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The surface chemistry of tropospheric gas - particle interactions

Applicant Ammann Markus
Number 149492
Funding scheme Project funding (Div. I-III)
Research institution Paul Scherrer Institut
Institution of higher education Paul Scherrer Institute - PSI
Main discipline Physical Chemistry
Start/End 01.12.2013 - 31.12.2016
Approved amount 520'110.00
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All Disciplines (2)

Discipline
Physical Chemistry
Climatology. Atmospherical Chemistry, Aeronomy

Keywords (7)

photochemistry; organic aerosol; heterogeneous chemistry; aerosol; halogens; uptake coefficient; atmospheric chemistry

Lay Summary (German)

Lead
Aerosole (auch als Feinstaub bezeichnet) spielen eine wichtige Rolle in der Umwelt. Chemische Umwandlungen von Aerosolteilchen spielen dabei eine essentielle Rolle. Solche Umwandlungen werden durch den Austausch von Hauptkomponenten und Spurenstoffen zwischen Partikelphase und Gasphase getrieben. Ein besseres Verständnis dieses Austauschs und im speziellen die chemischen und physikalischen Eigenschaften der Grenzschicht zwischen Partikel- und Gasphase stehen im Zentrum dieses Projekts.
Lay summary

Chemische Reaktionen von Spurengasen mit Aerosolteilchen haben einen Einfluss auf die Oxidationskapazität der Atmosphäre und auf die Zusammensetzung der Teilchen selbst. Dieses Projekt befasst sich in drei Teilprojekten mit solchen Prozessen. Im ersten Fall geht es um die Reaktion von Distickstoffpentoxid (N2O5) mit wässrigen Aerosolteilchen. Dieser Prozess hat einen direkten Einfluss auf das Ozonbudget.

Im zweiten Fall untersuchen wir die Spaltung von organischen Verbindungen und Nitrat auf Metalloxiden, wie sie in Mineralstaub (aufgewirbelter Wüstenstaub) oder in photokatalytischen Nanomaterialien vorkommen, die als Oberflächenbeschichtung zur Reinigung von Oberflächen von Gebäuden verwendet werden. Die potentiellen Produkte von solchen Reaktionen sind Aldehyde und reduzierte Stickoxidverbindungen, die, wieder in die Gasphase entlassen, als Vorläufer für Radikale wirken und deshalb die Oxidationskapazität der Luft beeinflussen.

Im dritten Fall versuchen wir die Reaktionen von Ozon mit Meersalz-Aerosol zu verstehen, die in der Chemie von marinen Luftmassen eine wichtige Rolle spielen. Solche Reaktionen führen zur Bildung von Halogenverbindungen in der Gasphase, die einen grossen Einfluss auf die Zusammensetzung der Troposphäre haben.

Im zweiten und dritten Teilprojekt stehen neben kinetischen Untersuchungen insbesondere die chemische Zusammensetzung und die Struktur der Phasengrenze zwischen wässriger Lösung und der Gasphase im Zentrum. Dafür steht uns eine neuartige Methode zur Verfügung - Hochdruck-Röntgenphotoemission -, die es uns erlaubt die obersten Molekülschichten der wässrigen Lösung in Kontakt mit der Gasphase zu untersuchen.

Unser Projekt soll einen Beitrag leisten zu einem quantitativen Verständnis der Atmosphärenchemie und Input liefern für detaillierte atmosphärenchemische Modelle. Zusätzlich möchten wir inbesondere unser Wissen über Grenzflächenphänomene in der Umwelt erweitern.

