Atmospheric Bases-Enhanced Iodic Acid Nucleation: Altitude-Dependent Characteristics and Molecular Mechanisms

Environmental Science & Technology, Год журнала: 2024, Номер unknown

Опубликована: Сен. 9, 2024

Iodic acid (IA), the key driver of marine aerosols, is widely detected within gas and particle phases in boundary layer (MBL) even free troposphere (FT). Although atmospheric bases like dimethylamine (DMA) ammonia (NH

Язык: Английский

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Adsorption Dynamics of Heavy Oil Droplets on Silica: Effect of Asphaltene Anionic Carboxylic

Journal of Molecular Graphics and Modelling, Год журнала: 2024, Номер 133, С. 108880 - 108880

Опубликована: Окт. 10, 2024

Язык: Английский

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Sulfuric Acid-Driven Nucleation Enhanced by Amines from Ethanol Gasoline Vehicle Emission: Machine Learning Model and Mechanistic Study

Environmental Science & Technology, Год журнала: 2024, Номер unknown

Опубликована: Дек. 5, 2024

The sulfuric acid (SA)-amine nucleation mechanism gained increasing attention due to its important role in atmospheric secondary particle formation. However, the intrinsic enhancing potential (IEP) of various amines remains largely unknown, restraining assessment on SA-amines at locations. Herein, machine learning (ML) models were constructed for high-throughput prediction IEP amines, and specific with high was investigated. formation free energy (Δ

Язык: Английский

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Molecular-level study on the role of methanesulfonic acid in iodine oxoacids nucleation

Опубликована: Окт. 11, 2023

Abstract. Iodic acid (HIO3) and iodous (HIO2) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO3-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO3-HIO2 process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO3 HIO2 jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO2. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO2-MSA binary HIO3-HIO2-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO3-HIO2-based cluster formation, even up 104-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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HIO₃–HIO₂-Driven Three-Component Nucleation: Screening Model and Cluster Formation Mechanism

Environmental Science & Technology, Год журнала: 2023, Номер 58(1), С. 649 - 659

Опубликована: Дек. 22, 2023

Iodine oxoacids (HIO3 and HIO2)-driven nucleation has been suggested to efficiently contribute new particle formation (NPF) in marine atmospheres. Abundant atmospheric precursors may further enhance HIO3–HIO2-driven through various multicomponent mechanisms. However, the specific enhancing potential (EP) of different remains largely unknown. Herein, EP-based screening model mechanism precursor with highest EP on HIO3–HIO2 were investigated. The free energies (ΔG), as critical parameters for evaluating EP, calculated dimers 63 selected HIO2. Based ΔG values, (1) a quantitative structure–activity relationship was developed other (2) concentrations (precursor)1(HIO2)1 dimer clusters assessed identify by combining earlier results HIO3 partner. Methanesulfonic acid (MSA) found be one EP. Finally, we that MSA can effectively at conditions studying larger MSA–HIO3–HIO2 clusters. These augment our current understanding MSA-driven suggest impact HIO2 aerosol nucleation.

Язык: Английский

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Reply on RC1

Опубликована: Янв. 4, 2024

Abstract. Iodic acid (HIO₃) and iodous (HIO₂) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO₃-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO₃-HIO₂ process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO₃ HIO₂ jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO₂. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO₂-MSA binary HIO₃-HIO₂-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO₃-HIO₂-based cluster formation, even up 10⁴-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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Revised manuscript file without editing tracks highlighted in red

Опубликована: Янв. 4, 2024

Abstract. Iodic acid (HIO₃) and iodous (HIO₂) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO₃-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO₃-HIO₂ process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO₃ HIO₂ jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO₂. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO₂-MSA binary HIO₃-HIO₂-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO₃-HIO₂-based cluster formation, even up 10⁴-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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Comment on egusphere-2023-2084

Опубликована: Янв. 4, 2024

Abstract. Iodic acid (HIO₃) and iodous (HIO₂) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO₃-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO₃-HIO₂ process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO₃ HIO₂ jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO₂. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO₂-MSA binary HIO₃-HIO₂-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO₃-HIO₂-based cluster formation, even up 10⁴-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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Reply on RC4

Опубликована: Янв. 4, 2024

Abstract. Iodic acid (HIO₃) and iodous (HIO₂) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO₃-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO₃-HIO₂ process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO₃ HIO₂ jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO₂. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO₂-MSA binary HIO₃-HIO₂-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO₃-HIO₂-based cluster formation, even up 10⁴-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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Reply on RC2

Опубликована: Янв. 4, 2024

Abstract. Iodic acid (HIO₃) and iodous (HIO₂) have been identified to nucleate effectively by the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment at CERN (He et al., 2021, Science), yet it may be hard explain all HIO₃-induced nucleation. Given complexity of marine atmosphere, other precursors involved. Methanesulfonic (MSA), as a widespread precursor over oceans, has proven play vital role in facilitating However, its kinetic impacts on synergistic nucleation iodine oxoacids remain unclear. Hence, we investigated MSA-involved HIO₃-HIO₂ process molecular level using density functional theory (DFT) Atmospheric Clusters Dynamic Code (ACDC). The results show that MSA can form stable clusters with HIO₃ HIO₂ jointly via hydrogen halogen bonds, well electrostatic attraction after proton transfer HIO₂. Thermodynamically, clustering occur nearly without free-energy barrier, following HIO₂-MSA binary HIO₃-HIO₂-MSA ternary pathway. Furthermore, adding significantly enhance rate HIO₃-HIO₂-based cluster formation, even up 10⁴-fold cold regions rich scarce iodine, such polar Ny-Ålesund Marambio. Thus, proposed more efficient mechanism provide theoretical evidence for explaining frequent intensive burst particles.

Язык: Английский

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