A pressurized flow reactor combustion experiment interfaced with synchrotron double imaging photoelectron photoion coincidence spectroscopy

Hoener, Martin; Kaczmarek, Dennis; Bierkandt, Thomas; Bodi, Andras; Hemberger, Patrick; Kasper, Tina

doi:10.1063/1.5141168

Cited by 9 publications

(10 citation statements)

References 53 publications

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“…The i 2 PEPICO setup is also described by Sztáray et al 36 . and Hoener et al 37 . for photolysis and pyrolysis experiments to study reaction kinetics and a new high‐pressure reactor experiment, respectively.…”

Section: Methodsmentioning

confidence: 99%

“…Except for the nbutane/H 2 flame, the i 2 PEPICO setup 35,36 was used for the investigation of the flames. The i 2 PEPICO setup is also described by Sztáray et al 36 and Hoener et al 37 for photolysis and pyrolysis experiments to study reaction kinetics and a new high-pressure reactor experiment, respectively. A schematic sketch of this setup is shown in Figure S1 in the Supporting Information.…”

Section: Investigated Flamesmentioning

confidence: 99%

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Observation of low‐temperature chemistry products in laminar premixed low‐pressure flames by molecular‐beam mass spectrometry

Bierkandt

Oßwald

Gaiser

et al. 2021

Int J of Chemical Kinetics

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The formation of typical low‐temperature oxidation products is observed in laminar premixed low‐pressure flames investigated by photoionization molecular‐beam mass spectrometry at the Swiss Light Source. The C1–C4 alkyl hydroperoxides can be identified in n‐butane‐ and 2‐butene‐doped hydrogen flames by their photoionization efficiency spectra at m/z 48, 62, 76, and 90. C1–C3 alkyl hydroperoxides are also observed in a propane‐doped hydrogen flame and in a neat propane flame. In addition, threshold photoelectron spectra reveal the presence of the alkyl hydroperoxides. In the 2‐butene/H2 flame, the photoionization spectrum at m/z 88 also enables the identification of butenyl hydroperoxides by comparison with calculated ionization energies of the alkenyl hydroperoxides and a literature spectrum. The low‐temperature species are formed close to the burner surface with maximum mole fractions at 0.25–0.75 mm above the burner. At 0.5 mm, even the methylperoxy radical (CH3OO) is measured for the first time in a laminar premixed flame. The rate of production analyses show that consumption of the hydroperoxyalkyl radicals results in the formation of cyclic ethers. In the n‐butane/H2 flame, ethylene oxide, oxetane, and methyloxirane are identified. Besides expected small oxygenated species, for example, formaldehyde or acetaldehyde, the larger C4 oxygenates butanone (C2H5COCH3) and 2,3‐butanedione (C4H6O2) are formed in the two C4 hydrocarbon‐doped hydrogen flames. Quantification of alkyl hydroperoxides with estimated photoionization cross sections based on the corresponding alcohols, which have similar photoelectron structures to the alkyl hydroperoxides, shows that mole fractions are on the order of 10−5–10−6 in the n‐butane/H2 flame. Measurements are corroborated by simulations, which also predict the presence of some peroxides in detectable concentrations, that is, mole fractions larger than 10−7, under the investigated conditions. The observation of peroxide species and cyclic ethers in the investigated laminar premixed flames give new insights into the contribution of low‐temperature combustion chemistry in a flame.

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Section: Methodsmentioning

confidence: 99%

Section: Investigated Flamesmentioning

confidence: 99%

Observation of low‐temperature chemistry products in laminar premixed low‐pressure flames by molecular‐beam mass spectrometry

Bierkandt

Oßwald

Gaiser

et al. 2021

Int J of Chemical Kinetics

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“…54 These benefits make double imaging PEPICO an attractive analytical tool to interface to a wide variety of sources (Figure 1(d)) from a supersonic expansion source to study cold and weakly bound systems, 73 through pyrolysis microreactors to reveal unimolecular thermal decomposition processes, 74 as well as bimolecular chemistry, 68 microwave discharge flow tube reactors, 75 flames, 69,70 and shock tubes, 76 to pressurized flow reactors. 77…”

