Experimental Confirmation of the Low‐Temperature Oxidation Scheme of Alkanes

Battin‐Leclerc, Frédérique; Herbinet, Olivier; Glaude, Pierre‐Alexandre; Fournet, René; Zhou, Zhongyue; Deng, Linhua; Guo, Huijun; Xie, Ming; Qi, Fei

doi:10.1002/ange.200906850

Cited by 29 publications

(23 citation statements)

References 23 publications

(24 reference statements)

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“…Due to the fragility of the RO-OH bond of hydroperoxides (the bond dissociation energy is around 43 kcal mol À1 ), ROOH can easily break and is usually present in trace amounts, which can hardly be measured (Battin-Leclerc, 2008). The hydroperoxides formed during the low-temperature oxidation of n-butane were firstly observed by our previous facility (Battin-Leclerc et al, 2010). In this work, the same experiment is repeated to test the performance of the new experimental setup.…”

Section: Hydroperoxides During Oxidation Of N-butane In Jet-stirred Rmentioning

confidence: 94%

“…Moreover, the isomers can be distinguished based on their different ionization energies by scanning their photoionization efficiency (PIE) spectra (Cool, McIlroy et al, 2005;Qi et al, 2006). The application of the molecular beam mass spectrometry with synchrotron VUV photoionization technique has achieved great success in this area, presenting sensitive and comprehensive measurements of components in combustion studies (Taatjes et al, 2005;Battin-Leclerc et al, 2010).…”

Section: Introductionmentioning

confidence: 99%

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The vacuum ultraviolet beamline/endstations at NSRL dedicated to combustion research

et al. 2016

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An undulator-based vacuum ultraviolet (VUV) beamline (BL03U), intended for combustion chemistry studies, has been constructed at the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China. The beamline is connected to the newly upgraded Hefei Light Source (HLS II), and could deliver photons in the 5-21 eV range, with a photon flux of 10(13) photons s(-1) at 10 eV when the beam current is 300 mA. The monochromator of the beamline is equipped with two gratings (200 lines mm(-1) and 400 lines mm(-1)) and its resolving power is 3900 at 7.3 eV for the 200 lines mm(-1) grating and 4200 at 14.6 eV for the 400 lines mm(-1) grating. The beamline serves three endstations which are designed for respective studies of premixed flame, fuel pyrolysis in flow reactor, and oxidation in jet-stirred reactor. Each endstation contains a reactor chamber, an ionization chamber where the molecular beam intersects with the VUV light, and a home-made reflectron time-of-flight mass spectrometer. The performance of the beamline and endstations with some preliminary results is presented here. The ability to detect reactive intermediates (e.g. H, O, OH and hydroperoxides) is advantageous in combustion chemistry research.

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Section: Hydroperoxides During Oxidation Of N-butane In Jet-stirred Rmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

The vacuum ultraviolet beamline/endstations at NSRL dedicated to combustion research

et al. 2016

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“…Another advanced VUV source provided by synchrotron radiation possesses unique properties of high energy resolution, high photon flux and easy photon energy tunability that make synchrotron VUV photoionization capable of minimizing fragmentation interference, detecting radicals and distinguishing isomers. Synchrotron VUV photoionization combined with molecular‐beam mass spectrometer, referred as SVUV‐PIMS, has been developed to be a powerful technique in the diagnosis of combustion flame and gas‐phase components in heterogeneous catalytic reactions …”

Section: Photoionization Mass Spectrometrymentioning

confidence: 99%

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

You

Huang

2019

ChemCatChem

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Heterogeneous catalytic reactions always involve surface intermediates on catalyst surfaces, and some of them also involve reactive and unstable gas-phase intermediates such as radicals and alkyl hydroperoxides. Online detection of these gas-phase intermediates is of great importance for fundamentally understanding reaction mechanisms of relevant heterogeneous catalytic reactions, designing structures of efficient catalysts and optimizing reactors. However, it has remained a long-time challenge due to the lack of routine characterization techniques. Herein we review recent progress on applications of photoionization mass spectrometry in online detection of reactive and unstable gas-phase intermediates in heterogeneous catalytic reactions. The development and advantages of photoionization mass spectrometry and the relevant equipment setup for heterogeneous catalysis studies are also described. Finally, a future perspective is given.[a] Dr. * (m/z = 15), C 2 H 5 * (m/z = 29) and allyl radical (CH 2 CHCH 2 * 4 5 6 7 8

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“…With alternative (bio)fuels, different species can occur in addition to the species pool from hydrocarbon combustion . Further diagnostic challenges arise in the low‐temperature ignition regime where numerous fuel‐specific labile oxygen‐rich intermediates occur—structures only recently detected experimentally . Exhaust gas recirculation will add potentially reactive CO 2 , H 2 O, and HC species to a fuel mixture.…”

Section: Diagnostics To Validate Chemical Mechanisms and Combustion mentioning

confidence: 99%

“…Observation of the species including radicals and labile oxygenated intermediates in low‐temperature oxidation and combustion is still in its early stages . The overview mass spectra in DME oxidation at 540 K of Moshammer et al .…”

Section: Opportunities For Diagnosticsmentioning

confidence: 99%

Combustion Chemistry Diagnostics for Cleaner Processes

Kohse‐Höinghaus

2016

Chemistry A European J

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Climate change, environmental problems, urban pollution, and the dependence on fossil fuels demand cleaner, renewable energy strategies. However, they also ask for urgent advances in combustion science to reduce emissions. For alternative fuels and new combustion regimes, crucial information about the chemical reactions from fuel to exhaust remains lacking. Understanding such relations between combustion process, fuel, and emissions needs reliable experimental data from a wide range of conditions to provide a firm basis for predictive modeling of practical combustion processes.

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Experimental Confirmation of the Low‐Temperature Oxidation Scheme of Alkanes

Cited by 29 publications

References 23 publications

The vacuum ultraviolet beamline/endstations at NSRL dedicated to combustion research

The vacuum ultraviolet beamline/endstations at NSRL dedicated to combustion research

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

Combustion Chemistry Diagnostics for Cleaner Processes

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