Eddy covariance flux measurements of ammonia by high temperature chemical ionisation mass spectrometry

Sintermann, Jörg; Spirig, C.; Jordan, Alfons; Kühn, U.; Ammann, Christof; Neftel, A.

doi:10.5194/amt-4-599-2011

Cited by 73 publications

(106 citation statements)

References 92 publications

(119 reference statements)

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“…Nowak et al (2007) found uncertainties in CIMS NH 3 measurements to be ±25-30 % during field operation. Sintermann et al (2011) found calibration accuracy of ∼ 5 % for a CIMS NH 3 instrument.…”

Section: Calibration Methodsmentioning

confidence: 99%

“…Conventional offline NH 3 sensors (passive filters, denuders and ion chromatography) often have sufficient sensitivity (< 1 ppbv NH 3 ), but have long integration times, lack the requisite selectivity and are labor intensive to analyze (Fehsenfeld et al, 2002;von Bobrutzki et al, 2010;Ellis et al, 2011). Chemical ionization mass spectrometry (CIMS) NH 3 instruments have high time resolution (seconds), selectivity and extremely high sensitivity (< 100 pptv NH 3 ), but require large power consumption (kW) and space (multiple instrument racks) (Nowak et al, 2007;Benson et al, 2010;Sintermann et al, 2011). Laser absorption spectrometers for gas-phase NH 3 have been developed for real-time, high-sensitivity and selective detection.…”

Section: J Miller Et Al: Open-path Qcl-based Ammonia Sensormentioning

confidence: 99%

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Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

et al. 2014

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Abstract. We demonstrate a compact, open-path, quantum cascade-laser-based atmospheric ammonia sensor operating at 9.06 µm for high-sensitivity, high temporal resolution, ground-based measurements. Atmospheric ammonia (NH 3 ) is a gas-phase precursor to fine particulate matter, with implications for air quality and climate change. Currently, NH 3 sensing challenges have led to a lack of widespread in situ measurements. Our open-path sensor configuration minimizes sampling artifacts associated with NH 3 surface adsorption onto inlet tubing and reduced pressure sampling cells, as well as condensed-phase partitioning ambiguities. Multi-harmonic wavelength modulation spectroscopy allows for selective and sensitive detection of atmospheric pressurebroadened absorption features. An in-line ethylene reference cell provides real-time calibration (±20 % accuracy) and normalization for instrument drift under rapidly changing field conditions. The sensor has a sensitivity and noise-equivalent limit (1σ ) of 0.15 ppbv NH 3 at 10 Hz, a mass of ∼ 5 kg and consumes ∼ 50 W of electrical power. The total uncertainty in NH 3 measurements is 0.20 ppbv NH 3 ± 10 %, based on a spectroscopic calibration method. Field performance of this open-path NH 3 sensor is demonstrated, with 10 Hz time resolution and a large dynamic response for in situ NH 3 measurements. This sensor provides the capabilities for improved in situ gas-phase NH 3 sensing relevant for emission source characterization and flux measurements.

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Section: Calibration Methodsmentioning

confidence: 99%

Section: J Miller Et Al: Open-path Qcl-based Ammonia Sensormentioning

confidence: 99%

Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

et al. 2014

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“…In the last decade, substantial progress has been made in the use of tunable diode laser absorption spectroscopy (TDLAS) and quantum cascade lasers (QCL) as well as devices originating from individual applications such as Fourier transform infrared (FTIR) spectrometers. The precision and fast response of these approaches has allowed first EC measurements of field scale N 2 O and CH 4 fluxes (Rinne et al, 2005;Denmead et al, 2010;Kroon et al, 2010;Neftel et al, 2010;Tuzson et al, 2010) as well as first NO 2 fluxes (Horii et al, 2004), whereas measurements of NH 3 fluxes by EC have been extremely limited (Famulari et al, 2004;Sutton et al, 2007;Sintermann et al, 2011), and are subject to substantial uncertainty (e.g. Shaw et al, 1998).…”

Section: Exchange Measurements Of Reactive Nitrogen Compoundsmentioning

confidence: 99%

“…In this approach, each class of compounds thermally dissociates to NO 2 and an accompanying radical (RO 2 , RO, OH) in separately thermostatted ovens at temperatures of 180, 330, and 550 • C for PN, AN, and HNO 3 , respectively. Sintermann et al (2011) use a system for fast NH 3 measurements with chemical ionisation mass spectrometry (CIMS) based on a commercial Proton Transfer Reaction-Mass Spectrometer (PTR-MS) within an EC setup over two agricultural fields in Oensingen, Switzerland, whereas the EC fluxes of NH 3 measured by Famulari et al (2004) during a two-month field campaign were conducted by the use of a TDLAS system.…”

Section: Exchange Measurements Of Reactive Nitrogen Compoundsmentioning

confidence: 99%

TRANC – a novel fast-response converter to measure total reactive atmospheric nitrogen

Marx¹,

Brümmer

Ammann

et al. 2012

Atmos. Meas. Tech.

