scholarly journals Mapping gaseous amines, ammonia, and their particulate counterparts in marine atmospheres of China’s marginal seas: Part 1 – Differentiating marine emission from continental transport

2021 ◽  
Author(s):  
Dihui Chen ◽  
Yanjie Shen ◽  
Juntao Wang ◽  
Yang Gao ◽  
Huiwang Gao ◽  
...  

Abstract. To study sea-derived gaseous amines, ammonia, and primary particulate aminium ions in the marine atmospheres of China's marginal seas, an onboard URG-9000D Ambient Ion Monitor-Ion chromatography (AIM-IC, Thermo Fisher) was set up on the front deck of the R/V Dongfanghong 3 to semi-continuously measure the spatiotemporal variations in the concentrations of atmospheric trimethylamine (TMAgas), dimethylamine (DMAgas), and ammonia (NH3gas) along with their particulate matter (PM2.5) counterparts. In this study, we differentiated marine emissions of the gas species originating from continental transport using data obtained from December 9 to 22, 2019 during the cruise over the Yellow and Bohai Seas, facilitated by additional measurements collected at a coastal site near the Yellow Sea during summer 2019. The data obtained during the cruise and the coastal site demonstrated that the observed TMAgas and protonated trimethylamine (TMAH+) in PM2.5 over the Yellow and Bohai Seas overwhelmingly originated from marine sources. During the cruise, there was no significant correlation (P > 0.05) between the simultaneously measured TMAH+ and TMAgas concentrations. Additionally, the concentrations of TMAH+ in the marine atmosphere varied around 0.28 ± 0.18 μg m−3 (average  ±  standard deviation), with several episodic hourly average values exceeding 1 μg m−3, which were approximately one order of magnitude larger than those of TMAgas (approximately 0.031 ± 0.009 μg m−3). Moreover, there was a significant negative correlation (P < 0.01) between the concentrations of TMAH+ and NH4+ in PM2.5 during the cruise. Therefore, the observed TMAH+ in PM2.5 was overwhelmingly derived from primary sea-spray aerosols. Using the TMAgas and TMAH+ in PM2.5 as tracers for sea-derived basic gases and sea-spray particulate aminium ions, the values of non-sea-derived DMAgas and NH3gas, as well as non-sea-spray particulate DMAH+ in PM2.5, were estimated, and the estimated average values of each species contributed to 16 %, 34 %, and 65 % of the observed average concentrations, respectively. Uncertainties remained in the estimations as TMAH+ may decompose into smaller molecules in seawater to varying extents. The non-sea-derived gases and non-sea-spray particulate DMAH+ likely originated from long-range transport from the upwind continents, according to the recorded offshore winds and increased concentrations of SO42− and NH4+ in PM2.5. The lack of a detectable increase in the particulate DMAH+, NH4+, and SO42− concentrations in several SO2 plumes did not support the secondary formation of particulate DMAH+ in the marine atmosphere.

2021 ◽  
Vol 21 (21) ◽  
pp. 16413-16425
Author(s):  
Dihui Chen ◽  
Yanjie Shen ◽  
Juntao Wang ◽  
Yang Gao ◽  
Huiwang Gao ◽  
...  

Abstract. To study sea-derived gaseous amines, ammonia, and primary particulate aminium ions in the marine atmosphere of China's marginal seas, an onboard URG-9000D Ambient Ion Monitor-Ion Chromatograph (AIM-IC, Thermo Fisher) was set up on the front deck of the R/V Dongfanghong-3 to semi-continuously measure the spatiotemporal variations in the concentrations of atmospheric trimethylamine (TMAgas), dimethylamine (DMAgas), and ammonia (NH3gas) along with their particulate matter (PM2.5) counterparts. In this study, we differentiated marine emissions of the gas species from continental transport using data obtained from 9 to 22 December 2019 during the cruise over the Yellow and Bohai seas, facilitated by additional short-term measurements collected at a coastal site near the Yellow Sea during the summer, fall, and winter of 2019. The data obtained from the cruise and coastal sites demonstrated that the observed TMAgas and protonated trimethylamine (TMAH+) in PM2.5 over the Yellow and Bohai seas overwhelmingly originated from marine sources. During the cruise, no significant correlation (P>0.05) was observed between the simultaneously measured TMAH+ and TMAgas concentrations. Additionally, the concentrations of TMAH+ in the marine atmosphere varied around 0.28±0.18 µg m−3 (average ± standard deviation), with several episodic hourly average values exceeding 1 µg m−3, which were approximately 1 order of magnitude larger than those of TMAgas (approximately 0.031±0.009 µg m−3). Moreover, there was a significant negative correlation (P<0.01) between the concentrations of TMAH+ and NH4+ in PM2.5. Therefore, the observed TMAH+ in PM2.5 was overwhelmingly derived from primary sea-spray aerosols. Using TMAgas and TMAH+ in PM2.5 as tracers for sea-derived basic gases and sea-spray particulate aminium ions, the values of non-sea-derived DMAgas, NH3gas, and non-sea-spray particulate DMAH+ in PM2.5 were estimated. The estimated average values of each species contributed 16 %, 34 %, and 65 % of the observed average concentrations for non-sea-derived DMAgas, NH3gas, and non-sea-spray particulate DMAH+ in PM2.5, respectively. Uncertainties remained in the estimations, as TMAH+ may decompose into smaller molecules in seawater to varying extents. The non-sea-derived gases and non-sea-spray particulate DMAH+ likely originated from long-range transport from the upwind continents based on the recorded offshore winds and increased concentrations of non-sea-salt SO42- (nss-SO42-) and NH4+ in PM2.5. The lack of a detectable increase in particulate DMAH+, NH4+, and nss-SO42- concentrations in several SO2 plumes did not support the secondary formation of particulate DMAH+ in the marine atmosphere.


