scholarly journals Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity

2022 ◽  
Vol 22 (1) ◽  
pp. 215-244
Author(s):  
Dalrin Ampritta Amaladhasan ◽  
Claudia Heyn ◽  
Christopher R. Hoyle ◽  
Imad El Haddad ◽  
Miriam Elser ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Liquid Phase ◽  
Relative Humidity ◽  
Water Uptake ◽  
Chemical Mechanism ◽  
European Organization ◽  
Seed Particles ◽  
Rich Liquid ◽  
Ammonium Bisulfate ◽  
Selection Of

Abstract. This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOAs) from the dark ozone-initiated oxidation of isoprene at low NOx conditions. We performed simulations of isoprene oxidation using a gas-phase chemical reaction mechanism based on the Master Chemical Mechanism (MCM) in combination with an equilibrium gas–particle partitioning model to predict the SOA concentration. The equilibrium model accounts for non-ideal mixing in liquid phases, including liquid–liquid phase separation (LLPS), and is based on the AIOMFAC (Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients) model for mixture non-ideality and the EVAPORATION (Estimation of VApour Pressure of ORganics, Accounting for Temperature, Intramolecular, and Non-additivity effects) model for pure compound vapour pressures. Measurements from the Cosmics Leaving Outdoor Droplets (CLOUD) chamber experiments, conducted at the European Organization for Nuclear Research (CERN) for isoprene ozonolysis cases, were used to aid in parameterizing the SOA yields at different atmospherically relevant temperatures, relative humidity (RH), and reacted isoprene concentrations. To represent the isoprene-ozonolysis-derived SOA, a selection of organic surrogate species is introduced in the coupled modelling system. The model predicts a single, homogeneously mixed particle phase at all relative humidity levels for SOA formation in the absence of any inorganic seed particles. In the presence of aqueous sulfuric acid or ammonium bisulfate seed particles, the model predicts LLPS to occur below ∼ 80 % RH, where the particles consist of an inorganic-rich liquid phase and an organic-rich liquid phase; however, this includes significant amounts of bisulfate and water partitioned to the organic-rich phase. The measurements show an enhancement in the SOA amounts at 85 % RH, compared to 35 % RH, for both the seed-free and seeded cases. The model predictions of RH-dependent SOA yield enhancements at 85 % RH vs. 35 % RH are 1.80 for a seed-free case, 1.52 for the case with ammonium bisulfate seed, and 1.06 for the case with sulfuric acid seed. Predicted SOA yields are enhanced in the presence of an aqueous inorganic seed, regardless of the seed type (ammonium sulfate, ammonium bisulfate, or sulfuric acid) in comparison with seed-free conditions at the same RH level. We discuss the comparison of model-predicted SOA yields with a selection of other laboratory studies on isoprene SOA formation conducted at different temperatures and for a variety of reacted isoprene concentrations. Those studies were conducted at RH levels at or below 40 % with reported SOA mass yields ranging from 0.3 % up to 9.0 %, indicating considerable variations. A robust feature of our associated gas–particle partitioning calculations covering the whole RH range is the predicted enhancement of SOA yield at high RH (> 80 %) compared to low RH (dry) conditions, which is explained by the effect of particle water uptake and its impact on the equilibrium partitioning of all components.

scholarly journals Modelling the gas–particle partitioning and water uptake of isoprene-derived secondary organic aerosol at high and low relative humidity

2021 ◽  
Author(s):  
Dalrin Ampritta Amaladhasan ◽  
Claudia Heyn ◽  
Christopher R. Hoyle ◽  
Imad El Haddad ◽  
Miriam Elser ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Liquid Phase ◽  
Relative Humidity ◽  
Chemical Mechanism ◽  
European Organization ◽  
Seed Particles ◽  
Ideal Mixing ◽  
Rich Liquid ◽  
Ammonium Bisulfate ◽  
Selection Of

