scholarly journals The impact of molecular self-organisation on the atmospheric fate of a cooking aerosol proxy

2021 ◽  
Author(s):  
Adam Milsom ◽  
Adam M. Squires ◽  
Andrew D. Ward ◽  
Christian Pfrang

Abstract. Atmospheric aerosols influence the climate via cloud droplet nucleation and can facilitate the long-range transport of harmful pollutants. The lifetime of such aerosols can therefore determine their environmental impact. Fatty acids are found in organic aerosol emissions with oleic acid, an unsaturated fatty acid, being a large contributor to cooking emissions. As a surfactant, oleic acid can self-organise into nanostructured lamellar bilayers with its sodium salt, and this self-organisation can influence reaction kinetics. We developed a kinetic multi-layer model-based description of decay data we obtained from laboratory experiments of the ozonolysis of coated films of this self-organised system, demonstrating a decreased diffusivity for both oleic acid and ozone due to lamellar bilayer formation. Diffusivity was further inhibited by a viscous oligomer product forming in the surface layers of the film. Our results indicate that nanostructure formation can increase the reactive half-life of oleic acid by an order of days at typical indoor and outdoor atmospheric ozone concentrations. We are now able to place nanostructure formation in an atmospherically meaningful and quantifiable context. These results have implications for the transport of harmful pollutants and the climate.

2011 ◽  
Vol 24 (7) ◽  
pp. 1897-1912 ◽  
Author(s):  
Wojciech W. Grabowski ◽  
Hugh Morrison

Abstract This paper extends the previous cloud-resolving modeling study concerning the impact of cloud microphysics on convective–radiative quasi equilibrium (CRQE) over a surface with fixed characteristics and prescribed solar input, both mimicking the mean conditions on earth. The current study applies sophisticated double-moment warm-rain and ice microphysics schemes, which allow for a significantly more realistic representation of the impact of aerosols on precipitation processes and on the coupling between clouds and radiative transfer. Two contrasting cloud condensation nuclei (CCN) characteristics are assumed, representing pristine and polluted conditions, as well as contrasting representations of the effects of entrainment and mixing on the mean cloud droplet size. In addition, four sets of sensitivity simulations are also performed with changes that provide a reference for the main simulation set. As in the previous study, the CRQE mimics the estimates of globally and annually averaged water and energy fluxes across the earth’s atmosphere. There are some differences from the previous study, however, consistent with the slightly lower water vapor content in the troposphere and significantly reduced lower-tropospheric cloud fraction in current simulations. There is also a significant reduction of the difference between the pristine and polluted cases, from ∼20 to ∼4 W m−2 at the surface from ∼20 to ∼9 W m−2 at the top of the atmosphere (TOA). The difference between the homogeneous and extremely inhomogeneous mixing scenarios, ∼20 W m−2 in the previous study, is reduced to a mere 2 (1) W m−2 at the surface (TOA). An unexpected difference between the previous and current simulations is the lower Bowen ratio of the surface heat flux, the partitioning of the total flux into sensible and latent components. It is shown that most of the change comes from the difference in the representation of rain evaporation in the subcloud layer in the single- and double-moment microphysics schemes. The difference affects the mean air temperature and humidity near the surface, and thus the Bowen ratio. The differences between the various simulations are discussed, contrasting the process-level approach with the impact of cloud microphysics on the quasi-equilibrium state with a more appropriate system dynamics approach. The key distinction is that the latter includes the interactions among all the processes in the modeled system.


2007 ◽  
Vol 64 (8) ◽  
pp. 2839-2861 ◽  
Author(s):  
Hugh Morrison ◽  
Wojciech W. Grabowski

This paper discusses the development and testing of a bulk warm-rain microphysics model that is capable of addressing the impact of atmospheric aerosols on ice-free clouds. Similarly to previous two-moment bulk schemes, this model predicts the mixing ratios and number concentrations of cloud droplets and drizzle/raindrops. The key elements of the model are the relatively sophisticated cloud droplet activation scheme and a comprehensive treatment of the collision–coalescence mechanism. For the latter, three previously published schemes are selected and tested, with a detailed (bin) microphysics model providing the benchmark. The unique aspect of these tests is that they are performed using a two-dimensional prescribed-flow (kinematic) framework, where both advective transport and gravitational sedimentation are included. Two quasi-idealized test cases are used, the first mimicking a single large eddy in a stratocumulus-topped boundary layer and the second representing a single shallow convective cloud. These types of clouds are thought to be the key in the indirect aerosol effect on climate. Two different aerosol loadings are considered for each case, corresponding to either pristine or polluted environments. In general, all three collision–coalescence schemes seem to capture key features of the bin model simulations (e.g., cloud depth, droplet number concentration, cloud water path, effective radius, precipitation rate, etc.) for the polluted and pristine environments, but there are detailed differences. Two of the collision–coalescence schemes require specification of the width of the cloud droplet spectrum, and model results show significant sensitivity to the specification of the width parameter. Sensitivity tests indicate that a one-moment version of the bulk model for drizzle/rain, which predicts rain/drizzle mixing ratio but not number concentration, produces significant errors relative to the bin model.