2019 ◽  
Vol 19 (1) ◽  
pp. 89-113 ◽  
Author(s):  
Yujiao Zhu ◽  
Kai Li ◽  
Yanjie Shen ◽  
Yang Gao ◽  
Xiaohuan Liu ◽  
...  

Abstract. We measured the particle number concentration, size distribution, and new particle formation (NPF) events in the marine atmosphere during six cruise campaigns over the marginal seas of China in 2011–2016 and one campaign from the marginal seas to the Northwest Pacific Ocean (NWPO) in 2014. We observed relatively frequent NPF events in the atmosphere over the marginal seas of China, i.e., on 23 out of 126 observational days, with the highest frequency of occurrence in fall, followed by spring and summer. In total, 22 out of 23 NPF events were found to be associated with the long-range transport of continental pollutants based on 24 h air mass back trajectories and pre-existing particle number concentrations, which largely exceeded the clean marine background, leaving one much weaker NPF event that was likely induced by oceanic precursors alone, as supported by multiple independent pieces of evidence. Although the long-range transport signal of continental pollutants can be clearly observed in the remote marine atmosphere over the NWPO, NPF events were observed on only 2 out of 36 days. The nucleation-mode particles (<30 nm), however, accounted for as high as 35 %±13 % of the total particle number concentration during the NWPO cruise campaign, implying the existence of many undetected NPF events in the near-sea-level atmosphere or above. To better characterize NPF events, we introduce a term called the net maximum increase in the nucleation-mode particle number concentration (NMINP) and correlate it with the formation rate of new particles (FR). We find a moderately good linear correlation between NMINP and FR at FR≤8 cm−3 s−1, but no correlation exists at FR>8 cm−3 s−1. The possible mechanisms are argued in terms of the roles of different vapor precursors. We also find that a ceiling exists for the growth of new particles from 10 nm to larger sizes in most NPF events. We thereby introduce a term called the maximum geometric median diameter of new particles (Dpgmax) and correlate it with the growth rate of new particles (GR). A moderately good linear correlation is also obtained between the Dpgmax and GR, and only GR values larger than 7.9 nm h−1 can lead to new particles growing with a Dpgmax beyond 50 nm based on the equation. By combining simultaneous measurements of the particle number size distributions and cloud condensation nuclei (CCN) at different super saturations (SS), we observed a clear increase in CCN when the Dpg of new particles exceeded 50 nm at SS=0.4 %. However, this case did not occur for SS=0.2 %. Consistent with the results of previous studies in the continental atmosphere, our results imply that particles smaller than 50 nm are unlikely activated as CCN at SS=0.4 % in the marine atmosphere. Moreover, κ decrease from 0.4 to 0.1 during the growth period of new particles, implying that organics likely overwhelm the growth of new particles to CCN size. The chemical analysis of nano-Micro-Orifice Uniform Deposit Impactor (nano-MOUDI) samples reveals that trimethylamine (TMA) and oxalic acid might appreciably contribute to the growth of new particles in some cases.


2015 ◽  
Vol 72 (9) ◽  
pp. 3487-3498 ◽  
Author(s):  
Qingjing Hu ◽  
Peiran Yu ◽  
Yujiao Zhu ◽  
Kai Li ◽  
Huiwang Gao ◽  
...  