Abstract. This study presents a characterization of the hygroscopic growth behaviour and effects of different inorganic seed particles on the formation of secondary organic aerosols (SOA) from the dark ozone-initiated oxidation of isoprene at low NOx conditions. We performed simulations of isoprene oxidation using a gas-phase chemical reaction mechanism based on the Master Chemical Mechanism (MCM) in combination with an equilibrium gas–particle partitioning model to predict the SOA concentration. The equilibrium model accounts for non-ideal mixing in liquid phases, including liquid–liquid phase separation (LLPS), and is based on the AIOMFAC model for mixture non-ideality and the EVAPORATION model for pure compound vapour pressures. Measurements from the Cosmics Leaving Outdoor Droplets (CLOUD) chamber experiments conducted at the European Organization for Nuclear Research (CERN) for isoprene ozonolysis cases, were used to aid in parameterizing the SOA yields at different atmospherically relevant temperatures, relative humidity (RH) and reacted isoprene concentrations. To represent the isoprene ozonolysis-derived SOA, a selection of organic surrogate species is introduced in the coupled modelling system. The model predicts a single, homogeneously mixed particle phase at all relative humidity levels for SOA formation in the absence of any inorganic seed particles. In the presence of aqueous sulfuric acid or ammonium bisulfate seed particles, the model predicts LLPS to occur below ~80 % RH, where the particles consist of an inorganic-rich liquid phase and an organic-rich liquid phase; however, with significant amounts of bisulfate and water partitioned to the organic-rich phase. The measurements show an enhancement in the SOA amounts at 85 % RH compared to 35 % RH for both the seed-free and seeded cases. The model predictions of RH-dependent SOA yield enhancements at 85 % RH vs. 35 % RH are 1.80 for a seed-free case, 1.52 for the case with ammonium bisulfate seed and 1.06 for the case with sulfuric acid seed. Predicted SOA yields are enhanced in the presence of an aqueous inorganic seed, regardless of the seed type (ammonium sulfate, ammonium bisulfate or sulfuric acid) in comparison with seed-free conditions at the same RH level. We discuss the comparison of model-predicted SOA yields with a selection of other laboratory studies on isoprene SOA formation conducted at different temperatures and for a variety of reacted isoprene concentrations.

scholarly journals Influence of Sulfuric Acid on the Performance of Ruthenium-based Catalysts in the Liquid-Phase Hydrogenation of Levulinic Acid to γ-Valerolactone

ChemSusChem ◽  
2017 ◽  
Vol 10 (14) ◽  
pp. 2891-2896 ◽  
Author(s):  
Jamal Ftouni ◽  
Homer C. Genuino ◽  
Ara Muñoz-Murillo ◽  
Pieter C. A. Bruijnincx ◽  
Bert M. Weckhuysen
Keyword(s):  
Sulfuric Acid ◽  
Liquid Phase ◽  
Levulinic Acid ◽  
Liquid Phase Hydrogenation

First global assessment of modelled aerosol hygroscopicity in the context of other aerosol optical properties

2021 ◽  
Author(s):  
Maria Ángeles Burgos Simón ◽  
Elisabeth Andrews ◽  
Gloria Titos ◽  
Angela Benedetti ◽  
Huisheng Bian ◽  
...  
Keyword(s):  
Optical Properties ◽  
Light Scattering ◽  
Relative Humidity ◽  
Water Uptake ◽  
Chem Phys ◽  
Earth System ◽  
Aerosol Optical Properties ◽  
System Models ◽  
Earth System Models