2016 ◽  
pp. 3564-3575 ◽  
Author(s):  
Ara Sergey Avetisyan

The efficiency of virtual cross sections method and MELS (Magneto Elastic Layered Systems) hypotheses application is shown on model problem about distribution of wave field in thin surface layers of waveguide when plane wave signal is propagating in it. The impact of surface non-smoothness on characteristics of propagation of high-frequency horizontally polarized wave signal in isotropic elastic half-space is studied. It is shown that the non-smoothness leads to strong distortion of the wave signal over the waveguide thickness and along wave signal propagation direction as well.  Numerical comparative analysis of change in amplitude and phase characteristics of obtained wave fields against roughness of weakly inhomogeneous surface of homogeneous elastic half-space surface is done by classical method and by proposed approach for different kind of non-smoothness.


2021 ◽  
Vol 13 (4) ◽  
pp. 640
Author(s):  
Sadroddin Alavipanah ◽  
Dagmar Haase ◽  
Mohsen Makki ◽  
Mir Muhammad Nizamani ◽  
Salman Qureshi

The changing climate has introduced new and unique challenges and threats to humans and their environment. Urban dwellers in particular have suffered from increased levels of heat stress, and the situation is predicted to continue to worsen in the future. Attention toward urban climate change adaptation has increased more than ever before, but previous studies have focused on indoor and outdoor temperature patterns separately. The objective of this research is to assess the indoor and outdoor temperature patterns of different urban settlements. Remote sensing data, together with air temperature data collected with temperature data loggers, were used to analyze land surface temperature (outdoor temperature) and air temperature (indoor temperature). A hot and cold spot analysis was performed to identify the statistically significant clusters of high and low temperature data. The results showed a distinct temperature pattern across different residential units. Districts with dense urban settlements show a warmer outdoor temperature than do more sparsely developed districts. Dense urban settlements show cooler indoor temperatures during the day and night, while newly built districts show cooler outdoor temperatures during the warm season. Understanding indoor and outdoor temperature patterns simultaneously could help to better identify districts that are vulnerable to heat stress in each city. Recognizing vulnerable districts could minimize the impact of heat stress on inhabitants.


2020 ◽  
Vol 20 (8) ◽  
pp. 5019-5033 ◽  
Author(s):  
Yuning Xie ◽  
Gehui Wang ◽  
Xinpei Wang ◽  
Jianmin Chen ◽  
Yubao Chen ◽  
...  

Abstract. The Chinese government has exerted strict emission controls to mitigate air pollution since 2013, which has resulted in significant decreases in the concentrations of air pollutants such as SO2. Strict pollution control actions also reduced the average PM2.5 concentration to the low level of 39.7 µg m−3 in urban Beijing during the winter of 2017. To investigate the impact of such changes on the physiochemical properties of atmospheric aerosols in China, we conducted a comprehensive observation focusing on PM2.5 in Beijing during the winter of 2017. Compared with the historical record (2014–2017), SO2 decreased to the low level of 3.2 ppbv in the winter of 2017, but the NO2 level was still high (21.4 ppbv in the winter of 2017). Accordingly, the contribution of nitrate (23.0 µg m−3) to PM2.5 far exceeded that of sulfate (13.1 µg m−3) during the pollution episodes, resulting in a significant increase in the nitrate-to-sulfate molar ratio. The thermodynamic model (ISORROPIA II) calculation results showed that during the PM2.5 pollution episodes particle pH increased from 4.4 (moderate acidic) to 5.4 (more neutralized) when the molar ratio of nitrate to sulfate increased from 1 to 5, indicating that aerosols were more neutralized as the nitrate content elevated. Controlled variable tests showed that the pH elevation should be attributed to nitrate fraction increase other than crustal ion and ammonia concentration increases. Based on the results of sensitivity tests, future prediction for the particle acidity change was discussed. We found that nitrate-rich particles in Beijing at low and moderate humid conditions (RH: 20 %–50 %) can absorb twice the amount of water that sulfate-rich particles can, and the nitrate and ammonia with higher levels have synergetic effects, rapidly elevating particle pH to merely neutral (above 5.6). As moderate haze events might occur more frequently under abundant ammonia and nitrate-dominated PM2.5 conditions, the major chemical processes during haze events and the control target should be re-evaluated to obtain the most effective control strategy.


