scholarly journals Diurnal cycle of iodine and mercury concentrations in Svalbard surface snow

2019 ◽  
Author(s):  
Andrea Spolaor ◽  
Elena Barbaro ◽  
David Cappelletti ◽  
Clara Turetta ◽  
Mauro Mazzola ◽  
...  

Abstract. Sunlit snow is highly photochemically active and plays an important role in the exchange of gas-phase species between the cryosphere to the atmosphere. Here, we investigate the behaviour of two selected species in surface snow: mercury (Hg) and iodine (I). Hg can deposit year-round and accumulate in the snowpack. However, photo-induced re-emission of gas phase Hg from the surface has been widely reported. Iodine is active in atmosphere new particle formation, especially in the marine boundary layer, and in the destruction of atmospheric ozone. It can also undergo photochemical re-emission. Although previous studies indicate possible post-depositional processes, little is known about the diurnal behaviour of these two species and their interaction in surface snow. The mechanisms are still poorly constrained and no field experiments have been performed in different seasons to investigate the magnitude of re-emission processes. Three high temporal resolution (hourly samples) 3 days long sampling campaign were carried out near Ny-Ålesund (Svalbard) to study the behaviour of mercury and iodine in surface snow under different sunlight and environmental conditions (24 h-darkness, 24 h-sunlight and day/night cycles). Our results indicate a clearly different behaviour of Hg and I in surface snow during the different campaign. The day/night experiments demonstrate the existence of a diurnal cycle in surface snow for Hg and iodine, indicating that these species are indeed influenced by the daily solar radiation cycle. Differently bromine did not show any diurnal cycle. The diurnal cycle disappeared also for Hg and iodine during the 24 h-sunlight period and during 24 h-darkness experiments supporting the idea of the occurrence (absence) of a continuous recycling/exchange at the snow-air interface. These results demonstrate that this surface snow recycling is seasonally dependent, through sunlight. They also highlight the non-negligible role that snowpack emissions have on ambient air concentrations and potentially on iodine-induced atmospheric nucleation processes.

2019 ◽  
Vol 19 (20) ◽  
pp. 13325-13339 ◽  
Author(s):  
Andrea Spolaor ◽  
Elena Barbaro ◽  
David Cappelletti ◽  
Clara Turetta ◽  
Mauro Mazzola ◽  
...  

Abstract. Sunlit snow is highly photochemically active and plays a key role in the exchange of gas phase species between the cryosphere and the atmosphere. Here, we investigate the behaviour of two selected species in surface snow: mercury (Hg) and iodine (I). Hg can deposit year-round and accumulate in the snowpack. However, photo-induced re-emission of gas phase Hg from the surface has been widely reported. Iodine is active in atmospheric new particle formation, especially in the marine boundary layer, and in the destruction of atmospheric ozone. It can also undergo photochemical re-emission. Although previous studies indicate possible post-depositional processes, little is known about the diurnal behaviour of these two species and their interaction in surface snow. The mechanisms are still poorly constrained, and no field experiments have been performed in different seasons to investigate the magnitude of re-emission processes Three sampling campaigns conducted at an hourly resolution for 3 d each were carried out near Ny-Ålesund (Svalbard) to study the behaviour of mercury and iodine in surface snow under different sunlight and environmental conditions (24 h darkness, 24 h sunlight and day–night cycles). Our results indicate a different behaviour of mercury and iodine in surface snow during the different campaigns. The day–night experiments demonstrate the existence of a diurnal cycle in surface snow for Hg and iodine, indicating that these species are indeed influenced by the daily solar radiation cycle. Differently, bromine did not show any diurnal cycle. The diurnal cycle also disappeared for Hg and iodine during the 24 h sunlight period and during 24 h darkness experiments supporting the idea of the occurrence (absence) of a continuous recycling or exchange at the snow–air interface. These results demonstrate that this surface snow recycling is seasonally dependent, through sunlight. They also highlight the non-negligible role that snowpack emissions have on ambient air concentrations and potentially on iodine-induced atmospheric nucleation processes.


