scholarly journals Effect of Bulk Composition on the Heterogeneous Oxidation of Semi-Solid Atmospheric Aerosols

Atmosphere ◽  
2019 ◽  
Vol 10 (12) ◽  
pp. 791
Author(s):  
Hanyu Fan ◽  
Fabien Goulay

The OH-initiated heterogeneous oxidation of semi-solid saccharide particles with varying bulk compositions was investigated in an atmospheric pressure flow tube at 30% relative humidity. Reactive uptake coefficients were determined from the rate loss of the saccharide reactants measured by mass spectrometry at different monosaccharide (methyl-β-d-glucopyranoside, C7H14O6) and disaccharide (lactose, C12H22O11) molar ratios. The reactive uptake for the monosaccharide was found to decrease from 0.53 ± 0.10 to 0.05 ± 0.06 as the mono-to-disaccharide molar ratio changed from 8:1 to 1:1. A reaction–diffusion model was developed in order to determine the effect of chemical composition on the reactive uptake. The observed decays can be reproduced using a Vignes relationship to predict the composition dependence of the reactant diffusion coefficients. The experimental data and model results suggest that the addition of the disaccharide significantly increases the particle viscosity leading to slower mass transport phenomena from the bulk to the particle surface and to a decreased reactivity. These findings illustrate the impact of bulk composition on reactant bulk diffusivity which determines the rate-limiting step during the chemical transformation of semi-solid particles in the atmosphere.

2011 ◽  
Vol 11 (14) ◽  
pp. 7343-7354 ◽  
Author(s):  
C. Pfrang ◽  
M. Shiraiwa ◽  
U. Pöschl

Abstract. Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.


2011 ◽  
Vol 11 (4) ◽  
pp. 13003-13033 ◽  
Author(s):  
C. Pfrang ◽  
M. Shiraiwa ◽  
U. Pöschl

Abstract. Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles representative of atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant time scales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.


2021 ◽  
Vol 29 (1) ◽  
Author(s):  
Kamrun Nahar Keya ◽  
Md. Kamrujjaman ◽  
Md. Shafiqul Islam

AbstractIn this paper, we consider a reaction–diffusion model in population dynamics and study the impact of different types of Allee effects with logistic growth in the heterogeneous closed region. For strong Allee effects, usually, species unconditionally die out and an extinction-survival situation occurs when the effect is weak according to the resource and sparse functions. In particular, we study the impact of the multiplicative Allee effect in classical diffusion when the sparsity is either positive or negative. Negative sparsity implies a weak Allee effect, and the population survives in some domain and diverges otherwise. Positive sparsity gives a strong Allee effect, and the population extinct without any condition. The influence of Allee effects on the existence and persistence of positive steady states as well as global bifurcation diagrams is presented. The method of sub-super solutions is used for analyzing equations. The stability conditions and the region of positive solutions (multiple solutions may exist) are presented. When the diffusion is absent, we consider the model with and without harvesting, which are initial value problems (IVPs) and study the local stability analysis and present bifurcation analysis. We present a number of numerical examples to verify analytical results.


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.


2020 ◽  
Author(s):  
Rinke J. van Tatenhove-Pel ◽  
Tomaž Rijavec ◽  
Aleš Lapanje ◽  
Iris van Swam ◽  
Emile Zwering ◽  
...  

AbstractMetabolic interactions between cells affect microbial community compositions and hence their function in ecosystems. It is well-known that under competition for the exchanged metabolite, concentration gradients constrain the distances over which interactions can occur. However, interaction distances are typically quantified in two-dimensional systems or without accounting for competition or other metabolite-removal, conditions which may not very often match natural ecosystems. We here analyze the impact of cell-to-cell distance on unidirectional cross-feeding in a three-dimensional system with competition for the exchanged metabolite. Effective interaction distances were computed with a reaction-diffusion model and experimentally verified by growing a synthetic consortium of 1 µm-sized metabolite producer, receiver and competitor cells in different spatial structures. We show that receivers cannot interact with producers ∼15 µm away from them, as product concentration gradients flatten close to producer cells. We developed an aggregation protocol and created variants of the receiver cells’ import system, to show that within producer-receiver aggregates even low affinity receiver cells could interact with producers. These results show that competition or other metabolite-removal of a public good in a three-dimensional system reduces the interaction distance to the low micrometer-range, highlighting the importance of concentration gradients as physical constraint for cellular interactions.


