Biodegradation of phenol and catechol in cloud water: comparison to chemical oxidation in the atmospheric multiphase system

Abstract. The sinks of hydrocarbons in the atmosphere are usually described by oxidation reactions in the gas and aqueous (cloud) phases. Previous lab studies suggest that in addition to chemical processes, biodegradation by bacteria might also contribute to the loss of organics in clouds; however, due to the lack of comprehensive data sets on such biodegradation processes, they are not commonly included in atmospheric models. In the current study, we measured the biodegradation rates of phenol and catechol, which are known pollutants, by one of the most active strains selected during our previous screening in clouds (Rhodococcus enclensis). For catechol, biodegradation is about 10 times faster than for phenol. The experimentally derived biodegradation rates are included in a multiphase box model to compare the chemical loss rates of phenol and catechol in both the gas and aqueous phases to their biodegradation rate in the aqueous phase under atmospheric conditions. Model results show that the degradation rates in the aqueous phase by chemical and biological processes for both compounds are similar to each other. During day time, biodegradation of catechol is even predicted to exceed the chemical activity in the aqueous phase and to represent a significant sink (17 %) of total catechol in the atmospheric multiphase system. In general, our results suggest that atmospheric multiphase models may be incomplete for highly soluble organics as biodegradation may represent an unrecognized efficient loss of such organics in cloud water.

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Biodegradation of phenol and catechol in cloud water: Comparison to chemical oxidation in the atmospheric multiphase system

10.5194/acp-2019-1048 ◽

2020 ◽

Author(s):

Saly Jaber ◽

Audrey Lallement ◽

Martine Sancelme ◽

Martin Leremboure ◽

Gilles Mailhot ◽

...

Keyword(s):

Aqueous Phase ◽

Chemical Oxidation ◽

Cloud Water ◽

Multiphase System ◽

Data Sets ◽

Biological Processes ◽

Atmospheric Conditions ◽

Oxidation Reactions ◽

Atmospheric Models ◽

Degradation Rates

Abstract. The sinks of hydrocarbons in the atmosphere are usually described by oxidation reactions in the gas and aqueous (cloud) phases. Previous lab studies suggest that in addition to chemical processes, biodegradation by bacteria might also contribute to the loss of organics in clouds; however, due to the lack of comprehensive data sets on such biodegradation processes, they are not commonly included in atmospheric models. In the current study, we measured the biodegradation rates of phenol and catechol, which are known pollutants, by one of the most active strains selected during our previous screening in clouds (Rhodococcus enclensis). For catechol, biodegradation transformation is about ten times faster than for phenol. The experimentally derived biodegradation rates are included in a multiphase box model to compare the chemical loss rates of phenol and catechol in both the gas and aqueous phases to their biodegradation rate in the aqueous phase under atmospheric conditions. Model results show that the degradation rates in the aqueous phase by chemical and biological processes for both compounds are similar to each other. During daytime, biodegradation of catechol is even predicted to exceed the chemical activity in the aqueous phase and to represent a significant sink (17 %) of total catechol in the atmospheric multiphase system. In general, our results suggest that atmospheric multiphase models may be incomplete for highly soluble organics as biodegradation may represent an unrecognized efficient loss of such organics in cloud water.

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Photochemistry versus biological activity towards organics in cloud water

10.5194/egusphere-egu2020-1517 ◽

2020 ◽

Author(s):

Amina Khaled ◽

Minghui Zhang ◽

Pierre Amato ◽

Anne-Marie Delort ◽

Barbara Ervens

Keyword(s):

