scholarly journals Ultraviolet Absorption Cross-Sections of Ammonia at Elevated Temperatures for Nonintrusive Quantitative Detection in Combustion Environments

2021 ◽  
pp. 000370282199044
Author(s):  
Wubin Weng ◽  
Shen Li ◽  
Marcus Aldén ◽  
Zhongshan Li

Ammonia (NH3) is regarded as an important nitrogen oxides (NOx) precursor and also as an effective reductant for NOx removal in energy utilization through combustion, and it has recently become an attractive non-carbon alternative fuel. To have a better understanding of thermochemical properties of NH3, accurate in situ detection of NH3 in high temperature environments is desirable. Ultraviolet (UV) absorption spectroscopy is a feasible technique. To achieve quantitative measurements, spectrally resolved UV absorption cross-sections of NH3 in hot gas environments at different temperatures from 295 K to 590 K were experimentally measured for the first time. Based on the experimental results, vibrational constants of NH3 were determined and used for the calculation of the absorption cross-section of NH3 at high temperatures above 590 K using the PGOPHER software. The investigated UV spectra covered the range of wavelengths from 190 nm to 230 nm, where spectral structures of the [Formula: see text] transition of NH3 in the umbrella bending mode, v2, were recognized. The absorption cross-section was found to decrease at higher temperatures. For example, the absorption cross-section peak of the (6, 0) vibrational band of NH3 decreases from ∼2 × 10−17 to ∼0.5 × 10−17 cm2/molecule with the increase of temperature from 295 K to 1570 K. Using the obtained absorption cross-section, in situ nonintrusive quantification of NH3 in different hot gas environments was achieved with a detection limit varying from below 10 parts per million (ppm) to around 200 ppm as temperature increased from 295 K to 1570 K. The quantitative measurement was applied to an experimental investigation of NH3 combustion process. The concentrations of NH3 and nitric oxide (NO) in the post flame zone of NH3–methane (CH4)–air premixed flames at different equivalence ratios were measured.

2018 ◽  
Vol 72 (9) ◽  
pp. 1388-1395 ◽  
Author(s):  
Wubin Weng ◽  
Tomas Leffler ◽  
Christian Brackmann ◽  
Marcus Aldén ◽  
Zhongshan Li

Spectrally resolved ultraviolet (UV) absorption cross-sections of gas-phase sodium chloride (NaCl), potassium hydroxide (KOH), and sodium hydroxide (NaOH) were measured, for the first time, in hot flue gases at different temperatures. Homogenous gas-phase NaCl, KCl (potassium chloride), NaOH, and KOH at temperatures 1200 K, 1400 K, 1600 K, and 1850 K were prepared in the post-flame zone of laminar flames by seeding nebulized droplets out of aqueous solution of corresponding alkali species. The amount of droplets seeded into the flame was kept constant, so the relative concentration of different alkali species can be derived. The broadband UV absorption cross-section of KCl vapor reported by Leffler et al. was adopted to derive the absorption cross-section curves of NaCl, NaOH, and KOH with the corresponding measured spectrally resolved absorbance spectra. No significant changes in the spectral structures in the absorption cross-sections were found as the temperature varied between 1200 K and 1850 K, except for NaOH at around 320 nm. The difference between the absorption spectral curves of alkali chlorides and hydroxides is significant at wavelengths above 300 nm, which thus can be used to distinguish and obtain the concentrations of alkali chlorides and hydroxides in the broadband UV absorption measurements.


2020 ◽  
Author(s):  
Thomas R. Lewis ◽  
Juan Carlos Gómez Martin ◽  
Mark A. Blitz ◽  
Carlos A. Cuevas ◽  
John M. C. Plane ◽  
...  

Abstract. Iodine oxides (IxOy) play an important role in the atmospheric chemistry of iodine. They are initiators of new particle formation events in the coastal and polar boundary layer and act as iodine reservoirs in tropospheric ozone-depleting chemical cycles. Despite the importance of the aforementioned processes, the photochemistry of these molecules has not been studied in detail previously. Here, we report the first determination of the absorption cross sections of IxOy, x = 2, 3, 5, y = 1–12 at λ = 355 nm by combining pulsed laser photolysis of I2/O3 gas mixtures in air with time-resolved photo-ionization time-of-flight mass spectrometry, using NO2 actinometry for signal calibration. The oxides selected for absorption cross section determinations are those presenting the strongest signals in the mass spectra, where signals containing 4 iodine atoms are absent. The method is validated by measuring the absorption cross section of IO at 355 nm, σ355 nm, IO = (1.2 ± 0.1) ×  10–18 cm2, which is found to be in good agreement with the most recent literature. The results obtained are: σ355 nm, I2O3 


2020 ◽  
Vol 20 (18) ◽  
pp. 10865-10887
Author(s):  
Thomas R. Lewis ◽  
Juan Carlos Gómez Martín ◽  
Mark A. Blitz ◽  
Carlos A. Cuevas ◽  
John M. C. Plane ◽  
...  