2019 ◽  
Vol 16 (150) ◽  
pp. 20180674 ◽  
Author(s):  
Gabriel E. Leventhal ◽  
Martin Ackermann ◽  
Konstanze T. Schiessl

Many microorganisms secrete molecules that interact with resources outside of the cell. This includes, for example, enzymes that degrade polymers like chitin, and chelators that bind trace metals like iron. In contrast to direct uptake via the cell surface, such release strategies entail the risk of losing the secreted molecules to environmental sinks, including ‘cheating’ genotypes. Nevertheless, such secretion strategies are widespread, even in the well-mixed marine environment. Here, we investigate the benefits of a release strategy whose efficiency has frequently been questioned: iron uptake in the ocean by secretion of iron chelators called siderophores. We asked the question whether the release itself is essential for the function of siderophores, which could explain why this risky release strategy is widespread. We developed a reaction–diffusion model to determine the impact of siderophore release on iron uptake from the predominant iron sources in marine environments, colloidal or particulate iron, formed due to poor iron solubility. We found that release of siderophores is essential to accelerate iron uptake, as secreted siderophores transform slowly diffusing large iron particles to small, quickly diffusing iron–siderophore complexes. In addition, we found that cells can synergistically share their siderophores, depending on their distance and the size of the iron sources. Our study helps understand why release of siderophores is so widespread: even though a large fraction of siderophores is lost, the solubilization of iron through secreted siderophores can efficiently increase iron uptake, especially if siderophores are produced cooperatively by several cells. Overall, resource uptake mediated via release of molecules transforming their substrate could be essential to overcome diffusion limitation specifically in the cases of large, aggregated resources. In addition, we find that including the reaction of the released molecule with the substrate can impact the result of cooperative and competitive interactions, making our model also relevant for release-based uptake of other substrates.


2019 ◽  
Vol 29 (14) ◽  
pp. 1930040 ◽  
Author(s):  
Qianqian Zheng ◽  
Jianwei Shen ◽  
Zhijie Wang

P53 plays a vital role in DNA repair, and several mathematical models of the p53-Mdm2 feedback loop were used to explain the biological mechanism. In this paper, a p53-Mdm2 model described by a delay reaction–diffusion equation is studied both analytically and numerically. This research aims to provide an understanding of the impact of delay and sustained pressure on the p53-Mdm2 dynamics and tries to explain some biological mechanism. It is found that the type of pattern formation is affected by Hopf bifurcation. Also, the amplitude equation in delay diffusive system is derived and it is shown that sustained stress plays an essential role in the function of p53. Finally, simulation is used to verify the theoretical results.


2019 ◽  
Vol 9 (1) ◽  
Author(s):  
Nick Pepper ◽  
Luca Gerardo-Giorda ◽  
Francesco Montomoli

Abstract Invasive species are recognized as a significant threat to biodiversity. The mathematical modeling of their spatio-temporal dynamics can provide significant help to environmental managers in devising suitable control strategies. Several mathematical approaches have been proposed in recent decades to efficiently model the dispersal of invasive species. Relying on the assumption that the dispersal of an individual is random, but the density of individuals at the scale of the population can be considered smooth, reaction-diffusion models are a good trade-off between model complexity and flexibility for use in different situations. In this paper we present a continuous reaction-diffusion model coupled with arbitrary Polynomial Chaos (aPC) to assess the impact of uncertainties in the model parameters. We show how the finite elements framework is well-suited to handle important landscape heterogeneities as elevation and the complex geometries associated with the boundaries of an actual geographical region. We demonstrate the main capabilities of the proposed coupled model by assessing the uncertainties in the invasion of an alien species invading the Basque Country region in Northern Spain.


2003 ◽  
Vol 39 (3-4) ◽  
pp. 407-425
Author(s):  
Jaroslav Sesták

The notion of heat is thoroughly analyzed and its historical links are search particularly with relation to both the Greek philosophy (Mile in print sians Pythagoreans, atomists, etc) and the in the present day thermal physics. Fluctuation, spontaneity and chaos is discussed. Thermodynamics is reviewed in the relation to both the traditional development and the modern description of disequilibria (open systems). Effect of dissipation is shown often to provide new, self-organized structures. Exploitation of fire and its conscious use as a manufacturing power are analyzed in terms of generalized engines to act in the sense of as the information transducers. The part 2 reveals the impact of mathematics as explained on some simple cases showing development of basic ideas (vibration, topology, bifurcations etc). Earth thermal environment is discussed in relation to the existence of life (antropy principles). Alternative theory of reaction-diffusion model of the space-time is put in contrast with big bang hypothesis and related to the herewith-discussed specialty of self-catalyzed chemical reactions. The text gives a consistent view to various historical and modern concepts that emerged during the gradual understanding of order and disorder.


2021 ◽  
Vol 0 (0) ◽  
pp. 0
Author(s):  
Deborah Lacitignola ◽  
Massimo Frittelli ◽  
Valerio Cusimano ◽  
Andrea De Gaetano

<p style='text-indent:20px;'>In this study, the formation of the adult sea urchin shape is rationalized within the Turing's theory paradigm. The emergence of protrusions from the expanding underlying surface is described through a reaction-diffusion model with Gray-Scott kinetics on a growing oblate spheroid. The case of slow exponential isotropic growth is considered. The model is first studied in terms of the spatially homogenous equilibria and of the bifurcations involved. Turing diffusion-driven instability is shown to occur and the impact of the slow exponential growth on the resulting Turing regions adequately discussed. Numerical investigations validate the theoretical results showing that the combination between an inhibitor and an activator can result in a distribution of spot concentrations that underlies the development of ambulacral tentacles in the sea urchin's adult stage. Our findings pave the way for a model-driven experimentation that could improve the current biological understanding of the gene control networks involved in patterning.</p>


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