Atmosphere ◽  
2021 ◽  
Vol 12 (5) ◽  
pp. 647
Author(s):  
Tobias Baur ◽  
Johannes Amann ◽  
Caroline Schultealbert ◽  
Andreas Schütze

More and more metal oxide semiconductor (MOS) gas sensors with digital interfaces are entering the market for indoor air quality (IAQ) monitoring. These sensors are intended to measure volatile organic compounds (VOCs) in indoor air, an important air quality factor. However, their standard operating mode often does not make full use of their true capabilities. More sophisticated operation modes, extensive calibration and advanced data evaluation can significantly improve VOC measurements and, furthermore, achieve selective measurements of single gases or at least types of VOCs. This study provides an overview of the potential and limits of MOS gas sensors for IAQ monitoring using temperature cycled operation (TCO), calibration with randomized exposure and data-based models trained with advanced machine learning. After lab calibration, a commercial digital gas sensor with four different gas-sensitive layers was tested in the field over several weeks. In addition to monitoring normal ambient air, release tests were performed with compounds that were included in the lab calibration, but also with additional VOCs. The tests were accompanied by different analytical systems (GC-MS with Tenax sampling, mobile GC-PID and GC-RCP). The results show quantitative agreement between analytical systems and the MOS gas sensor system. The study shows that MOS sensors are highly suitable for determining the overall VOC concentrations with high temporal resolution and, with some restrictions, also for selective measurements of individual components.


ACS Omega ◽  
2021 ◽  
Vol 6 (3) ◽  
pp. 2410-2419
Author(s):  
Junyao Li ◽  
Narcisse T. Tsona ◽  
Shanshan Tang ◽  
Xiuhui Zhang ◽  
Lin Du

2012 ◽  
Vol 9 (2) ◽  
pp. 970-979
Author(s):  
Young-Kyo Seo ◽  
Sung-Ok Baek

Some of glycol ethers, such as 2-methoxyethanol (2-ME) and 2-ethoxyethanol (2-EE) are known to be toxic and classified as hazardous air pollutants in USA, Japan and Germany. In Korea, however, there has been no study conducted so far for these compounds in ambient air. In addition, no clear methodologies for the measurement of glycol ethers have been yet established. We carried out this study to evaluate a sampling and analytical method for the determination of glycol ethers, in ambient air samples collected in specific industrial areas of South Korea. To measure glycol ethers, adsorption sampling and thermal desorption with GC/MS analysis were used in this study. The analytical method showed good repeatability, linearity and sensitivity. The lower detection limits were estimated to be approximately 0.3∼0.5 ppb. Based on storage tests, it was suggested that samples should be analyzed within two weeks. It was also demonstrated that this method can be used for the simultaneous measurement of glycol ethers and other aromatic VOCs such as benzene, toluene, and xylenes. Field sampling campaign was carried out at 2 sites, located in a large industrial area, from October 2006 to June 2007, and a total of 480 samples were collected seasonally. Among them, 2-ME was not detected from any samples, while 2-EE and 2-Ethyloxyethylacetate (2-EEA) were found in 7 and 70 samples, respectively. The measured concentrations of 2-EE and 2-EEA for samples were ranged from 0.7-2.5 ppb and from 0.5-10.5 ppb, respectively. To our knowledge, this is the first measurement report for glycol ethers in the ambient atmosphere not only in Korea but also the rest of the world.


2011 ◽  
Vol 11 (7) ◽  
pp. 3243-3261 ◽  
Author(s):  
P. Wojtal ◽  
J. D. Halla ◽  
R. McLaren

Abstract. A complete understanding of the formation mechanism of nitrous acid (HONO) in the ambient atmosphere is complicated by a lack of understanding of processes occurring when aqueous water is present. We report nocturnal measurements of HONO, SO2 and NO2 by differential optical absorption spectroscopy over the ocean surface in a polluted marine environment. In this aqueous environment, we observed reproducible pseudo steady states (PSS) of HONO every night, that are fully formed shortly after sunset, much faster than seen in urban environments. During the PSS period, HONO is constant with time, independent of air mass source and independent of the concentration of NO2. The independence of HONO on the concentration of NO2 implies a 0° order formation process, likely on a saturated surface, with reversible partitioning of HONO to the gas phase, through vaporization and deposition to the surface. We observed median HONO/NO2 ratios starting at 0.13 at the beginning of the PSS period (with an apparent lower bound of 0.03), rising to median levels of ~0.30 at the end of the PSS period (with an upper bound >1.0). The implication of these numbers is that they suggest a common surface mechanism of HONO formation on terrestrial and aqueous surfaces, with an increase in the HONO/NO2 ratio with the amount of water available at the surface. The levels of HONO during the nocturnal PSS period are positively correlated with temperature, consistent with a partitioning of HONO from the surface to the gas phase with an apparent enthalpy of vaporization of ΔHSNL (HONO)=55.5±5.4 kJ mol−1. The formation mechanism on aqueous surfaces is independent of relative humidity (RH), despite observation of a negative HONO-RH correlation. A conceptual model for HONO formation on ambient aqueous surfaces is presented, with the main elements being the presence of a surface nanolayer (SNL), highly acidic and saturated with N(IV) precursors, production of HNO3, that diffuses to underlying water layers, and HONO, which partitions reversibly between the SNL and the gas phase. Implications of the conceptual model are discussed.