<p>The particle hygroscopic growth impacts the optical properties of aerosols and, in turn, affects the aerosol-radiation interaction and calculation of the Earth’s radiative balance. The dependence of particle light scattering on relative humidity (RH) can be described by the scattering enhancement factor f(RH), defined as the ratio between the particle light scattering coefficient at a given RH divided by its dry value.</p><p>The first effort of the AeroCom Phase III – INSITU experiment was to develop an observational dataset of scattering enhancement values at 26 sites to study the uptake of water by atmospheric aerosols, and evaluate f(RH) globally (Burgos et al., 2019). Model outputs from 10 Earth System Models (CAM, CAM-ATRAS, CAM-Oslo, GEOS-Chem, GEOS-GOCART, MERRAero, TM5, OsloCTM3, IFS-AER, and ECMWF) were then evaluated against this in-situ dataset. Building on these results, we investigate f(RH) in the context of other aerosol optical and chemical properties, making use of the same 10 Earth System Models (ESMs) and in-situ measurements as in Burgos et al. (2020) and Titos et al. (2021).</p><p>Given the difficulties of deploying and maintaining instrumentation for long-term, accurate and comprehensive f(RH) observations, it is desirable to find an observational proxy for f(RH). This observation-based proxy would also need to be reproduced in modelling space. Our aim here is to evaluate how ESMs currently represent the relationship between f(RH), scattering Ångström exponent (SAE), and single scattering albedo (SSA). This work helps to identify current challenges in modelling water-uptake by aerosols and their impact on aerosol optical properties within Earth system models.</p><p>We start by analyzing the behavior of SSA with RH, finding the expected increase with RH for all site types and models. Then, we analyze the three variables together (f(RH)-SSA-SAE relationship). Results show that hygroscopic particles tend to be bigger and scatter more than non-hygroscopic small particles, though variability within models is noticeable. This relationship can be further studied by relating SAE to model chemistry, by selecting those grid points dominated by a single chemical component (mass mixing ratios > 90%). Finally, we analyze model performance at three specific sites representing different aerosol types: Arctic, marine and rural. At these sites, the model data can be exactly temporally and spatially collocated with the observations, which should help to identify the models which exhibit better agreement with measurements and for which aerosol type.</p><p> </p><p>Burgos, M.A. et al.: A global view on the effect of water uptake on aerosol particle light scattering. Sci Data 6, 157. https://doi.org/10.1038/s41597-019-0158-7, 2019.</p><p>Burgos, M.A. et al.: A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity, Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, 2020.</p><p>Titos, G. et al.: A global study of hygroscopicity-driven light scattering enhancement in the context of other in-situ aerosol optical properties, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2020-1250, in review, 2020.</p>

scholarly journals Effects of Different Pretreatments and Seed Coat on Dormancy and Germination of Seeds of Senna obtusifolia (L.) H.S. Irwin & Barneby (Fabaceae)

2016 ◽  
Vol 8 (2) ◽  
pp. 77
Author(s):  
Stephen I. Mensah ◽  
Chimezie Ekeke
Keyword(s):  
Sulfuric Acid ◽  
Seed Dormancy ◽  
Water Uptake ◽  
Seed Coat ◽  
Critical Factor ◽  
Potassium Nitrate ◽  
Ex Situ ◽  
Mechanical Resistance ◽  
Physical Dormancy ◽  
Senna Obtusifolia

<p class="1Body">The seed dormancy of <em>Senna obtusifolia</em> was investigated through various methods, namely pretreatments in concentrated sulfuric acid, 2% potassium nitrate (KNO<sub>3</sub>), 99% ethanol, 99% methanol, and in hydrogen perioxide; examination of the seed coverings; and the determination of water uptake by the seeds in order to ascertain the most effective technique for breaking dormancy and also determine the dormancy type. The results showed that sulfuric acid treatment recorded the highest germination (100%); followed by 2% hydrogen peroxide treatment (24%) in 15minutes immersion. The methanol and ethanol pretreatments gave 18.33% and 16.5% germinations respectively. Pretreatment in 2% potassium nitrate gave the lowest germination (8.50%), while the intact seeds of <em>S. obtusifiolia</em> (control) gave 0% germination. The anatomy of the seed coat indicated the presence of hard, thickened and specialized cells of cuticle, macrosclereids, osteoscereids, and disintegrated parenchyma layers. The water uptake of intact seeds was low (13.5%) after 24 hr imbibitions. These findings revealed that the seed coat acts as barrier to germination by preventing water absorption, possibly gaseous diffusion in and out of the seed and conferring mechanical resistance to the protrusion of embryo. Pretreatments, such as immersion in H<sub>2</sub>SO<sub>4 </sub>will soften the seed coat and permit germination. Seed dormancy in <em>S. obtusifolia </em>can be considered of physical nature and classified as physical dormancy. The results obtained in this study may serve as useful information in the production and improvement of <em>S. obtusifolia </em>seedlings, as knowledge on seed dormancy and germination is a critical factor and requirements to the understanding of the propagation of this plant either in situ or ex-situ, in view of the economic potentials/attributes of this species.</p>

scholarly journals Liquid–liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride

