Dimethylamine and ammonia measurements with ion chromatography during the CLOUD4 campaign

Praplan, Arnaud P.; Bianchi, Federico; Dommen, Josef; Baltensperger, Urs

doi:10.5194/amt-5-2161-2012

Cited by 47 publications

(47 citation statements)

References 28 publications

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“…The facility is described in more detail by Kirkby et al (2011). Thorough cleaning with ultra-pure water and heat (373 K) decreases contaminant levels such as ammonia and amines to a few pptv, and volatile organic compounds to below 1 ppbv (Praplan et al, 2012;Schnitzhofer et al, 2014). However, only heating and flushing with the ultra-pure air of the chamber has been performed between experiments with ammonia and dimethyl amine and the experiments presented in this paper, which is somewhat less efficient than the use of water.…”

Section: Methodsmentioning

confidence: 99%

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

et al. 2015

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Abstract. This study presents the difference between oxidised organic compounds formed by α-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone.We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation.

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Section: Methodsmentioning

confidence: 99%

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

et al. 2015

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“…2.4). We can give some estimate of the contaminant levels of the dominant amine, C 2 H 7 N, based on measurements from later CLOUD campaigns when dimethylamine was also added into the chamber in several experiments (Praplan et al, 2012;Almeida et al, 2013). These estimates are based on direct measurements of dimethylamine concentrations down to 0.2 pptv performed during the later experiments and on measurements of the content of C 2 H 7 N in clusters seen by the APi-TOF.…”

Section: Contaminant Amines In Growing Anion Clustersmentioning

confidence: 99%

On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

et al. 2015

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Abstract. The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH 3 ) and sulfuric acid (H 2 SO 4 ). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH 3 -H 2 SO 4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH 3 ] in the range from < 2 to 1400 pptv, [H 2 SO 4 ] from 3.3 × 10 6 to 1.4 × 10 9 cm −3 (0.1 to 56 pptv), and a temperature range from −25 to +20 • C. Negatively and positively charged clusters were directly measured by an atmospheric pressure interface time-of-flight (APi-TOF)Published by Copernicus Publications on behalf of the European Geosciences Union. S. Schobesberger et al.: On the composition of ammonia-sulfuric-acid clustersmass spectrometer, as they initially formed from gas-phase NH 3 and H 2 SO 4 , and then grew to larger clusters containing more than 50 molecules of NH 3 and H 2 SO 4 , corresponding to mobility-equivalent diameters greater than 2 nm. Water molecules evaporate from these clusters during sampling and are not observed. We found that the composition of the NH 3 -H 2 SO 4 clusters is primarily determined by the ratio of gas-phase concentrations [NH 3 ] is mostly larger than 10. We compared our results from CLOUD with APi-TOF measurements of NH 3 -H 2 SO 4 anion clusters during new-particle formation in the Finnish boreal forest. However, the exact role of NH 3 -H 2 SO 4 clusters in boundary layer particle formation remains to be resolved.

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“…For the scope of this paper it is sufficient to note that just the relative change in the DMA signal is required to obtain the wall loss rate, while the absolute measurement is not a necessity. Overall, the different methods for determination of the DMA mixing ratios, including also the direct IC measurement (Praplan et al, 2012), yield consistent results and the error bars in Fig. 6 indicate the uncertainty.…”

Section: Sensitivity Studiesmentioning

confidence: 86%

Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (< 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest

et al. 2015

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Abstract. Atmospheric amines may play a crucial role in formation of new aerosol particles via nucleation with sulfuric acid. Recent studies have revealed that concentrations below 1 pptV can significantly promote nucleation of sulfuric acid particles. While sulfuric acid detection is relatively straightforward, no amine measurements to date have been able to reach the critical sub-pptV concentration range and atmospheric amine concentrations are in general poorly characterized. In this work we present a proof-of-concept of an instrument capable of detecting dimethyl amine (DMA) with concentrations even down to 70 ppqV (parts per quadrillion, 0.07 pptV) for a 15 min integration time. Detection of ammonia and amines other than dimethyl amine is discussed. We also report results from the first ambient measurements performed in spring 2013 at a boreal forest site. While minute signals above the signal-to-noise ratio that could be attributed to trimethyl or propyl amine were observed, DMA concentration never exceeded the detection threshold of ambient measurements (150 ppqV), thereby questioning, though not excluding, the role of DMA in nucleation at this location.

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Dimethylamine and ammonia measurements with ion chromatography during the CLOUD4 campaign

Cited by 47 publications

References 28 publications

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (< 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest

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Dimethylamine and ammonia measurements with ion chromatography during the CLOUD4 campaign

Cited by 47 publications

References 28 publications

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (&lt; 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest

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Product

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Bisulfate – cluster based atmospheric pressure chemical ionization mass spectrometer for high-sensitivity (< 100 ppqV) detection of atmospheric dimethyl amine: proof-of-concept and first ambient data from boreal forest