracted from the HITRAN/HITEMP database was performed and compared with the observed flame spectra. The proper prediction of the hot water lines may help to clarify the potential spectral interferences associated with minor species measurements.

An in situ set up for the detection of CO(2) from catalytic CO oxidation by using planar laser-induced fluorescence.

We report the first experiment carried out on an in situ setup, which allows for detection of CO(2) from catalytic CO oxidation close to a model catalyst under realistic reaction conditions by the means of planar laser-induced fluorescence (PLIF) in the mid-infrared spectral range. The onset of the catalytic reaction as a function of temperature was followed by PLIF in a steady state flow reactor. After taking into account the self-absorption of CO(2), a good agreement between the detected CO(2) fluorescence signal and the CO(2) mass spectrometry signal was shown. The observed difference to previously measured onset temperatures for the catalytic ignition is discussed and the potential impact of IR-PLIF as a detection technique in catalysis is outlined.

Real-Time Gas-Phase Imaging over a Pd(110) Catalyst during CO Oxidation by Means of Planar Laser-Induced Fluorescence

The gas composition surrounding a catalytic sample has direct impact on its surface structure, which is essential when in situ investigations of model catalysts are performed. Herein a study of the gas phase close to a Pd(110) surface during CO oxidation under semirealistic conditions is presented. Images of the gas phase, provided by planar laser-induced fluorescence, clearly visualize the formation of a boundary layer with a significantly lower CO partial pressure close to the catalytically active surface, in comparison to the overall concentration as detected by mass spectrometry. The CO partial pressure variation within the boundary layer will have a profound effect on the catalysts’ surface structure and function and needs to be taken into consideration for in situ model catalysis studies.

Two-dimensional temperature measurements in flames using filtered Rayleigh scattering at 254 nm

Two-dimensional temperature measurements using filtered Rayleigh scattering (FRS) have been demonstrated. A tunable single-longitudinal-mode alexandrite laser was employed to provide the tunable narrow-line-width ultraviolet laser beam at 254 nm. Isotopic-enhanced mercury was utilized as an ultraviolet atomic filter. The strong absorption of the filter enabled effective suppression of elastic background. The transmission curve of the mercury filter was characterized by combining experimental measurements and proper modeling. The Rayleigh–Brillouin spectral profiles were calculated employing the S6 model. Quantitative interpretations of two-dimensional FRS signals were performed in both premixed and diffusion flames. The temperature values obtained were in good agreement with adiabatic calculations and earlier measurements.

Spatially and temporally resolved gas distributions around heterogeneous catalysts using infrared planar laser-induced fluorescence

Visualizing and measuring the gas distribution in close proximity to a working catalyst is crucial for understanding how the catalytic activity depends on the structure of the catalyst. However, existing methods are not able to fully determine the gas distribution during a catalytic process. Here we report on how the distribution of a gas during a catalytic reaction can be imaged in situ with high spatial (400 μm) and temporal (15 μs) resolution using infrared planar laser-induced fluorescence. The technique is demonstrated by monitoring, in real-time, the distribution of carbon dioxide during catalytic oxidation of carbon monoxide above powder catalysts. Furthermore, we demonstrate the versatility and potential of the technique in catalysis research by providing a proof-of-principle demonstration of how the activity of several catalysts can be measured simultaneously, either in the same reactor chamber, or in parallel, in different reactor tubes.

Single-shot imaging of ground-state hydrogen atoms with a nonlinear laser spectroscopic technique

We report on a novel nonlinear laser spectroscopic technique for single-shot imaging of ground-state hydrogen atoms in harsh environments. H atoms from the ground state were first pumped to the 2s state via a two-photon excitation with a 243 nm laser beam, and the population of the 2s state was further probed through the 2s-4p transition with conventional polarization spectroscopy at 486 nm. A single Nd:YAG-pumped optical parametric oscillator laser system was enough to provide both laser beams. Single-shot visualization of native H atoms in an atmospheric pressure premixed H(2)/O(2) flame is demonstrated.

2D and 3D imaging of the gas phase close to an operating model catalyst by planar laser induced fluorescence

In recent years, efforts have been made in catalysis related surface science studies to explore the possibilities to perform experiments at conditions closer to those of a technical catalyst, in particular at increased pressures. Techniques such as high pressure scanning tunneling/atomic force microscopy (HPSTM/AFM), near ambient pressure x-ray photoemission spectroscopy (NAPXPS), surface x-ray diffraction (SXRD) and polarization-modulation infrared reflection absorption spectroscopy (PM-IRAS) at semi-realistic conditions have been used to study the surface structure of model catalysts under reaction conditions, combined with simultaneous mass spectrometry (MS). These studies have provided an increased understanding of the surface dynamics and the structure of the active phase of surfaces and nano particles as a reaction occurs, providing novel information on the structure/activity relationship. However, the surface structure detected during the reaction is sensitive to the composition of the gas phase close to the catalyst surface. Therefore, the catalytic activity of the sample itself will act as a gas-source or gas-sink, and will affect the surface structure, which in turn may complicate the assignment of the active phase. For this reason, we have applied planar laser induced fluorescence (PLIF) to the gas phase in the vicinity of an active model catalysts. Our measurements demonstrate that the gas composition differs significantly close to the catalyst and at the position of the MS, which indeed should have a profound effect on the surface structure. However, PLIF applied to catalytic reactions presents several beneficial properties in addition to investigate the effect of the catalyst on the effective gas composition close to the model catalyst. The high spatial and temporal resolution of PLIF provides a unique tool to visualize the on-set of catalytic reactions and to compare different model catalysts in the same reactive environment. The technique can be applied to a large number of molecules thanks to the technical development of lasers and detectors over the last decades, and is a complementary and visual alternative to traditional MS to be used in environments difficult to asses with MS. In this article we will review general considerations when performing PLIF experiments, our experimental set-up for PLIF and discuss relevant examples of PLIF applied to catalysis.

Comparison of AP-XPS and PLIF Measurements during CO Oxidation over Pd Single Crystals

The interaction between the gas-phase molecules and a catalyst surface is crucial for the surface structure and are therefore important to consider when the active phase of a catalyst is studied. In this study we have used two different techniques to study the gas phase during CO oxidation over Pd single crystals. Gas-phase imaging by planar laser-induced fluorescence (PLIF) shows that a spherical boundary layer with a decreasing gradient of CO2 concentration out from the surface, is present close to the surface when the Pd crystal is highly active. Within this boundary layer the gas composition is completely different than that detected at the outlet of the chamber. The PLIF images of the gas-phase distribution are used to achieve a better understanding of the gas composition between the surface and the detector of a set-up for ambient pressure X-ray photoelectron spectroscopy (AP-XPS), a common technique for surface structure determination of model catalysts. The results show that also the gas-phase peaks present in the AP-XPS spectra truly represent the gas closest to the surface, which facilitates the interpretation of the AP-XPS spectra and thereby also the understanding of the mechanism behind the reaction process.