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

Zhou, Zhongyue; Du, Xuewei; Yang, Jiuzhong; Wang, Yizun; Li, Chaoyang; Shen, Wei; Du, Liangliang; Li, Yuyang; Qi, Fei; Wang, Qiuping

doi:10.1107/s1600577516005816

Cited by 169 publications

(97 citation statements)

References 49 publications

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“…The qualification was accomplished by scanning the photoionization efficiency (PIE) spectrum of a designated mass peak . The quantification was performed according to the ion signal intensities and photoionization cross‐sections of species . To realize the accurate quantification, the flow rate of MeOH vapour was calculated carefully by controlling two mass flow controllers (MFCs), not simply by the flow rate difference between the MFCs.…”

Section: Methodsmentioning

confidence: 99%

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

Wen

Zhou

et al. 2020

Angew Chem Int Ed

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HCHO has been confirmed as an active intermediate in the methanol‐to‐hydrocarbon (MTH) reaction, and is critical for interpreting the mechanisms of coke formation. Here, HCHO was detected and quantified during the MTH process over HSAPO‐34 and HZSM‐5 by in situ synchrotron radiation photoionization mass spectrometry. Compared with conventional methods, excellent time‐resolved profiles were obtained to study the formation and fate of HCHO, and other products during the induction, steady‐state reaction, and deactivation periods. Similar formation trends of HCHO and methane, and their close correlation in yields suggest that they are derived from disproportionation of methanol at acidic sites. In the presence of Y2O3, the amount of HCHO changes, affecting the hydrogen‐transfer processes of olefins into aromatics and aromatics into cokes. The yield of HCHO affects the aromatic‐based cycle and the formation of ethylene, indicating that ethylene is mainly formed from the aromatic‐based cycle.

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Section: Methodsmentioning

confidence: 99%

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

Wen

Zhou

et al. 2020

Angew Chem Int Ed

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“…Similar operating conditions were used, but replacing He by Ar that served as a reference in the SVUV-PI-MBMS data evaluation. The apparatus has been described elsewhere [20]. Gas samples were extracted from the JSR by a quartz sampling cone.…”

Section: Jsr-svuv-pi-mbms Experimentsmentioning

confidence: 99%

Low-temperature gas-phase oxidation of diethyl ether: Fuel reactivity and fuel-specific products

Tran

Herbinet

et al. 2019

Proceedings of the Combustion Institute

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144

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Diethyl ether (DEE) has been recently suggested as a potential biofuel for compression-ignition engines that are known to be significantly controlled by low-temperature (LT) chemistry. However, the LT oxidation of DEE has not fully been understood in term of the formation of LT fuel-specific products. We have thus studied the oxidation of DEE by examining detailed profiles of its oxidation products under LT conditions (400-1100 K). To this end, we have used a dedicated experimental setup including a nearly-atmospheric jet-stirred reactor (JSR) coupled to online gas chromatography (GC). The experiments were complemented by measurements made with a JSR coupled to tunable synchrotron vacuum ultraviolet (SVUV) photoionization (PI) molecular-beam mass spectrometry (MBMS) for a cross-validation of the identification of important LT species. Experimental results indicate that DEE is very reactive; it starts to react around 425 K. DEE exhibits an unusual oxidation behavior with two negative temperature coefficient (NTC) zones in the JSR study. Because of this two-NTC observation, additional experiments were performed with a plug flow reactor (PFR) combined with electron ionization (EI)-MBMS, confirming this behavior in the two types of reactor. Moreover, about 20 oxidation species in C1-C4 range were detected with several intermediates containing 2-3 O-atoms. Acetic acid is found to peak at 525 K with a very large amount, suggesting that it is a key species in the early stage of DEE's LT oxidation. Possible DEE-consumption paths leading to acetic acid formation could play an important role in the oxidation mechanism of DEE. A new model is proposed based on the present experimental observations to include new primary LT reaction paths. The model reproduces the experimental phenomena quite well and enhances the understanding of the two-NTC-zone occurrence and of intermediates containing 2-3 O-atoms during the LT oxidation of DEE.

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“…to confirm important trends obtained in the JSR-GC experiments, (ii) to detect species that cannot be measured by GC such as hydroperoxide species, and (iii) to assist in the identification of important LT intermediates. A detailed description of the apparatus is available in [18,19].…”

Section: Combination Of Jsr and Svuv-pi-mbms (Hefei)mentioning

confidence: 99%

Probing the low-temperature chemistry of di-n-butyl ether: Detection of previously unobserved intermediates

Tran

Wullenkord

et al. 2019

Combustion and Flame

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Din -butyl ether (DBE, C8H18O) has been proposed as a promising biofuel for diesel engines, but details of its low-temperature (LT) oxidation chemistry are not well understood. This paper reports new speciation data obtained in the temperature range of 400-1100 K at ϕ=1 and nearly-atmospheric pressure, using a plug flow reactor (PFR) combined with electron ionization (EI) molecular-beam mass spectrometry (MBMS) and two different jet-stirred reactors (JSRs) coupled with either online gas chromatography (GC) or tunable synchrotron vacuum ultraviolet (SVUV) photoionization (PI)-MBMS. The experimental results confirm that DBE is very reactive and exhibits two negativetemperature coefficient (NTC) zones around 500-550 K and 650-750 K. Speciation data with about 40 C0-C8 species are presented, including about 20 LT species not reported previously. Among those, fuel-specific C8H16O2 cyclic ethers were quantified. Also, butanoic acid, which is present in highest amounts among the detected LT intermediates, and C8H14O3 diones, were found to peak already near 500 K, suggesting their importance in the LT chemistry of DBE. Signals of several highly oxygenated peroxides (e.g., C8H14O5 and C8H16O6) were detected, indicating third O2 addition steps. Respective reaction pathways are suggested and discussed based on these experimental results. To better understand the LT chemistry of DBE, the present data were compared to two recent DBE models [L. Cai et al. Combust. Flame. 161 (2014) 798-809 and S. Thion et al. Combust. Flame 185 (2017) 4-15]. Significant discrepancies between the experimental data and both models were found for important LT intermediates, of which many were not included in the respective mechanisms. The results reported in the present study thus provide new opportunities for refining DBE kinetic models.

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

Cited by 169 publications

References 49 publications

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

Low-temperature gas-phase oxidation of diethyl ether: Fuel reactivity and fuel-specific products

Probing the low-temperature chemistry of di-n-butyl ether: Detection of previously unobserved intermediates

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