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Abstract. The input and loss of plant available nitrogen (reactive nitrogen: N r ) from/to the atmosphere can be an important factor for the productivity of ecosystems and thus for its carbon and greenhouse gas exchange. We present a novel converter for reactive nitrogen (TRANC: Total Reactive Atmospheric Nitrogen Converter), which offers the opportunity to quantify the sum of all airborne reactive nitrogen compounds ( N r ) in high time resolution. The basic concept of the TRANC is the full conversion of all N r to nitrogen monoxide (NO) within two reaction steps. Initially, reduced N r compounds are being oxidised, and oxidised N r compounds are thermally converted to lower oxidation states. Particulate N r is being sublimated and oxidised or reduced afterwards. In a second step, remaining higher nitrogen oxides or those generated in the first step are catalytically converted to NO with carbon monoxide used as reduction gas. The converter is combined with a fast response chemiluminescence detector (CLD) for NO analysis and its performance was tested for the most relevant gaseous and particulate N r species under both laboratory and field conditions. Recovery rates during laboratory tests for NH 3 and NO 2 were found to be 95 and 99 %, respectively, and 97 % when the two gases were combined. In-field longterm stability over an 11-month period was approved by a value of 91 % for NO 2 . Effective conversion was also found for ammonium and nitrate containing particles. The recovery rate of total ambient N r was tested against the sum of individual measurements of NH 3 , HNO 3 , HONO, NH + 4 , NO − 3 , and NO x using a combination of different well-established devices. The results show that the TRANC-CLD system precisely captures fluctuations in N r concentrations and also matches the sum of all individual N r compounds measured by the different single techniques. The TRANC features a specific design with very short distance between the sample air inlet and the place where the thermal and catalytic conversions to NO occur. This assures a short residence time of the sample air inside the instrument, and minimises wall sorption problems of water soluble compounds. The fast response time (e-folding times of 0.30 to 0.35 s were found during concentration step changes) and high accuracy in capturing the dominant N r species enables the converter to be used in an eddy covariance setup. Although a source attribution of specific N r compounds is not possible, the TRANC is a new reliable tool for permanent measurements of the net N r flux between ecosystem and atmosphere at a relatively low maintenance and reasonable cost level allowing for diurnal, seasonal and annual investigations.

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“…The outflow was sampled into a high-temperature (HT)-CIMS (modified Ionicon PTR-MS in O 2 mode as used by Kuhn et al, 2011;Sintermann et al, 2011Sintermann et al, , 2014 for online analysis of NH 3 and TMA. Calibration factors similar to those used by Sintermann et al (2014) were applied.…”

Section: Appendix A: Figure 1: Methodsmentioning

confidence: 99%

Ideas and perspectives: on the emission of amines from terrestrial vegetation in the context of new atmospheric particle formation

Sintermann

Neftel

2015

Biogeosciences

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Abstract. In this article we summarise recent science which shows how airborne amines, specifically methylamines (MAs), play a key role in new atmospheric particle formation (NPF) by stabilising small molecule clusters. Agricultural emissions are assumed to constitute the most important MA source, but given the short atmospheric residence time of MAs, they can hardly have a direct impact on NPF events observed in remote regions. This leads us to the presentation of existing knowledge focussing on natural vegetationrelated MA sources. High MA contents as well as emissions by plants was already described in the 19th century. Strong MA emissions predominantly occur during flowering as part of a pollination strategy. The behaviour is species-specific, but examples of such species are common and widespread. In addition, vegetative plant tissue exhibiting high amounts of MAs might potentially lead to significant emissions. The decomposition of organic material constitutes another, potentially ubiquitous, source of airborne MAs. These mechanisms would provide sources, which could be crucial for the amine's role in NPF, especially in remote regions. Knowledge about vegetation-related amine emissions is, however, very limited, and thus it is also an open question how global change and the intensified cycling of reactive nitrogen over the last 200 years have altered amine emissions from vegetation with a corresponding effect on NPF.

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Eddy covariance flux measurements of ammonia by high temperature chemical ionisation mass spectrometry

Cited by 73 publications

References 92 publications

Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

Open-path, quantum cascade-laser-based sensor for high-resolution atmospheric ammonia measurements

TRANC – a novel fast-response converter to measure total reactive atmospheric nitrogen

Ideas and perspectives: on the emission of amines from terrestrial vegetation in the context of new atmospheric particle formation

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