Direct link to Lay Summary Last update: 22.10.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Efficient bulk mass accommodation and dissociation of N2O5 in neutral aqueous aerosol
Gržinić Goran, Bartels-Rausch Thorsten, Türler Andreas, Ammann Markus (2017), Efficient bulk mass accommodation and dissociation of N2O5 in neutral aqueous aerosol, in Atmospheric Chemistry and Physics, 17(10), 6493-6502.
Chemical Composition and Properties of the Liquid–Vapor Interface of Aqueous C1 to C4 Monofunctional Acid and Alcohol Solutions
Lee Ming-Tao, Orlando Fabrizio, Artiglia Luca, Chen Shuzhen, Ammann Markus (2016), Chemical Composition and Properties of the Liquid–Vapor Interface of Aqueous C1 to C4 Monofunctional Acid and Alcohol Solutions, in The Journal of Physical Chemistry A, 120(49), 9749-9758.
Introducing Time Resolution to Detect Ce 3+ Catalytically Active Sites at the Pt/CeO 2 Interface through Ambient Pressure X-ray Photoelectron Spectroscopy
Artiglia Luca, Orlando Fabrizio, Roy Kanak, Kopelent René, Safonova Olga, Nachtegaal Maarten, Huthwelker Thomas, van Bokhoven Jeroen A. (2016), Introducing Time Resolution to Detect Ce 3+ Catalytically Active Sites at the Pt/CeO 2 Interface through Ambient Pressure X-ray Photoelectron Spectroscopy, in The Journal of Physical Chemistry Letters, 8(1), 102-108.
The effect of viscosity on the HO2 uptake by sucrose and secondary organic aerosol particles
Lakey Pascale S. J., Berkemeier Thomas, Krapf Manuel, Dommen Josef, Steimer Sarah S., Whalley Lisa K., Ingham Trevor, Baeza-Romero Maria T., Pöschl Ulrich, Shiraiwa Manabu, Ammann Markus, Heard Dwayne E. (2016), The effect of viscosity on the HO2 uptake by sucrose and secondary organic aerosol particles, in Atmospheric Chemistry and Physics, 16(20), 13035-13047.
The Environmental Photochemistry of Oxide Surfaces and the Nature of Frozen Salt Solutions: A New in Situ XPS Approach
Orlando Fabrizio, Waldner Astrid, Bartels-Rausch Thorsten, Birrer Mario, Kato Shunsuke, Lee Ming-Tao, Proff Christian, Huthwelker Thomas, Kleibert Armin, van Bokhoven Jeroen, Ammann Markus (2016), The Environmental Photochemistry of Oxide Surfaces and the Nature of Frozen Salt Solutions: A New in Situ XPS Approach, in Topics in Catalysis, 59(5-7), 591-604.
Chemical Composition and Properties of the Liquid–Vapor Interface of Aqueous C1 to C4 Monofunctional Acid and Alcohol Solutions
Lee Ming-Tao, Orlando Fabrizio, Artiglia Luca, Chen Shuzhen, Ammann Markus (2016), Chemical Composition and Properties of the Liquid–Vapor Interface of Aqueous C1 to C4 Monofunctional Acid and Alcohol Solutions, in The Journal of Physical Chemistry A, 120, 9749-9758.
Organic Nitrate Contribution to New Particle Formation and Growth in Secondary Organic Aerosols from α-Pinene Ozonolysis
Berkemeier T., Ammann M., Mentel T.F., Pöschl U., Shiraiwa M. (2016), Organic Nitrate Contribution to New Particle Formation and Growth in Secondary Organic Aerosols from α-Pinene Ozonolysis, in Environmental Science & Technology, 50(12), 6334-6342.
Exploring the Environmental Photochemistry on the TiO2(110) Surface in Situ by Near Ambient Pressure X-ray Photoelectron Spectroscopy
Lampimäki M. Schreiber S. Zelenay V. Křepelová A. Birrer M. Axnanda S. Mao B. Liu Z. (2015), Exploring the Environmental Photochemistry on the TiO2(110) Surface in Situ by Near Ambient Pressure X-ray Photoelectron Spectroscopy, in The Journal of Physical Chemistry C, 119(13), 7076-7085.
Heterogeneous Photochemistry in the Atmosphere
George C. Ammann M. D’Anna B. Donaldson D. J. and Nizkorodov S. A. (2015), Heterogeneous Photochemistry in the Atmosphere, in Chemical Reviews, 115(10), 4218-4258.
Ion Spatial Distributions at the Air– and Vacuum–Aqueous K2CO3 Interfaces
Brown M. A. Lee M.-T. Kleibert A. Ammann M. and Giorgi J. B. (2015), Ion Spatial Distributions at the Air– and Vacuum–Aqueous K2CO3 Interfaces, in The Journal of Physical Chemistry C, 119(9), 4976-4982.
The Competition Between Organics and Bromide at the Aqueous Solution–Air Interface as Seen from Ozone Uptake Kinetics and X-ray Photoelectron Spectroscopy
Lee Ming-Tao, Brown Matthew A., Kato Shunsuke, Kleibert Armin, Tuerler Andreas, Ammann Markus (2015), The Competition Between Organics and Bromide at the Aqueous Solution–Air Interface as Seen from Ozone Uptake Kinetics and X-ray Photoelectron Spectroscopy, in The Journal of Physical Chemistry A, 119, 4600-4608.
Viscosity controls humidity dependence of N2O5 uptake to citric acid aerosol
Gržinić G., Bartels-Rausch T. Berkemeier T. Türler A. Ammann M. (2015), Viscosity controls humidity dependence of N2O5 uptake to citric acid aerosol, in Atmospheric Chemistry and Physics, 15, 13615-13625.
Liquid–Vapor Interface of Formic Acid Solutions in Salt Water: A Comparison of Macroscopic Surface Tension and Microscopic in Situ X-ray Photoelectron Spectroscopy Measurements
Pruyne Jefferson G., Lee Ming-Tao, Fábri Csaba, Beloqui Redondo Amaia, Kleibert Armin, Ammann Markus, Brown Matthew A., Krisch Maria J. (2014), Liquid–Vapor Interface of Formic Acid Solutions in Salt Water: A Comparison of Macroscopic Surface Tension and Microscopic in Situ X-ray Photoelectron Spectroscopy Measurements, in The Journal of Physical Chemistry C, 118(50), 29350-29360.
Production and use of 13N labeled N2O5 to determine gas–aerosol interaction kinetics
Gržinić Goran, Bartels-Rausch Thorsten, Birrer Mario, Türler Andreas, Ammann Markus (2014), Production and use of 13N labeled N2O5 to determine gas–aerosol interaction kinetics, in Radiochimica Acta, 102, 1025-1025.