2013 ◽  
Vol 13 (23) ◽  
pp. 11723-11734 ◽  
Author(s):  
Y. You ◽  
L. Renbaum-Wolff ◽  
A. K. Bertram
Keyword(s):  
Phase Separation ◽  
Sodium Chloride ◽  
Liquid Phase ◽  
Relative Humidity ◽  
Ammonium Sulfate ◽  
Inorganic Salt ◽  
Liquid Phase Separation ◽  
Inorganic Salts ◽  
Organic Species ◽  
Liquid Liquid Phase Separation

Abstract. As the relative humidity varies from high to low values in the atmosphere, particles containing organic species and inorganic salts may undergo liquid–liquid phase separation. The majority of the laboratory work on this subject has used ammonium sulfate as the inorganic salt. In the following we studied liquid–liquid phase separation in particles containing organics mixed with the following salts: ammonium sulfate, ammonium bisulfate, ammonium nitrate and sodium chloride. In each experiment one organic was mixed with one inorganic salt and the liquid–liquid phase separation relative humidity (SRH) was determined. Since we studied 23 different organics mixed with four different salts, a total of 92 different particle types were investigated. Out of the 92 types, 49 underwent liquid–liquid phase separation. For all the inorganic salts, liquid–liquid phase separation was never observed when the oxygen-to-carbon elemental ratio (O : C) &amp;geq; 0.8 and was always observed for O : C < 0.5. For 0.5 &amp;leq; O : C < 0.8, the results depended on the salt type. Out of the 23 organic species investigated, the SRH of 20 organics followed the trend: (NH4)2SO4 &amp;geq; NH4HSO4 &amp;geq; NaCl &amp;geq; NH4NO3. This trend is consistent with previous salting out studies and the Hofmeister series. Based on the range of O : C values found in the atmosphere and the current results, liquid–liquid phase separation is likely a frequent occurrence in both marine and non-marine environments.

scholarly journals Isolated individuals and groups show opposite preferences toward humidity

2018 ◽  
Author(s):  
Mariano Calvo Martín ◽  
Stamatios C. Nicolis ◽  
Isaac Planas-Sitjà ◽  
Jean-Christophe de Biseau ◽  
Jean-Louis Deneubourg
Keyword(s):  
Relative Humidity ◽  
Environmental Conditions ◽  
Group Level ◽  
Individual Level ◽  
Negative Effect ◽  
Multi Level ◽  
The Individual ◽  
Shed Light ◽  
Selection Of

AbstractCockroaches, like most social arthropods, are led to choose collectively among different alternative resting places. These decisions are modulated by different factors, such as environmental conditions (temperature, relative humidity) and sociality (groups size, nature of communications). The aim of this study is to establish the interplay between environmental conditions and the modulation of the interactions between individuals within a group leading to an inversion of preferences. We show that the preferences of isolated cockroaches and groups of 16 individuals, on the selection of the relative humidity of a shelter are inversed and shed light on the mechanisms involved. We suggest that the relative humidity has a multi-level influence on cockroaches, manifested as an attractant effect at the individual level and as a negative effect at the group level, modulating the interactions.

scholarly journals Deliquescence, efflorescence, and phase miscibility of mixed particles of ammonium sulfate and isoprene-derived secondary organic material

2012 ◽  
Vol 12 (4) ◽  
pp. 9903-9943 ◽  
Author(s):  
M. L. Smith ◽  
A. K. Bertram ◽  
S. T. Martin
Keyword(s):  
Liquid Phase ◽  
Relative Humidity ◽  
Ammonium Sulfate ◽  
Organic Material ◽  
Important Variable ◽  
Oxidation Products ◽  
Liquid Separation ◽  
Inorganic Particles ◽  
Photo Oxidation ◽  
Hygroscopic Properties