Abstract. Iodine oxides (IxOy) play an important role in the atmospheric chemistry of iodine. They are initiators of new particle formation events in the coastal and polar boundary layers and act as iodine reservoirs in tropospheric ozone-depleting chemical cycles. Despite the importance of the aforementioned processes, the photochemistry of these molecules has not been studied in detail previously. Here, we report the first determination of the absorption cross sections of IxOy, x=2, 3, 5, y=1–12 at λ=355 nm by combining pulsed laser photolysis of I2∕O3 gas mixtures in air with time-resolved photo-ionization time-of-flight mass spectrometry, using NO2 actinometry for signal calibration. The oxides selected for absorption cross-section determinations are those presenting the strongest signals in the mass spectra, where signals containing four iodine atoms are absent. The method is validated by measuring the absorption cross section of IO at 355 nm, σ355nm,IO= (1.2±0.1) ×10-18 cm2, which is found to be in good agreement with the most recent literature. The results obtained are σ355nm,I2O3<5×10-19 cm2 molec.−1, σ355nm,I2O4= (3.9±1.2)×10-18 cm2 molec.−1, σ355nm,I3O6= (6.1±1.6)×10-18 cm2 molec.−1, σ355nm,I3O7= (5.3±1.4)×10-18 cm2 molec.−1, and σ355nm,I5O12= (9.8±1.0)×10-18 cm2 molec.−1. Photodepletion at λ=532 nm was only observed for OIO, which enabled determination of upper limits for the absorption cross sections of IxOy at 532 nm using OIO as an actinometer. These measurements are supplemented with ab initio calculations of electronic spectra in order to estimate atmospheric photolysis rates J(IxOy). Our results confirm a high J(IxOy) scenario where IxOy is efficiently removed during daytime, implying enhanced iodine-driven ozone depletion and hindering iodine particle formation. Possible I2O3 and I2O4 photolysis products are discussed, including IO3, which may be a precursor to iodic acid (HIO3) in the presence of HO2.


1997 ◽  
Vol 51 (9) ◽  
pp. 1311-1315 ◽  
Author(s):  
J. Vattulainen ◽  
L. Wallenius ◽  
J. Stenberg ◽  
R. Hernberg ◽  
V. Linna

A heated and pressurized quartz cell with 150.5-mm pathlength was used to experimentally determine UV absorption spectra and further absorption cross sections of SO2, C2H2, and O2 in the wavelength range between 200 and 400 nm. Spectra were recorded at room temperature, and at 600 and 800 °C and at absolute pressures between 1 and 6 bar. A 30-W deuterium lamp was used as a light source, and the light was detected with a photomultiplier tube through a 0.4-m Czerny–Turner monochromator. Slit widths of the monochromator were adjusted to achieve a 5 Å measurement bandwidth, and the scan through the wavelength range was made in 5 Å steps. For each individual temperature and pressure level, a reference spectrum was first recorded with the cell filled with nitrogen. After this, the cell was filled with the selected species mixed with nitrogen, and the absorption spectra were recorded in similar conditions. The studied gas mixtures were calibrated to 3% accuracy.


2014 ◽  
Vol 2 (31) ◽  
pp. 6353-6361 ◽  
Author(s):  
Yuting Gao ◽  
Yi Qu ◽  
Tao Jiang ◽  
Hao Zhang ◽  
Nannan He ◽  
...  

Three alkyl-triphenylamine end-capped triazines (ATT-(1–3)) with AIE were synthesized, and the two-photon absorption cross section of ATT-3 was 10 003 GM.


2020 ◽  
Vol 126 (3) ◽  
Author(s):  
Ulrich Retzer ◽  
Hannah Ulrich ◽  
Florian J. Bauer ◽  
Stefan Will ◽  
Lars Zigan

1969 ◽  
Vol 47 (10) ◽  
pp. 1823-1834 ◽  
Author(s):  
Robert E. Huffman

The current status of absorption cross-section measurements for aeronomic use is reviewed. Recommended values for the gases O2, N2, O, and O3 are given at wavelengths where there is strong atmospheric absorption in the 3500–10 Å region. A table of absorption and ionization cross-sections at important solar emission lines is given. The problem of insufficient resolution at some wavelengths is discussed, and information on photolysis products is given where available.


Sign in / Sign up

Export Citation Format

Share Document