Field Evidence of Nocturnal Multiphase Production of Iodic Acid

Environmental Science & Technology Letters, Journal Year: 2024, Volume and Issue: 11(7), P. 709 - 715

Published: June 6, 2024

Iodic acid (HIO3) is ubiquitously present in the atmosphere and has garnered extensive attention recent years for its contribution to particle formation growth. The understanding of underlying mechanisms, especially inland urban areas, remains severely limited. In this study, through concurrent measurements gas-phase iodic particulate iodine Yangtze River Delta region, we observed continuous nighttime production acid. We found that elevated concentrations ozone (O3) are required effectively form nocturnal acid, with rate which being proportional product concentration aerosol components concentration. Furthermore, was significantly lower than accumulated amount gaseous condensation. These findings suggest species, such as those deriving from condensation do not act terminal products atmospheric cycle. Instead, they can rapidly revert gas phase multiphase reactions. This process may explain why, absence significant sources on land, maintain relatively high contribute

Language: Английский

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

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 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

Language: 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, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 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

Language: Английский

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

Published: Oct. 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.

Language: Английский

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

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 58(1), P. 649 - 659

Published: Dec. 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.

Language: Английский

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Reply on RC1

Published: Jan. 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.

Language: Английский

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Revised manuscript file without editing tracks highlighted in red

Published: Jan. 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.

Language: Английский

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Comment on egusphere-2023-2084

Published: Jan. 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.

Language: Английский

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Reply on RC4

Published: Jan. 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.

Language: Английский

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Reply on RC2

Published: Jan. 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.

Language: Английский

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