Methyl cyanide and hydrogen cyanide measurements in the lower stratosphere: Implications for methyl cyanide sources and sinks

Schneider, Johannes; Bürger, V.; Arnold, Frank

doi:10.1029/97jd02364

Cited by 59 publications

(60 citation statements)

References 32 publications

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“…In situ measurements were first made in the stratosphere using NI-CIMS (negative ion-chemical ionisation mass spectrometer) (Schneider et al, 1997). Tropospheric measurements were then made by long-path Fourier transform IR (FTIR) spectroscopy within BB plumes (Goode et al, 2000a, b;Yokelson et al, 2007b), with a gas chromatography (GC) system, using a reduction gas detector (RGD) , by NI-CIMS using CF 3 O − as the reagent ion (Crounse et al, 2006Yokelson et al, 2007a), and by PTR-MS (proton transfer-mass spectrometry) (Knighton et al, 2009).…”

Section: Introductionmentioning

confidence: 99%

Airborne hydrogen cyanide measurements using a chemical ionisation mass spectrometer for the plume identification of biomass burning forest fires

et al. 2013

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A chemical ionisation mass spectrometer (CIMS) was developed for measuring hydrogen cyanide (HCN) from biomass burning events in Canada using I⁻ reagent ions on board the FAAM BAe-146 research aircraft during the BORTAS campaign in 2011. The ionisation scheme enabled highly sensitive measurements at 1 Hz frequency through biomass burning plumes in the troposphere.

A strong correlation between the HCN, carbon monoxide (CO) and acetonitrile (CH₃CN) was observed, indicating the potential of HCN as a biomass burning (BB) marker. A plume was defined as being 6 standard deviations above background for the flights. This method was compared with a number of alternative plume-defining techniques employing CO and CH₃CN measurements. The 6-sigma technique produced the highest R² values for correlations with CO. A normalised excess mixing ratio (NEMR) of 3.68 ± 0.149 pptv ppbv⁻¹ was calculated, which is within the range quoted in previous research (Hornbrook et al., 2011). The global tropospheric model STOCHEM-CRI incorporated both the observed ratio and extreme ratios derived from other studies to generate global emission totals of HCN via biomass burning. Using the ratio derived from this work, the emission total for HCN from BB was 0.92 Tg (N) yr⁻¹

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Section: Introductionmentioning

confidence: 99%

Airborne hydrogen cyanide measurements using a chemical ionisation mass spectrometer for the plume identification of biomass burning forest fires

et al. 2013

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“…In-situ HCN measurements were first made in the stratosphere by NI-CIMS (e.g., Schneider et al, 1997). Later, in-situ measurements in the troposphere were made by (1) long-path Fourier transform IR (FTIR) spectroscopy within BB plumes (Goode et al, 2000;Yokelson et al, 2007), (2) a GC system, using a reduction gas detector (RGD) , (3) NI-CIMS using trifluoromethoxide (CF 3 O − ) as reagent ion (Crounse et al, 2006(Crounse et al, , 2009Yokelson et al, 2007), and (4) PTR-MS (Knighton et al, 2009).…”

Section: Introductionmentioning

confidence: 99%

A gas chromatographic instrument for measurement of hydrogen cyanide in the lower atmosphere

et al. 2012

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Abstract. A gas-chromatographic (GC) instrument was developed for measuring hydrogen cyanide (HCN) in the lower atmosphere. The main features of the instrument are (1) a cryogen-free cooler for sample dehumidification and enrichment, (2) a porous polymer PLOT column for analyte separation, (3) a flame thermionic detector (FTD) for sensitive and selective detection, and (4) a dynamic dilution system for calibration. We deployed the instrument for a ∼4 month period from January-June, 2010 at the AIRMAP atmospheric monitoring station Thompson Farm 2 (THF2) in rural Durham, NH. A subset of measurements made during 3-31 March is presented here with a detailed description of the instrument features and performance characteristics. The temporal resolution of the measurements was ∼20 min, with a 75 s sample capture time. The 1σ measurement precision was <10 % and the instrument response linearity was excellent on a calibration scale of 0.10-0.75 ppbv (±5 %). The estimated method detection limit (MDL) and accuracy were 0.021 ppbv and 15 %, respectively. From 3-31 March 2010, ambient HCN mixing ratios ranged from 0.15-1.0 ppbv (±15 %), with a mean value of 0.36 ± 0.16 ppbv (1σ ). The approximate mean background HCN mixing ratio of 0.20 ± 0.04 ppbv appeared to agree well with tropospheric column measurements reported previously. The GC-FTD HCN measurements were strongly correlated with acetonitrile (CH 3 CN) measured concurrently with a proton transfer-reaction mass spectrometer (PTR-MS), as anticipated given our understanding that the nitriles share a common primary biomass burning source to the global atmosphere. The nitriles were overall only weakly correlated with carbon monoxide (CO), which is reasonable considering the greater diversity of sources for CO. However, strong correlations with CO were observed on several nights under stable atmospheric conditions and suggest regional combustion-based sources for the nitriles. These results demonstrate that the GC-FTD instrument is capable of making long term, in-situ measurements of HCN in the lower atmosphere. To date, similar measurements have not been performed, yet they are critically needed to (1) better evaluate the regional scale distribution of HCN in the atmosphere and (2) discern the influence of biomass burning on surface air composition in remote regions.

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“…Early in situ measurements of acetonitrile are somewhat contradictory, and significantly lower than more recent measurements; see Schneider et al (1997) for an in depth discussion. A number of early studies made use of the ionmolecule reaction mass spectrometry (IMRMS) technique, in which the detection relies on the ion-molecule reaction in which a CH 3 CN molecule displaces one water ligand from a hydrated H + (H 2 O) n cluster.…”

Section: Introductionmentioning

confidence: 77%

“…Unfortunately, the reverse reaction becomes more efficient at higher water vapour abundance and ion hydration, which increases with relative humidity. For this reason it is expected that IMRMS measurements in the troposphere and near the tropopause will be underestimated (Schneider et al, 1997), but not measurements in the stratosphere. Comparisons with these early measurements need to be made with care.…”

Section: Introductionmentioning

confidence: 99%

ACE-FTS observations of acetonitrile in the lower stratosphere

Harrison

Bernath

2013

Atmos. Chem. Phys.

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This work reports the first infrared satellite remote-sensing measurements of acetonitrile (CH₃CN) in the Earth's atmosphere using solar occultation measurements made by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) between 2004 and 2011. The retrieval scheme uses new quantitative laboratory spectroscopic measurements of acetonitrile (Harrison and Bernath, 2012). Although individual ACE-FTS profile measurements are dominated by measurement noise, median profiles in 10° latitude bins show a steady decline in volume mixing ratio from ~150 ppt (parts per trillion) at 11.5 km to < 40 ppt at 25.5–29.5 km. These new measurements agree well with the scant available air- and balloon-borne data in the lower stratosphere. An acetonitrile stratospheric lifetime of 73 ± 20 yr has been determined

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Methyl cyanide and hydrogen cyanide measurements in the lower stratosphere: Implications for methyl cyanide sources and sinks

Cited by 59 publications

References 32 publications

Airborne hydrogen cyanide measurements using a chemical ionisation mass spectrometer for the plume identification of biomass burning forest fires

Airborne hydrogen cyanide measurements using a chemical ionisation mass spectrometer for the plume identification of biomass burning forest fires

A gas chromatographic instrument for measurement of hydrogen cyanide in the lower atmosphere

ACE-FTS observations of acetonitrile in the lower stratosphere

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