Biological Activity ◽

Aqueous Phase ◽

Process Model ◽

Cloud Model ◽

Liquid Water Content ◽

Cloud Water ◽

Multiphase System ◽

Reaction Rate Constants ◽

Cloud Parameters ◽

Inorganic Species

The aqueous phase of clouds is a complex atmospheric medium containing a multitude of organic and inorganic species with different reactivities. The main oxidant towards organics in the aqueous phase is the OH radical. Many studies have identified biological material as a major fraction of ambient aerosol loading with bacteria being a small fraction. Laboratory experiments in our and other research groups have shown that microbial degradation of small organics (e.g., formic and acetic acids) can efficiently occur in artificial and real cloud water in competition to chemical radical reactions. However, in current models, it is usually assumed that bacteria are not metabolically active in the atmosphere. The aim of our study is to identify conditions, under which biological activity is significant in the multiphase system for specific organic compounds. Using a cloud multiphase process model, we compare the predicted fractions of organics consumed by radicals in the gas and aqueous phases to that by microbial processes of bacteria in the aqueous phase over large ranges of microphysical (e.g., cloud liquid water content, drop number), biological (cell concentration and activity) and chemical parameters (reaction rate constants and Henry&#8217;s law constants). We identify the organic properties and cloud parameters under which metabolic processes represent major atmospheric sinks for organics. In our cloud model, we consider the fact that only a small number fraction of droplets contain active bacteria cells. As many other models might not be able to describe such microphysical details, we also suggest simplified model approaches to represent microbial activity in clouds.

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Supplementary material to "Biodegradation of phenol and catechol in cloud water: Comparison to chemical oxidation in the atmospheric multiphase system"

10.5194/acp-2019-1048-supplement ◽

2020 ◽

Author(s):

Saly Jaber ◽

Audrey Lallement ◽

Martine Sancelme ◽

Martin Leremboure ◽

Gilles Mailhot ◽

...

Keyword(s):

Chemical Oxidation ◽

Cloud Water ◽

Multiphase System ◽

Supplementary Material

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Methodology of Research in Micropollutants – Heavy Metals

Water Science & Technology ◽

10.2166/wst.1982.0037 ◽

1982 ◽

Vol 14 (12) ◽

pp. 107-125 ◽

Cited By ~ 15

Author(s):

Roland Wollast

Keyword(s):

Heavy Metals ◽

Mathematical Models ◽

Aqueous Phase ◽

Suspended Matter ◽

Solid Phase ◽

Aquatic Organisms ◽

Biological Processes ◽

Particulate Phase ◽

Sources Of Pollution ◽

Adsorption Desorption

A comparison of the concentration of dissolved and of particulate heavy metals in the aquatic system indicates that these elements are strongly enriched in the suspended matter. The transfer between the aqueous phase and the solid phase may be due to dissolution-precipitation reactions, adsorption-desorption processes or biological processes. When these processes are identified, it is further possible to develop mathematical models which describe the behaviour of these elements. The enrichment of heavy metals in the particulate phase suspended or deposited and in aquatic organisms constitutes a powerful tool in order to evaluate sources of pollution.

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Engineering motile aqueous phase-separated droplets via liposome stabilisation

Nature Communications ◽

10.1038/s41467-021-21832-x ◽

2021 ◽

Vol 12 (1) ◽

Author(s):

Shaobin Zhang ◽

Claudia Contini ◽

James W. Hindley ◽

Guido Bolognesi ◽

Yuval Elani ◽

...

Keyword(s):

Aqueous Phase ◽

Marangoni Effect ◽

Living Systems ◽

Biological Processes ◽

Biological Applications ◽

Emulsion System ◽

Biotechnological Potential ◽

New Directions ◽

Directional Motion ◽

The Stability

AbstractThere are increasing efforts to engineer functional compartments that mimic cellular behaviours from the bottom-up. One behaviour that is receiving particular attention is motility, due to its biotechnological potential and ubiquity in living systems. Many existing platforms make use of the Marangoni effect to achieve motion in water/oil (w/o) droplet systems. However, most of these systems are unsuitable for biological applications due to biocompatibility issues caused by the presence of oil phases. Here we report a biocompatible all aqueous (w/w) PEG/dextran Pickering-like emulsion system consisting of liposome-stabilised cell-sized droplets, where the stability can be easily tuned by adjusting liposome composition and concentration. We demonstrate that the compartments are capable of negative chemotaxis: these droplets can respond to a PEG/dextran polymer gradient through directional motion down to the gradient. The biocompatibility, motility and partitioning abilities of this droplet system offers new directions to pursue research in motion-related biological processes.