Collaboration

Group / person Country
Types of collaboration
H. Herrmann, IFT Leipzig Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
D. Heard, Leeds University Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
M. Shiraiwa and U. Pöschl, Max Planck Institute for Chemistry Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
J. van Bokhoven and M. Brown, ETH Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
APXPS 2016 - 3rd Annual Workshop on Ambient Pressure X-ray Photoelectron Spectroscopy Poster HCl on the ice surface: insights from ambient pressure spectroscopies 12.12.2016 Oxford, Great Britain and Northern Ireland Orlando Fabrizio; Ammann Markus;
Seminar at Lille University Individual talk Surface reaction limited transformation of atmospheric particles: kinetics and spectroscopy 06.12.2016 Lille, France Ammann Markus;
XPS ANALYSIS : from measurements to scientific answers Poster The affinity of propionic acid and sodium propionate for the liquid-vapor interface as seen from liquid jet XPS 26.09.2016 Roscoff, France Chen Shuzhen;
Towards a molecular level understand of atmospheric aerosols Talk given at a conference TRACING HALIDE OXIDATION AT THE SEA SPRAY PARTICLE – AIR INTERFACE AND BEYOND 28.08.2016 Santa Cruz / CA, United States of America Ammann Markus;
Towards a molecular level understand of atmospheric aerosols Talk given at a conference Tracing halide oxidation at the salt solution – air interface and beyond 28.08.2016 Santa Cruz, United States of America Ammann Markus;
Seminar at University of British Columbia Talk given at a conference Surface reaction limited oxidation in atmospheric particles: kinetics and spectroscopy 26.08.2016 Vancouver, Canada Ammann Markus;
Gordon Research Conference on Atmospheric Chemistry Talk given at a conference Hockey, Waboba or snorkelling at the halide solution air interface 02.08.2016 Waterville, NH, United States of America Ammann Markus;
Seminar at Max Planck Institute for Chemistry Individual talk Surface reaction limited oxidation in atmospheric particles: kinetics and spectroscopy 30.06.2016 Mainz, Germany Ammann Markus;
The Future of X-Ray and Electron Spectroscopies Poster In Situ Cell Design for Solid/Vapor Interfaces and First Results in Environmental TiO2 Photocatalysis 15.06.2016 Uppsala, Sweden Orlando Fabrizio; Ammann Markus;
Seminar at Institute for Tropospheric Chemistry Talk given at a conference Tracing halide oxidation at the salt solution – air interface and beyond 12.05.2016 Leipzig, Germany Ammann Markus;
European Geosciences Union General Assembly 2016 Talk given at a conference Unravelling Air-Sea Interactions Driven by Photochemistry in the Sea-Surface Microlayer 17.04.2016 Wien, Austria Ammann Markus;
European Geosciences Union General Assembly 2016 Talk given at a conference Non-conventional halide oxidation pathways: oxidation by imadozle triplet and surface specific oxidation by ozone 17.04.2016 Wien, Austria Ammann Markus;
Swiss Working Group for Surface and Interface Science (SAOG) Poster Surface reactions studied by coated wall flow tubes: Temperature dependence of O3 - Br reaction over NaBr films 22.01.2016 Fribourg, Switzerland Ammann Markus;
American Chemical Society 62nd International Symposium & Exhibition Talk given at a conference Near Ambient Pressure XPS at the SLS – In Situ Cell Design for Solid/Vapor Interfaces and First Results in Environmental TiO2 Photocatalysis 18.10.2015 San Jose, CA, United States of America Orlando Fabrizio;
International workshop on: Surface Chemistry and Near-Ambient Pressure Photoemission Talk given at a conference Composition of the sea-salt solution-air interface as effected by organics 10.12.2014 Gyf-sur-Yvette, France Ammann Markus; Lee Ming-Tao; Orlando Fabrizio;
International workshop on: Surface Chemistry and Near-Ambient Pressure Photoemission Talk given at a conference Photoelectron spectroscopy on ice, mineral oxides and aqueous solutions of atmospheric relevance 10.12.2014 Gyf-sur-Yvette, France Orlando Fabrizio; Lee Ming-Tao; Ammann Markus;
AVS 61st International Symposium and Exhibition - In situ spectroscopy and microscopy focus Talk given at a conference Photoelectron spectroscopy on ice, mineral oxides and aqueous solutions of atmospheric relevance 10.11.2014 Baltimore, United States of America Ammann Markus;
Towards a molecular-level unterstanding of atmospheric aerosols Talk given at a conference The role of the surface in chemical transformations of aerosol particles 31.08.2014 Ascona, Switzerland Ammann Markus;
2014 International Aerosol Conference Poster Humidity Dependence of N2O5 Uptake to Citric Acid Aerosol Particles 28.08.2014 Bexco, Busan, Korean Republic (South Korea) Grzinic Goran;
248th American Chemical Society National Meeting & Exposition Talk given at a conference Composition of the sea-salt solution-air interface as effected by organics 11.08.2014 San Francisco, United States of America Lee Ming-Tao;
Telluride Workshop New Insights Into Gas-Phase Atmospheric Chemistry Talk given at a conference Oxidant exchange between the gas and aerosol phase: physical state effects, photochemistry and the role of surfaces 28.07.2014 Telluride, Colorado, United States of America Ammann Markus;
PhotoPAQ Conference 2014: Photocatalysis: Science and Application for Urban Air Quality Talk given at a conference Photocatalysis of NOX on TiO2 caught in the act 15.04.2014 Lyon, France Ammann Markus;
Kolloquium Physikalische Chemie ETH Zürich Individual talk The reaction of ozone with aerosol particles: 04.03.2014 Zürich, Switzerland Ammann Markus;
Evolution of Surface Science and Technologies Poster The sea-salt solution-air interfacial composition via liquid microjet XPS 24.01.2014 Fribourg, Switzerland Lee Ming-Tao;


