First detection of a key intermediate in the oxidation of fuel + NO systems: HONO

Marrodán, Lorena; Song, Yu; Herbinet, Olivier; Alzueta, María U.; Fittschen, Christa; Ju, Yiguang; Battin‐Leclerc, Frédérique

doi:10.1016/j.cplett.2019.01.038

Cited by 23 publications

(16 citation statements)

References 33 publications

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“…However, for gasoline vehicles, the correlations between HONO and NOx emissions as well as HONO and NO 2 emissions are both poor (Figure S10). This might be attributable to the difference in the gas compositions of the exhausts of gasoline and diesel vehicles, such as carbonyl compounds, suggesting that the gas composition could be an important factor influencing the HONO emissions. ,, Therefore, although the ER HONO/NOx is widely used to estimate the HONO emissions from vehicles when HONO emission factors are not available, the low correlations between HONO and NOx found in this study indicated that such a proxy may bring high uncertainties in estimating the HONO emissions from the vehicles.…”

Section: Resultsmentioning

confidence: 80%

“…As ECE has higher frequencies of accelerations and decelerations, vehicles under the same emission control standard generally have higher HONO emissions for ECE driving cycles than those for the SSM cycles. This is probably because frequent speed changes can lead to incomplete combustion in the engine and promote the HONO formation from NO 2 and intermediate species such as HO 2 , CH 2 O, and CH 3 O, 19,35 indicating that the HONO emissions are sensitive to driving conditions.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

Liao

Zhang

et al. 2020

Environ. Sci. Technol.

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Nitrous acid (HONO) plays an important role in the budget of hydroxyl radical (•OH) in the atmosphere. Vehicular emissions are a crucial primary source of atmospheric HONO, yet remain poorly investigated, especially for diesel trucks. In this study, we developed a novel portable online vehicular HONO exhaust measurement system featuring an innovative dilution technique. Using this system coupled with a chassis dynamometer, we for the first time investigated the HONO emission characteristics of 17 light-duty diesel trucks (LDDTs) and 16 light-duty gasoline vehicles in China. Emissions of HONO from LDDTs were found to be significantly higher than previous studies and gasoline vehicles tested in this study. The HONO emission factors of LDDTs decrease significantly with stringent control standards: 1.85 ± 1.17, 0.59 ± 0.25, and 0.15 ± 0.14 g/kg for China III, China IV, and China V, respectively. In addition, we found poor correlations between HONO and NOx emissions, which indicate that using the ratio of HONO to NOx emissions to infer HONO emissions might lead to high uncertainty of HONO source budget in previous studies. Lastly, the HONO emissions are found to be influenced by driving conditions, highlighting the importance of conducting on-road measurements of HONO emissions under real-world driving conditions. More direct measurements of the HONO emissions are needed to improve the understanding of the HONO emissions from mobile and other primary sources.

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Section: Resultsmentioning

confidence: 80%

Section: ■ Results and Discussionmentioning

confidence: 99%

High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

Liao

Zhang

et al. 2020

Environ. Sci. Technol.

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“…When its initial mole fraction is 500 ppm, NO starts to be consumed at 625 K; meanwhile, the mole fraction of NO2 increases sharply to reach approximately 300 ppm. Above 650 K, NO is fully consumed, and the amount of NO2 continues gradually increasing until 750 K. Concerning HONO, for which the quantification procedure under oxidation process was demonstrated elsewhere [45] its produced mole fraction is nearly 100 ppm at a temperature of 650 K. The HONO mole fraction also increases until the temperature is 725 K. After that, it decays as the temperature further increases. When NO2 (400 ppm) is added as a reactant, the onset temperature for its consumption is approximately 575 K, which is consistent with that of neat n-pentane as is shown in Figure 2.…”

Section: Oxidation Of Neat N-pentane: the Effect Of Different Bath Gasesmentioning

confidence: 99%

“…It was found that HONO signals were below the estimated/calculated detection limit (3 ppm) [44]. More recently, HONO signals were successfully identified and quantified during n-pentane JSR oxidation in the presence of NO [45].…”