2005 ◽  
Vol 5 (12) ◽  
pp. 3277-3287 ◽  
Author(s):  
P. Vaattovaara ◽  
M. Räsänen ◽  
T. Kühn ◽  
J. Joutsensaari ◽  
A. Laaksonen

Abstract. New particle formation and growth has a very important role in many climate processes. However, the overall knowlegde of the chemical composition of atmospheric nucleation mode (particle diameter, d<20 nm) and the lower end of Aitken mode particles (d≤50 nm) is still insufficient. In this work, we have applied the UFO-TDMA (ultrafine organic tandem differential mobility analyzer) method to shed light on the presence of an organic fraction in the nucleation mode size class in different atmospheric environments. The basic principle of the organic fraction detection is based on our laboratory UFO-TDMA measurements with organic and inorganic compounds. Our laboratory measurements indicate that the usefulness of the UFO-TDMA in the field experiments would arise especially from the fact that atmospherically the most relevant inorganic compounds do not grow in subsaturated ethanol vapor, when particle size is 10 nm in diameter and saturation ratio is about 86% or below it. Furthermore, internally mixed particles composed of ammonium bisulfate and sulfuric acid with sulfuric acid mass fraction ≤33% show no growth at 85% saturation ratio. In contrast, 10 nm particles composed of various oxidized organic compounds of atmospheric relevance are able to grow in those conditions. These discoveries indicate that it is possible to detect the presence of organics in atmospheric nucleation mode sized particles using the UFO-TDMA method. In the future, the UFO-TDMA is expected to be an important aid to describe the composition of atmospheric newly-formed particles.


2014 ◽  
Vol 7 (1) ◽  
pp. 81-93 ◽  
Author(s):  
D. J. Miller ◽  
K. Sun ◽  
L. Tao ◽  
M. A. Khan ◽  
M. A. Zondlo

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 (NH3) is a gas-phase precursor to fine particulate matter, with implications for air quality and climate change. Currently, NH3 sensing challenges have led to a lack of widespread in situ measurements. Our open-path sensor configuration minimizes sampling artifacts associated with NH3 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 pressure-broadened 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 NH3 at 10 Hz, a mass of ~ 5 kg and consumes ~ 50 W of electrical power. The total uncertainty in NH3 measurements is 0.20 ppbv NH3 ± 10%, based on a spectroscopic calibration method. Field performance of this open-path NH3 sensor is demonstrated, with 10 Hz time resolution and a large dynamic response for in situ NH3 measurements. This sensor provides the capabilities for improved in situ gas-phase NH3 sensing relevant for emission source characterization and flux measurements.


2018 ◽  
Vol 18 (9) ◽  
pp. 6367-6380 ◽  
Author(s):  
Marja Hemmilä ◽  
Heidi Hellén ◽  
Aki Virkkula ◽  
Ulla Makkonen ◽  
Arnaud P. Praplan ◽  
...  