Awards

Title Year
Poster Award SAOG - Swiss Working Group for Surface and Interface Science January 2015 2015

Associated projects

Number Title Start Funding scheme
170747 Ambient pressure XPS for operando studies of (photoelectro)chemical reactions at the solid-liquid interface 01.01.2017 R'EQUIP
130175 Heterogeneous chemistry of tropospheric aerosol particles with nitrogen oxides from trace gas kinetics, surface chemical and bulk structural perspectives 01.09.2010 Project funding (Div. I-III)
139139 Near ambient pressure photoelectron spectroscopy for environmental and catalysis research 01.12.2011 R'EQUIP
169176 Multiphase kinetics and chemistry at aqueous solution and mineral oxide - air interfaces 01.01.2017 Project funding (Div. I-III)
163074 Feedbacks between atmospheric aerosol microphysics and photochemical aging 01.01.2016 Project funding (Div. I-III)

Abstract

The atmosphere is a multiphase system of gas, solid and liquid phases. The condensed phases as part of aerosols and clouds are important ingredients of atmospheric composition, biogeochemical cycles, human health or climate. Gas - condensed phase interactions are at the origin of aerosol and cloud particle transformations that affect the atmospheric oxidation capacity or the climate forcing by aerosols and clouds. Improving our understanding of such interactions improve our assessment of the impact of human activities on atmospheric composition and climate change or human health. This project aims at investigating gas particle - interactions in terms of two aspects: i) quantifying the kinetics of important reactions in terms of net loss from the gas phase or of net gain of products in the particle or gas phase; ii) understanding the interfacial chemistry under atmospheric conditions as relevant for gas-particle reactions. The project is divided into three subprojects: A) Quantifying uptake of dinitrogen pentoxide to proxies of tropospheric particles: in this work we are interested in understanding the overall kinetics with different relevant aerosol substrates as a function of humidity, temperature and nitrate content. The proposed isotopic labeling experiments allow addressing specifically the kinetics of the disproportionation reaction of dinitrogen pentoxide (N2O5) into nitronium and nitrate ions, which is a key step in the heterogeneous hydrolysis of N2O5. B) Understanding photochemical transformations on metal oxides: in this work we will use surface spectroscopy to explore the surface chemical evolution of nitrogen and organic compounds during photocatalytic processes, in the context of both, photochemistry with mineral dust in the atmosphere and processes on TiO2 containing coatings and paints for self-cleaning and depolluting purposes. C) Investigating the impact of organic species on oxidant - sea salt interactions: This part deals with the release of halogen compounds formed by oxidation of halogenide ions by ozone in ocean water and sea salt aerosol and the role of organic species therein. This is a combination of kinetic experiments in a flow tube and surface spectroscopy on a liquid jet of model solutions.In the two main new proposed activities of this project, we put strong emphasis on surface spectroscopy experiments with near ambient pressure photoemission (NAPP) at SLS, a novel technique recently built up by our group in collaboration with partners and cofunded by SNF. This technique provides excellent opportunities in disentangling important processes at condensed matter - air interfaces of environmental materials.
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