Section: Introductionmentioning

confidence: 99%

Effects of Bath Gas and NO_x Addition on n-Pentane Low-Temperature Oxidation in a Jet-Stirred Reactor

et al. 2019

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The oxidation of n-pentane (C5H12) in different bath gases (He, Ar, and CO2) and in Ar with NO2 or NO addition has been studied in a jet-stirred reactor at 107 kPa, temperatures between 500 and 1100 K, with a fixed residence time of 2.0 s, under stoichiometric conditions. Four different quantification diagnostics were used: gas chromatography, a chemiluminescence NOx analyzer, continuous wave cavity ring-down spectroscopy, and Fourier transform infrared spectroscopy. The results showed that the onset temperature of the fuel reactivity was the same (575 K) regardless of the type of bath gases. Although the low-temperature fuel oxidation window was not affected by the type of bath gas, the n-pentane conversion was slightly larger when diluted in Ar through the negative temperature coefficient (NTC) region (625-725 K). Above 800 K, the reactivity according to the diluent was in the order CO2 > Ar > He. In the presence of NO2 or NO, it was found that the consumption rate of n-pentane exhibited a different trend below 700 K. The presence of NO2 did not modify the fuel conversion below 675 K. On the contrary, NO addition increased the onset temperature of the fuel reactivity by 75 K and almost no NTC zone was observed. This clearly indicated that NO addition inhibited n-pentane oxidation below 675 K. Above 700 K, n-pentane conversion was promoted by the presence of both NOx additives. The intermediate species HONO was quantified, and a search for HCN and CH3NO2 species was also attempted. A new detailed kinetic mechanism was developed, which allowed a good prediction of the experimental data. Reaction rate and sensitivity analyses were conducted to illustrate the different kinetic regimes induced by the NOx addition. The inhibition by NO of the n-pentane oxidation below 675 K can be explained by its direct reaction with C5H11O2 radicals disfavoring the classical promoting channels via isomerizations, second O2 addition, and formation of ketohydroperoxides, the well-known branching agents during alkane oxidation. With respect to NO2 addition, the major consumption route is via NO2 + CH3 = NO + CH3O, which is not directly related to the direct fuel consumption. HONO formation mainly derives from NO2 reacting with CHiO (i = 2, 3). The reaction, HONO + M = OH + NO + M, is one of the most sensitive reactions for HONO depletion.

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“…It was already used in previous studies to quantify intermediates like hydrogen peroxide and HONO during the oxidation of fuels. 42,43 Ammonia has strong absorption lines in the wavenumber range 6637-6643 cm −1 , making the quantification accurate and providing a good sensibility. Fig.…”

Section: View Article Onlinementioning

confidence: 99%

An experimental, theoretical and kinetic-modeling study of the gas-phase oxidation of ammonia

et al. 2020

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First detection of a key intermediate in the oxidation of fuel + NO systems: HONO

Cited by 23 publications

References 33 publications

High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

Effects of Bath Gas and NO_x Addition on n-Pentane Low-Temperature Oxidation in a Jet-Stirred Reactor

An experimental, theoretical and kinetic-modeling study of the gas-phase oxidation of ammonia

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First detection of a key intermediate in the oxidation of fuel + NO systems: HONO

Cited by 23 publications

References 33 publications

High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

High Gaseous Nitrous Acid (HONO) Emissions from Light-Duty Diesel Vehicles

Effects of Bath Gas and NOx Addition on n-Pentane Low-Temperature Oxidation in a Jet-Stirred Reactor

An experimental, theoretical and kinetic-modeling study of the gas-phase oxidation of ammonia

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First detection of a key intermediate in the oxidation of fuel + NO systems: HONO

Effects of Bath Gas and NO_x Addition on n-Pentane Low-Temperature Oxidation in a Jet-Stirred Reactor