Abstract In this paper, the concentration, the size distribution, and the formation of dimethylaminium (DMA+) and trimethylaminium (TMA+) ions in atmospheric particles were studied during a cruise campaign over the Yellow Sea and the Bohai Sea of China in May 2012. The concentrations of DMA+ and TMA+ in particles smaller than 11 µm were 4.4 ± 3.7 and 7.2 ± 7.1 nmol m−3, respectively. The two ions had a good correlation (R2 = 0.86), and both had a moderately good correlation with chlorophyll a fluorescence (R2 = 0.66–0.67). The observed concentrations were from one to three orders of magnitude larger than the concentrations reported in other marine atmospheres. They were also much larger than the values observed at a coastal site neighboring the Yellow Sea in May–June 2013. The high concentrations of DMA+ and TMA+ observed in the marine atmosphere were probably associated with local biogenic activity instead of the long-range transport of these species from adjacent continents. The calculated mole ratios of (DMA+ + TMA+) to in different-sized particles over the seas indicated that (DMA+ + TMA+) most likely played an important role in neutralizing acidic species in particles less than 0.43 µm but not in particles of other sizes. Size distributions of DMA+ and TMA+ in the marine and coastal atmospheres were analyzed in terms of the respective contribution of gas–particle partitioning, cloud/fog processing of TMA+ and DMA+, bioaerosols, and sea-salt aerosols to the observed concentrations of the two ions over the seas.


2018 ◽  
Author(s):  
Yujiao Zhu ◽  
Kai Li ◽  
Yanjie Shen ◽  
Yang Gao ◽  
Xiaohuan Liu ◽  
...  

Abstract. To study the particle number concentration, size distribution and new particle formation (NPF) events in marine atmosphere, we made measurements during six cruise campaigns over the marginal seas of China in 2011–2016 and one campaign from the marginal seas to the Northwest Pacific Ocean (NWPO) in 2014. We observed relatively frequent NPF events in the atmosphere over the marginal seas of China, i.e., 23 out of 126 observational days with the highest occurrence frequency in fall, followed by spring and summer. 22 out of 23 NPF events were analyzed to be associated with the long-range transport of continental pollutants based on 24-hr air mass back trajectories and the preexisting particle number concentrations largely exceeding the clean marine background, leaving one much weaker NPF event to be likely induced by oceanic precursors alone and supported by multiple independent evidences. Although the long-range transport signal of continental pollutants can be clearly observed in the remote marine atmosphere over the NWPO, NPF events were observed only in 2 days out of 36 days. The nucleation mode particles ( 8 cm−3 s−1. The possible mechanisms were argued in terms of roles of different vapor precursors. We also found a ceiling existing for the growth of new particles from 10 nm to larger size in most of NPF events. We thereby introduce a term, i.e., the maximum geometric median diameter of new particles (Dpgmax) and correlate it with the growth rate of new particles (GR). A moderately good linear correlation was also obtained between Dpgmax and GR, and only GR larger than 7.9 nm h−1 can lead to new particles growing with Dpgmax beyond 50 nm. Combining simultaneous measurements of the particle number size distributions and cloud condensation nuclei (CCN) at different super saturations (SS), we indeed observed a clear increase in CCN when the Dpg of new particles exceeded 50 nm at SS = 0.4 %. However, it was not the case for SS = 0.2 %. Consistent with previous studies in continental atmosphere, our results implied that 50 nm can be used as the threshold for new particles to be activated as CCN in the marine atmosphere. Moreover, the κ decreased from 0.4 to 0.1 during the growth period of new particles, implying that organics likely overwhelmed the growth of new particle to CCN size. The chemical analysis of nano-MOUDI samples revealed TMA and oxalic acid may play the important role in the growth of new particles.


2021 ◽  
Author(s):  
Yating Gao ◽  
Dihui Chen ◽  
Yanjie Shen ◽  
Yang Gao ◽  
Huiwang Gao ◽  
...  

Abstract. In this study, spatiotemporal heterogeneities in the concentrations of alkaline gases and their particulate counterparts in the marine atmosphere over China's marginal seas were investigated in terms of causes and chemical conversion during two winter cruise campaigns, using semi-continuous measurements made by an onboard URG-9000D Ambient Ion Monitor-Ion chromatograph (AIM-IC, Thermofisher). During the cruise campaign over the East China Sea on December 27, 2019–January 6, 2020, the concentrations of atmospheric trimethylamine (TMAgas) varied by approximately one order of magnitude, with an average (±standard deviation) of 0.10 ± 0.04 µg m−3. Corresponding means were 0.037 ± 0.011 µg m−3 over the Yellow Sea on 7–16 January 2020 and 0.031 ± 0.009 μg m−3 over the Yellow Sea and the Bohai Sea on 9–22 December 2019. In contrast, the simultaneously observed concentrations of TMA in PM2.5, detected as TMAH+, over the East China Sea were 0.098 ± 0.068 µg m−3 and substantially smaller than 0.28 ± 0.18 μg m−3 over the Yellow Sea and the Bohai Sea on 9–22 December 2019. A significant correlation between TMAgas and particulate TMAH+ was obtained over the East China Sea, but no correlation existed over the Yellow Sea and Bohai Sea. The proportional or disproportional variations in concentrations of TMAgas with particulate TMAH+ over the sea zones were likely attributed to the difference in enrichment of TMAH+ in the sea surface microlayer. In addition, spatiotemporal heterogeneities in concentrations of atmospheric ammonia (NH3gas), atmospheric dimethylamine (DMAgas), and DMA in PM2.5, detected as DMAH+, were also investigated. Case analyses were performed to illustrate the formation and chemical conversion of particulate aminium ions in marine aerosols. Finally, we hypothesized a release of basic gases and particulate counterparts from the ocean to the atmosphere, together with secondary formation of DMAH+ and chemical conversion of TMAH+, in the marine atmosphere.