Abstract. We measured amines in boreal forest air in Finland both in gas and particle phases with 1 h time resolution using an online ion chromatograph (instrument for Measuring AeRosols and Gases in Ambient Air – MARGA) connected to an electrospray ionization quadrupole mass spectrometer (MS). The developed MARGA-MS method was able to separate and detect seven different amines: monomethylamine (MMA), dimethylamine (DMA), trimethylamine (TMA), ethylamine (EA), diethylamine (DEA), propylamine (PA), and butylamine (BA). The detection limits of the method for amines were low (0.2–3.1 ng m−3), the accuracy of IC-MS analysis was 11–37 %, and the precision 10–15 %. The proper measurements in the boreal forest covered about 8 weeks between March and December 2015. The amines were found to be an inhomogeneous group of compounds, showing different seasonal and diurnal variability. Total MMA (MMA(tot)) peaked together with the sum of ammonia and ammonium ions already in March. In March, monthly means for MMA were < 2.4 and 6.8 ± 9.1 ng m−3 in gas and aerosol phases, respectively, and for NH3 and NH4+ these were 52 ± 16 and 425 ± 371 ng m−3, respectively. Monthly medians in March for MMA(tot), NH3, and NH4+ were < 2.4, 19 and 90 ng m−3, respectively. DMA(tot) and TMA(tot) had summer maxima indicating biogenic sources. We observed diurnal variation for DMA(tot) but not for TMA(tot). The highest concentrations of these compounds were measured in July. Then, monthly means for DMA were < 3.1 and 8.4 ± 3.1 ng m−3 in gas and aerosol phases, respectively, and for TMA these were 0.4 ± 0.1 and 1.8 ± 0.5 ng m−3. Monthly medians in July for DMA were below the detection limit (DL) and 4.9 ng m−3 in gas and aerosol phases, respectively, and for TMA these were 0.4 and 1.4 ng m−3. When relative humidity of air was > 90 %, gas-phase DMA correlated well with 1.1–2 nm particle number concentration (R2=0.63) suggesting that it participates in atmospheric clustering. EA concentrations were low all the time. Its July means were < 0.36 and 0.4 ± 0.4 ng m−3 in gas and aerosol phases, respectively, but individual concentration data correlated well with monoterpene concentrations in July. Monthly means of PA and BA were below detection limits at all times.


2011 ◽  
Vol 71-78 ◽  
pp. 2679-2682
Author(s):  
Xiu Hua Zhu ◽  
Song Tao Qin ◽  
Qian Xu ◽  
Yu Wen Ni ◽  
Ji Ping Chen ◽  
...  

Ambient air of Dalian was sampled with active high-volume air samplers in early spring time. The concentrations and the congeners between gas phase and particulate phase of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs) in the air were measured. Samples analysis results showed that the concentration of PCDD/Fs in particulate phase was higher than that in gas phase. The ratio of PCDD to PCDF in gaseous phase and particulate phase was lower than 0.4. The main sources of atmospheric PCDD/Fs in Dalian early spring season were coal-related source. The total I-TEQ in gaseous phase and particulate phase was 30.3 and 143.6 fg m-3, respectively. The I-TEQ of Dalian early spring atmosphere was lower than international standard, the atmospheric quality in Dalian was better.


2011 ◽  
Vol 8 (4) ◽  
pp. 399 ◽  
Author(s):  
Lutz Ahrens ◽  
Mahiba Shoeib ◽  
Sabino Del Vento ◽  
Garry Codling ◽  
Crispin Halsall

Environmental contextPerfluoroalkyl compounds are of rising environmental concern because of their ubiquitous distribution in remote regions like the Arctic. The present study quantifies these contaminants in the gas and particle phases of the Canadian Arctic atmosphere. The results demonstrate the important role played by gas–particle partitioning in the transport and fate of perfluoroalkyl compounds in the atmosphere. AbstractPolyfluoroalkyl compounds (PFCs) were determined in high-volume air samples during a ship cruise onboard the Canadian Coast Guard Ship Amundsen crossing the Labrador Sea, Hudson Bay and the Beaufort Sea of the Canadian Arctic. Five PFC classes (i.e. perfluoroalkyl carboxylates (PFCAs), polyfluoroalkyl sulfonates (PFSAs), fluorotelomer alcohols (FTOHs), fluorinated sulfonamides (FOSAs), and sulfonamidoethanols (FOSEs)) were analysed separately in the gas phase collected on PUF/XAD-2 sandwiches and in the particle phase on glass-fibre filters (GFFs). The method performance of sampling, extraction and instrumental analysis were compared between two research groups. The FTOHs were the dominant PFCs in the gas phase (20–138 pg m–3), followed by the FOSEs (0.4–23 pg m–3) and FOSAs (0.5–4.7 pg m–3). The PFCAs could only be quantified in the particle phase with low levels (<0.04–0.18 pg m–3). In the particle phase, the dominant PFC class was the FOSEs (0.3–8.6 pg m–3). The particle-associated fraction followed the general trend of: FOSEs (~25 %) > FOSAs (~9 %) > FTOHs (~1 %). Significant positive correlation between ∑FOSA concentrations in the gas phase and ambient air temperature indicate that cold Arctic surfaces, such as the sea-ice snowpack and surface seawater could be influencing FOSAs in the atmosphere.


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