Low-temperature gas-phase oxidation of diethyl ether: Fuel reactivity and fuel-specific products
Low-temperature gas-phase oxidation of diethyl ether: Fuel reactivity and fuel-specific products
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乙醚低温气相氧化：燃料反应性和燃料专用产品
DOI：
10.1016/j.proci.2018.05.135
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发表时间：
2019
影响因子：
3.4
通讯作者：
Battin Leclerc Frederique
中科院分区：
文献类型：
--
作者：
Luc Sy Tran;Herbinet Olivier;Li Yuyang;Wullenkord Julia;Zeng Meirong;Braeuer Eike;Qi Fei;Kohse Hoeinghaus Katharina;Battin Leclerc Frederique
二乙醚(DIE)最近被认为是压燃式发动机的一种潜在的生物燃料，众所周知，这种发动机受到低温(LT)化学的显著控制。然而，DEE的LT氧化在LT燃料专有产物的形成方面还没有被完全理解。因此，我们通过考察其在LT条件下(400-1100 K)氧化产物的详细轮廓来研究其氧化。为此，我们使用了一个专用的实验装置，包括一个与在线气相色谱(GC)耦合的近大气喷射搅拌反应器(JSR)。实验得到了JSR与可调谐同步真空紫外光电离(PI)分子束质谱(MBMS)相结合的测量的补充，用于交叉验证重要LT物种的鉴定。实验结果表明，DeE非常活跃；它在425 左右开始反应。在JSR研究中，Dee表现出异常的氧化行为，有两个负温度系数(Ntc)区。由于这种两个NTC的观测，我们还使用了与电子电离(EI)-MBMS相结合的推流反应器(PFR)进行了额外的实验，证实了这两种类型的反应器中的这种行为。此外，在C_1单键C_4范围内检测到约20个氧化物种，其中几个中间体含有2-3个O-原子。冰醋酸在525 K处有一个很大的峰值，表明它是DEE的LT氧化早期的关键物种。可能的De消耗途径可能在DEE的氧化机理中起着重要作用。在现有实验观察的基础上提出了一个新的模型，该模型包含了新的初级LT反应路径。该模型较好地再现了实验现象，并增强了对DIE LT氧化过程中双NTC区的存在和含2-3个O原子的中间体的理解。
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 C1single bondC4range 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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影响因子：
9
作者：
Gillespie, Fiona;Metcalfe, Wayne K.;Dirrenberger, Patricia;Herbinet, Olivier;Glaude, Pierre-Alexandre;Battin-Leclerc, Frederique;Curran, Henry J.
通讯作者：
Curran, Henry J.
DOI：
10.1016/j.jlp.2005.07.001
发表时间：
2005-07-01
影响因子：
3.5
作者：
Naito, M;Radcliffe, C;Tamura, M
通讯作者：
Tamura, M
DOI：
10.1016/j.proci.2016.05.044
发表时间：
2017
期刊：
--
影响因子：
--
作者：
Anne Rodriguez;O. Herbinet;Zhandong Wang;F. Qi;C. Fittschen;P. R. Westmoreland;F. Battin‐Leclerc
通讯作者：
Anne Rodriguez;O. Herbinet;Zhandong Wang;F. Qi;C. Fittschen;P. R. Westmoreland;F. Battin‐Leclerc
影响因子：
6.3
作者：
Cuoci, A.;Frassoldati, A.;Ranzi, E.
通讯作者：
Ranzi, E.
DOI：
10.1098/rspa.1959.0151
发表时间：
1959-09
期刊：
Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences
影响因子：
--
作者：
D. Waddington
通讯作者：
D. Waddington