Section: Spectroscopic Toolsmentioning

confidence: 99%

“…As a result, more radicals are formed, and the experiments allow the investigation of the complex interplay between the fuel decomposition and the radical pool on the one hand and pollutant formation from combustion intermediates on the other hand. 77 4.3. Ignition Chemistry.…”

Section: Clean Combustionmentioning

confidence: 99%

“…The chemical complexity increases because flames reach much higher temperatures than can be achieved in reactor experiments. As a result, more radicals are formed, and the experiments allow the investigation of the complex interplay between the fuel decomposition and the radical pool on the one hand and pollutant formation from combustion intermediates on the other hand …”

Section: Clean Combustionmentioning

confidence: 99%

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Photoelectron Photoion Coincidence Spectroscopy Provides Mechanistic Insights in Fuel Synthesis and Conversion

et al. 2021

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Clean combustion, i.e., the reduction of NOx and soot emissions, and carbon neutrality, achieved in part by biofuel synthesis, are major milestones in the transition to a sustainable future. To overcome empiric and time-consuming process optimization steps, we need detailed reaction mechanistic and chemical insights on these processes. Be it in combustion or in catalysis, highly reactive intermediates, such as radicals, carbenes, and ketenes drive chemical reactions. Knowing the fate of these species helps develop strategies to optimize chemical energy conversion processes. This calls for advanced mass spectrometric tools, which enable the detection of transient species. In this review, we report on the application of state-of-the-art photoelectron photoion coincidence (PEPICO) spectroscopy with vacuum ultraviolet (VUV) synchrotron radiation as advanced diagnostic tools in catalysis and combustion research. We discuss reaction mechanisms in biomass conversion to sustainable fuels, where we report on the pyrolysis of wood samples probed using VUV photoionization mass spectrometry (PIMS) and obtain deep mechanistic insights in the (non)catalytic pyrolysis of lignin model compounds with PEPICO detection. PEPICO is also shown to contribute to the mechanistic understanding of catalysis by unveiling catalytic alkane valorization mechanisms. We discuss how PEPICO detection advances combustion diagnostics, thanks to the application of photoelectron spectroscopy and velocity map imaging. We report on mechanistic aspects of ignition, such as fuel radical formation and oxidation to peroxy species, and discuss reaction pathways of pollutant formation. In addition, we zoom into the elementary reactions of combustion and discuss isomer-selective kinetics experiments on radical oxidation. Newly revealed reaction pathways to polycyclic aromatic hydrocarbon (PAH) formation are also detailed. Finally, we describe current instrumental developments to improve PEPICO detection and report on innovative sources, reactors, and reaction sampling approaches to be combined with this technique.

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Pyrolysis of ethanol studied in a new high-repetition-rate shock tube coupled to synchrotron-based double imaging photoelectron/photoion coincidence spectroscopy

Nagaraju

Tranter

Ardila

et al. 2021

Combustion and Flame

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A pressurized flow reactor combustion experiment interfaced with synchrotron double imaging photoelectron photoion coincidence spectroscopy

Abstract: A pressurized flow reactor combustion experiment interfaced with synchrotron double imaging photoelectron photoion coincidence spectroscopy, Rev. Sci. Instrum. 91 (2020) 045115.

Cited by 9 publications

References 53 publications

Observation of low‐temperature chemistry products in laminar premixed low‐pressure flames by molecular‐beam mass spectrometry

Observation of low‐temperature chemistry products in laminar premixed low‐pressure flames by molecular‐beam mass spectrometry

Photoelectron Photoion Coincidence Spectroscopy Provides Mechanistic Insights in Fuel Synthesis and Conversion

Pyrolysis of ethanol studied in a new high-repetition-rate shock tube coupled to synchrotron-based double imaging photoelectron/photoion coincidence spectroscopy

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