研究目的
Investigating the oxidation of a monolayer model for the air–water interface of marine aerosols by nitrate radicals (NO3?), focusing on the effects on pure and mixed films with palmitic acid and palmitoleic acid, and the role of subphase composition.
研究成果
NO3? oxidation does not fully remove model marine aerosol monolayers on atmospherically relevant timescales, with saturated tails remaining at the interface. The presence of CaCl2 in the subphase significantly extends the lifetime of unsaturated tails due to enhanced chain interactions, suggesting that aerosols may retain surfactant coatings longer than previously thought, impacting surface tension and chemical transport.
研究不足
The IRRAS data are semi-quantitative and sensitive to orientation changes; evaporation affects IRRAS focus over time; deuterated POA was not available, limiting detailed analysis; the study focuses on model systems, which may not fully represent real atmospheric conditions.
1:Experimental Design and Method Selection:
The study used a combination of neutron reflectometry (NR) and Fourier transform infra-red reflection absorption spectroscopy (IRRAS) in a custom-designed setup to observe mixed organic monolayers at the air–water interface in situ. Brewster angle microscopy (BAM) was used for complementary structural analysis.
2:Sample Selection and Data Sources:
Monolayers were prepared using galactocerebroside (GCB), palmitic acid (PA), and palmitoleic acid (POA) spread from chloroform solutions on pure water or CaCl2 subphases. Deuterated versions were used for NR contrast.
3:List of Experimental Equipment and Materials:
Equipment included a neutron reflectometer (INTER at ISIS), FTIR spectrometer (Thermo-Nicolet iS50), BAM (Accurion Nanofilm EP3-096), Langmuir trough, gas flow systems for NO3? generation, and various chemicals from suppliers like Sigma Aldrich.
4:Experimental Procedures and Operational Workflow:
Monolayers were spread on the subphase, and NO3? was introduced. NR and IRRAS data were collected simultaneously at intervals, with BAM used for offline characterization. Data were analyzed using MOTOFIT for NR and peak integration for IRRAS.
5:Data Analysis Methods:
NR data were fitted to extract surface coverage using models in MOTOFIT, while IRRAS data provided semi-quantitative trends in CH and CD bond concentrations.
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FTIR Spectrometer
iS50
Thermo-Nicolet
Used for in situ Fourier transform infra-red reflection absorption spectroscopy (IRRAS) to monitor CH and CD bonds in monolayers.
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Neutron Reflectometer
INTER
ISIS Neutron and Muon Source
Used for specular neutron reflectometry to measure surface coverage and thickness of monolayers.
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Brewster Angle Microscope
EP3-096
Accurion
Used for Brewster angle microscopy (BAM) to visualize monolayer morphology and structure.
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Langmuir Trough
DLS1140
NIMA
Used for preparing and compressing monolayers, with surface pressure measurement.
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Ozoniser
SOG-2
Ultra-Violet Products Ltd.
Used to generate ozone (O3) from oxygen for producing nitrate radicals.
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Syringe
50 μL spade-ended
Hamilton
Used to spread monolayer solutions onto the subphase.
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D2O
Sigma Aldrich
Used to prepare null-reflecting water subphases for neutron reflectometry.
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CaCl2
General Purpose Grade
Fisher Scientific
Used to prepare salt subphases for experiments.
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CHCl3
Sigma Aldrich
Used as a solvent for spreading monolayer components.
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d31-PA
Sigma Aldrich
Deuterated palmitic acid used in mixed monolayers for neutron contrast.
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GCB
Sigma Aldrich
Galactocerebroside used as a model compound for monolayers.
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PA
Sigma Aldrich
Palmitic acid used in mixed monolayers.
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POA
Sigma Aldrich
Palmitoleic acid used in mixed monolayers.
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NO2 Gas
1000 ppm in air
Scientific and Technical Gases Ltd.
Used to generate nitrate radicals in the gas flow system.
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O2 Gas
BOC
Used as a carrier gas and for ozone generation.
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