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The Lead Dioxide Anode. II. The Kinetics and Participation of the Lead Dioxide Electrode in Electrochemical Oxidation Reactions in Sulfuric Acid

Australian Journal of Chemistry ◽

10.1071/ch9891527 ◽

1989 ◽

Vol 42 (9) ◽

pp. 1527 ◽

Cited By ~ 3

Author(s):

TH Randle ◽

AT Kuhn

Keyword(s):

Sulfuric Acid ◽

Electrochemical Oxidation ◽

Maximum Rate ◽

Lead Dioxide ◽

Chemical Oxidation ◽

Oxidation Reactions ◽

Electrochemical Regeneration ◽

Electrode Surfaces ◽

Lead Dioxide Electrode ◽

Lead Dioxide Anode

Lead dioxide is a strong oxidizer in sulfuric acid, consequently electrochemical oxidation of solution species at a lead dioxide anode may occur by a two-step, C-E process (chemical oxidation of solution species by PbO2 followed by electrochemical regeneration of the reduced lead dioxide surface). The maximum rate of each step has been determined in sulfuric acid for specified lead dioxide surfaces and compared with the rates observed for the electrochemical oxidation of cerium(III) and manganese(II) on the same electrode surfaces. While the rate of electrochemical oxidation of a partially reduced PbO2 surface may be sufficient to support the observed rates of CeIII and MnII oxidation at the lead dioxide anode, the rate of chemical reaction between PbO2 and the reducing species is not. Hence it is concluded that the lead dioxide electrode functions as a simple, 'inert' electron-transfer agent during the electrochemical oxidation of CellI and MnII in sulfuric acid. In general, it will most probably be the rate of the chemical step which determines the feasibility or otherwise of the C-E mechanism.

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The Three-Cornered Hat Method for Estimating Error Variances of Three or More Atmospheric Data Sets – Part II: Evaluating Radio Occultation and Radiosonde Observations, Global Model Forecasts, and Reanalyses

Journal of Atmospheric and Oceanic Technology ◽

10.1175/jtech-d-20-0209.1 ◽

2021 ◽

Author(s):

Therese Rieckh ◽

Jeremiah P. Sjoberg ◽

Richard A. Anthes

Keyword(s):

Radio Occultation ◽

State Of The Art ◽

Specific Humidity ◽

Data Sets ◽

Error Growth ◽

Atmospheric Conditions ◽

Error Statistics ◽

Weather And Climate ◽

Atmospheric Data ◽

The Impact

AbstractWe apply the three-cornered hat (3CH) method to estimate refractivity, bending angle, and specific humidity error variances for a number of data sets widely used in research and/or operations: radiosondes, radio occultation (COSMIC, COSMIC-2), NCEP global forecasts, and nine reanalyses. We use a large number and combinations of data sets to obtain insights into the impact of the error correlations among different data sets that affect 3CH estimates. Error correlations may be caused by actual correlations of errors, representativeness differences, or imperfect co-location of the data sets. We show that the 3CH method discriminates among the data sets and how error statistics of observations compare to state-of-the-art reanalyses and forecasts, as well as reanalyses that do not assimilate satellite data. We explore results for October and November 2006 and 2019 over different latitudinal regions and show error growth of the NCEP forecasts with time. Because of the importance of tropospheric water vapor to weather and climate, we compare error estimates of refractivity for dry and moist atmospheric conditions.

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Impact of planetary waves on infrasound propagation uncertainties

10.5194/egusphere-egu21-15038 ◽

2021 ◽

Author(s):

Elisabeth Blanc ◽

Patrick Hupe ◽

Bernd Kaifler ◽

Natalie Kaifler ◽

Alexis Le Pichon ◽

...