2018 ◽  
Vol 84 (10) ◽  
pp. 23-28
Author(s):  
D. A. Golentsov ◽  
A. G. Gulin ◽  
Vladimir A. Likhter ◽  
K. E. Ulybyshev

Destruction of bodies is accompanied by formation of both large and microscopic fragments. Numerous experiments on the rupture of different samples show that those fragments carry a positive electric charge. his phenomenon is of interest from the viewpoint of its potential application to contactless diagnostics of the early stage of destruction of the elements in various technical devices. However, the lack of understanding the nature of this phenomenon restricts the possibility of its practical applications. Experimental studies were carried out using an apparatus that allowed direct measurements of the total charge of the microparticles formed upon sample rupture and determination of their size and quantity. The results of rupture tests of duralumin and electrical steel showed that the size of microparticles is several tens of microns, the particle charge per particle is on the order of 10–14 C, and their amount can be estimated as the ratio of the cross-sectional area of the sample at the point of discontinuity to the square of the microparticle size. A model of charge formation on the microparticles is developed proceeding from the experimental data and current concept of the electron gas in metals. The model makes it possible to determine the charge of the microparticle using data on the particle size and mechanical and electrical properties of the material. Model estimates of the total charge of particles show order-of-magnitude agreement with the experimental data.


2021 ◽  
Author(s):  
Parsoa Khorsand ◽  
Fereydoun Hormozdiari

Abstract Large scale catalogs of common genetic variants (including indels and structural variants) are being created using data from second and third generation whole-genome sequencing technologies. However, the genotyping of these variants in newly sequenced samples is a nontrivial task that requires extensive computational resources. Furthermore, current approaches are mostly limited to only specific types of variants and are generally prone to various errors and ambiguities when genotyping complex events. We are proposing an ultra-efficient approach for genotyping any type of structural variation that is not limited by the shortcomings and complexities of current mapping-based approaches. Our method Nebula utilizes the changes in the count of k-mers to predict the genotype of structural variants. We have shown that not only Nebula is an order of magnitude faster than mapping based approaches for genotyping structural variants, but also has comparable accuracy to state-of-the-art approaches. Furthermore, Nebula is a generic framework not limited to any specific type of event. Nebula is publicly available at https://github.com/Parsoa/Nebula.


2021 ◽  
pp. 263208432110100
Author(s):  
Satyendra Nath Chakrabartty

Background Scales for evaluating insomnia differ in number of items, response format, and result in different scores distributions and score ranges and may not facilitate meaningful comparisons. Objectives Transform ordinal item-scores of three scales of insomnia to continuous, equidistant, monotonic, normally distributed scores, avoiding limitations of summative scoring of Likert scales. Methods Equidistant item-scores by weighted sum using data-driven weights to different levels of different items, considering cell frequencies of Item-Levels matrix, followed by normalization and conversion to [1, 10]. Equivalent test-scores (as sum of transformed item- scores) for a pair of scales were found by Normal Probability curves. Empirical illustration given. Results Transformed test-scores are continuous, monotonic and followed Normal distribution with no outliers and tied scores. Such test-scores facilitate ranking, better classification and meaningful comparison of scales of different lengths and formats and finding equivalent score combinations of two scales. For a given value of transformed test-score of a scale, easy alternate method avoiding integration proposed to find equivalent scores of another scales. Equivalent scores of scales help to relate various cut-off scores of different scales and uniformity in interpretations. Integration of various scales of insomnia is achieved by finding one-to-one correspondence among the equivalent score of various scales with correlation over 0.99 Conclusion Resultant test-scores facilitated undertaking analysis in parametric set up. Considering the theoretical advantages including meaningfulness of operations, better comparison, use of such method of transforming scores of Likert items/test is recommended test and items, Future studies were suggested.


2020 ◽  
Vol 20 (11) ◽  
pp. 6687-6706
Author(s):  
Mikhail Paramonov ◽  
Saskia Drossaart van Dusseldorp ◽  
Ellen Gute ◽  
Jonathan P. D. Abbatt ◽  
Paavo Heikkilä ◽  
...  

Abstract. Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II) in the winter–spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L−1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1–0.5 µm in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 µm particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.


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