2015 ◽  
Vol 8 (4) ◽  
pp. 4307-4323
Author(s):  
P. Wu ◽  
X. Dong ◽  
B. Xi

Abstract. In this study, we retrieve and document drizzle properties, and investigate the impact of drizzle on cloud property retrievals from ground-based measurements at the ARM Azores site from June 2009 to December 2010. For the selected cloud and drizzle samples, the drizzle occurrence is 42.6% with a maximum of 55.8% in winter and a minimum of 35.6% in summer. The annual means of drizzle liquid water path LWPd, effective radius rd, and number concentration Nd for the rain (virga) samples are 5.48 (1.29) g m−2, 68.7 (39.5) μm, and 0.14 (0.38) cm−3. The seasonal mean LWPd values are less than 4% of the MWR-retrieved LWP values. The annual mean differences in cloud-droplet effective radius with and without drizzle are 0.12 and 0.38 μm, respectively, for the virga and rain samples. Therefore, we conclude that the impact of drizzle on cloud property retrievals is insignificant at the ARM Azores site.


Author(s):  
Takuya Kubo ◽  
Jisun Im ◽  
Xin Wang ◽  
James E. Whitten ◽  
Koji Otsuka ◽  
...  

Author(s):  
Aidan Hughes ◽  
Sung Yun Jun ◽  
Camillo Gentile ◽  
Derek Caudill ◽  
Jack Chuang ◽  
...  

2012 ◽  
Vol 37 (1) ◽  
pp. 40-47 ◽  
Author(s):  
Aleksandra Arsić ◽  
Vesna Vučić ◽  
Jasna Tepšić ◽  
Sanja Mazić ◽  
Marina Djelić ◽  
...  

The impact of chronic, intense exercise, such as in elite athletes, on phospholipids fatty acids (FA) composition has not been studied in women so far. This study aimed to investigate FA profiles in plasma and erythrocytes phospholipids in elite female water polo (N = 15) and football (N = 19) players in comparison with sedentary women. In spite of similar dietary patterns, as assessed by a food frequency questionnaire, plasma FA profile in the football players showed significantly higher proportions of stearic acid, oleic acid, and monounsaturated FA (MUFA), and significantly lower proportions of total and n-6 polyunsaturated FA (PUFA) than in the water polo and control group. The water polo players had higher percentages of palmitoleic acid and arachidonic acid than the control subjects. Erythrocyte FA profile differed among groups. We found significantly higher proportion of oleic acid and MUFA in the football group than in the controls, and decreased stearic acid and elevated palmitic and palmitoleic acid in the water polo players than in the other 2 groups. Both groups of athletes had significantly lower percentages of n-6 dihomo-γ-linolenic acid, n-6 PUFA, and total PUFA compared with the controls. The estimated activities of elongase and desaturases in erythrocytes were also altered in the athletes. Our results indicate that long-term, intense physical training significantly affects FA status of plasma and erythrocyte phospholipids in women. The observed differences between the water polo and the football players suggest that the type of regular training may contribute to the altered metabolism of FA, although possible genetic differences among the 3 study groups cannot be ruled out.


2016 ◽  
Vol 16 (2) ◽  
pp. 777-797 ◽  
Author(s):  
A Vara-Vela ◽  
M. F. Andrade ◽  
P. Kumar ◽  
R. Y. Ynoue ◽  
A. G. Muñoz

Abstract. The objective of this work is to evaluate the impact of vehicular emissions on the formation of fine particles (PM2.5;  ≤  2.5 µm in diameter) in the Sao Paulo Metropolitan Area (SPMA) in Brazil, where ethanol is used intensively as a fuel in road vehicles. The Weather Research and Forecasting with Chemistry (WRF-Chem) model, which simulates feedbacks between meteorological variables and chemical species, is used as a photochemical modelling tool to describe the physico-chemical processes leading to the evolution of number and mass size distribution of particles through gas-to-particle conversion. A vehicular emission model based on statistical information of vehicular activity is applied to simulate vehicular emissions over the studied area. The simulation has been performed for a 1-month period (7 August–6 September 2012) to cover the availability of experimental data from the NUANCE-SPS (Narrowing the Uncertainties on Aerosol and Climate Changes in Sao Paulo State) project that aims to characterize emissions of atmospheric aerosols in the SPMA. The availability of experimental measurements of atmospheric aerosols and the application of the WRF-Chem model made it possible to represent some of the most important properties of fine particles in the SPMA such as the mass size distribution and chemical composition, besides allowing us to evaluate its formation potential through the gas-to-particle conversion processes. Results show that the emission of primary gases, mostly from vehicles, led to a production of secondary particles between 20 and 30 % in relation to the total mass concentration of PM2.5 in the downtown SPMA. Each of PM2.5 and primary natural aerosol (dust and sea salt) contributed with 40–50 % of the total PM10 (i.e. those  ≤  10 µm in diameter) concentration. Over 40 % of the formation of fine particles, by mass, was due to the emission of hydrocarbons, mainly aromatics. Furthermore, an increase in the number of small particles impaired the ultraviolet radiation and induced a decrease in ozone formation. The ground-level O3 concentration decreased by about 2 % when the aerosol-radiation feedback is taken into account.


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