Keyword(s):

Wave Activity ◽

Atmospheric Dynamics ◽

Planetary Waves ◽

Data Sets ◽

Atmospheric Models ◽

Period Range ◽

Weather Forecasts ◽

Atmospheric Disturbances ◽

Medium Range ◽

Model Improvement

The uncertainties in the infrasound technology arise from the middle atmospheric disturbances, which are partly underrepresented in the atmospheric models such as in the European Centre for Medium-Range Weather Forecasts (ECMWF) products used for infrasound propagation simulations. In the framework of the ARISE (Atmospheric dynamics Research InfraStructure in Europe) project, multi-instrument observations are performed to provide new data sets for model improvement and future assimilations. In an unexpected way, new observations using the autonomous CORAL lidar showed significant differences between ECMWF analysis fields and observations in Argentina in the period range between 0.1 and 10 days. The model underestimates the wave activity, especially in the summer. During the same season, the infrasound bulletins of the IS02 station in Argentina indicate the presence of two prevailing directions of the detections, which are not reflected by the simulations. Observations at the Haute Provence Observatory (OHP) are used for comparison in different geophysical conditions. The origin of the observed anomalies are discussed in term of planetary waves effect on the infrasound propagation.

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Aqueous-Phase Photochemical Formation of Peroxyl Radicals and Singlet Molecular Oxygen in Cloud Water Samples from Across the United States

Aquatic and Surface Photochemistry ◽

10.1201/9781351069847-20 ◽

2018 ◽

pp. 231-240

Author(s):

John M. Allen ◽

Bruce C. Faust

Keyword(s):

United States ◽

Molecular Oxygen ◽

Aqueous Phase ◽

Water Samples ◽

The United States ◽

Cloud Water ◽

Peroxyl Radicals ◽

Singlet Molecular Oxygen ◽

Photochemical Formation

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Photooxidation and ozonolysis of Δ3-carene and its oxidation product caronaldehyde in the atmospheric simulation chamber SAPHIR

10.5194/egusphere-egu21-1284 ◽

2021 ◽

Author(s):

Luisa Hantschke ◽

Anna Novelli ◽

Birger Bohn ◽

Changmin Cho ◽

David Reimer ◽

...

Keyword(s):

Oxidation Product ◽

Boreal Forests ◽

Oxidation Products ◽

Organic Nitrate ◽

Organic Nitrates ◽

Peroxy Radicals ◽

Atmospheric Conditions ◽

Oxidation Reactions ◽

Reaction Rate Constants ◽

Simulation Chamber

Of the total global annual monoterpene emissions, &#916;3-carene contributes 4.5 %, making it the 7th most abundant monoterpene worldwide. As it is primarily emitted by pine trees, &#916;3-carene can regionally gain in importance, for example in boreal forests and Mediterranean regions.&#160; Oxidation products of monoterpenes such as organic nitrates and aldehydes are known to impact the formation of secondary pollutants such as ozone and particles, so understanding their atmospheric formation and fate is crucial.The photooxidation and ozonolysis of &#916;3-carene and the photooxidation and photolysis of its main daytime photooxidation product caronaldehyde were investigated in the atmospheric simulation chamber SAPHIR. Oxidation reactions were studied under atmospheric conditions with high (> 8 ppbv) and low (< 2 ppbv) NOx concentrations. Reaction rate constants of the reaction of &#916;3-carene with OH and O3, and of the reaction of caronaldehyde with OH as well as photolysis frequencies of caronaldehyde were determined. Production and destruction rates of the sum of hydroxyl and peroxy radicals (ROx = OH+HO2+RO2) were analysed to determine if there were unaccounted production and loss processes of radicals in the oxidation of &#916;3-carene. The yield of &#916;3-carene&#8217;s oxidation product caronaldehyde was determined from measured timeseries from OH photooxidation and ozonolysis experiments. Additionally, the OH yield from ozonolysis of &#916;3-carene was determined.Organic nitrate (RONO2) yields of the reaction of RO2 + NO, from RO2 produced from the reactions of &#916;3-carene and caronaldehyde with OH were determined by analyzing the reactive nitrogen species (NOy) in the chamber.

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