Abstract. The hygroscopic phase transitions of ammonium sulfate mixed with isoprene-derived secondary organic material were investigated in aerosol experiments. The organic material was produced by isoprene photo-oxidation at 40% relative humidity. The low volatility fraction of the photo-oxidation products condensed onto ammonium sulfate particles. The particle-phase organic material had oxygen-to-carbon ratios of 0.67 to 0.74 for mass concentrations of 20 to 30 μg m−3. The deliquescence, efflorescence, and phase miscibility of the mixed particles were investigated using a dual arm tandem differential mobility analyzer. The isoprene photo-oxidation products induced deviations in behavior relative to pure ammonium sulfate. Compared to an efflorescence relative humidity (ERH) of 30 to 35% for pure ammonium sulfate, efflorescence was eliminated for mixed aqueous particles having organic volume fractions ε of approximately 0.6 and greater. Compared to a deliquescence relative humidity (DRH) of 80% for pure ammonium sulfate, the DRH steadily decreased for increasing ε, approaching a DRH of 40% for ε of 0.9. Parameterizations of the DRH(ε) and ERH(ε) curves were as follows: DRH(ε)= Σ i ci,d xi valid for 0 ≤ ε ≤ 0.86 and ERH(ε)= Σ i ci,e xi valid for 0 ≤ ε ≤ 0.55 for the coefficients c0,d= 80.67, c0,e = 28.35, c1,d= −11.45, c1,e = −13.66, c2,d = 0, c2,e = 0, c3,d = 57.99, c3,e = −83.80, c4,d = −106.80, and c4,d = 0. The molecular description that is thermodynamically implied by these strongly sloped DRH(ε) and ERH(ε) curves is that the organic isoprene photo-oxidation products, the inorganic ammonium sulfate, and water form a miscible liquid phase even at low relative humidity. This phase miscibility is in contrast to the liquid-liquid separation that occurs for some other types of secondary organic material. These differences in liquid-liquid separation are consistent with a prediction recently presented in the literature that the bifurcation between liquid-liquid phase separation versus mixing depends on the oxygen-to-carbon ratio of the organic material. The conclusions are that the influence of secondary organic material on the hygroscopic properties of ammonium sulfate varies with organic composition and that the degree of oxygenation of the organic material, which is a measurable characteristic of complex organic materials, is an important variable influencing the hygroscopic properties of mixed organic-inorganic particles.

scholarly journals KRETERIA DESAIN FOTOBIOREAKTOR SISTEM AIRLIFT REACTOR

2016 ◽  
Vol 11 (1) ◽  
pp. 27
Author(s):  
Arif Dwi Santoso ◽  
Abdil H.S ◽  
Diyono .
Keyword(s):  
Global Warming ◽  
Carbon Capture ◽  
Human Life ◽  
Co2 Reduction ◽  
Chemical Mechanism ◽  
Co2 Uptake ◽  
Environmental Technology ◽  
Negative Impacts ◽  
Air Lift ◽  
Selection Of

Global warming has become an increasingly important issue around the world today due to the rise of anthropogenic greenhouse gases emission, which gives several negative impacts on human life. There are some techniques have been studied and assessed i.e. physical mechanism by injected CO2 to the geological formations, chemical mechanism with artificial tree technology and biological mechanism by increasing the primary production through iron enrichment in high nutrient-low chlorophyll (HNLC) waters as well as mixing of water column below the sea surface. Those technologies, which are well known as Carbon Capture Storage ‘(CCS) technology, are expected to be applied to reduce the oncentration of anthropogenic CO2 in the atmosphere and to minimize the global warming. The Center of Environmental Technology, Agency for the Assessment and Application of Technology (BPPT) will carry out a research concerning CO2 reduction by a phytoplankton culture in a photobioreactor in three years. The main objective of this research is to assess the CO2 uptake capability of tropical phytoplankton. In this paper, we would showed the creteria and design to assembly a photobioreactor esspesially a air lift photobioreactor. To improve performance photobioreaktor, the materials included design criteria and the dynamics of fluids in fotobioreaktor have to considered propoerly. Other the hand, the selection of the most productive species and selection of appropriate media and economically also important to be done. Keywords: global warming, creteria and design, greenhouse gas, air lift photobioreactor

Hg-rich liquid-phase epitaxy of Hg1−xCdxTe

1994 ◽  
Vol 29 (1-4) ◽  
pp. 41-83 ◽  
Author(s):  
M.H. Kalisher ◽  
P.E. Herning ◽  
T. Tung
Keyword(s):  
Liquid Phase ◽  
Liquid Phase Epitaxy ◽  
Rich Liquid
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