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Characterizing the Effects of Aeroso...

Chen, Yuzhi.

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Characterizing the Effects of Aerosol Sulfate, Phase State and Aging on Atmospheric Secondary Organic Aerosol Formation from Isoprene Epoxydiols.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Characterizing the Effects of Aerosol Sulfate, Phase State and Aging on Atmospheric Secondary Organic Aerosol Formation from Isoprene Epoxydiols./
Author:	Chen, Yuzhi.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2021,
Description:	237 p.
Notes:	Source: Dissertations Abstracts International, Volume: 82-12, Section: B.
Contained By:	Dissertations Abstracts International82-12B.
Subject:	Environmental science. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28265130
ISBN:	9798516059315

Characterizing the Effects of Aerosol Sulfate, Phase State and Aging on Atmospheric Secondary Organic Aerosol Formation from Isoprene Epoxydiols.
Chen, Yuzhi.

Characterizing the Effects of Aerosol Sulfate, Phase State and Aging on Atmospheric Secondary Organic Aerosol Formation from Isoprene Epoxydiols. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 237 p.

Source: Dissertations Abstracts International, Volume: 82-12, Section: B.

Thesis (Ph.D.)--The University of North Carolina at Chapel Hill, 2021.

This item must not be sold to any third party vendors.

Atmospheric fine particulate matter (PM2.5, aerosols with aerodynamic diameters <= 2.5 μm) has a key role in Earth's climate system as well as adversely affects air quality and human health. Organic matter is a substantial PM2.5 component and is mostly generated from atmospheric oxidations of volatile organic compounds (VOCs). Atmospheric oxidation of isoprene, the most abundant VOC emitted from trees, is currently estimated to contribute ~ 30% of the global organic mass fraction of PM2.5. Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), key isoprene oxidation products under low-nitric oxide (NO) conditions, with acidic inorganic sulfate (Sulfinorg) aerosol yields substantial amounts of secondary organic aerosol (SOA) through rapid formation of polyols, low-volatility organosulfates (OSs) and oligomers. Over the last decade, IEPOX multiphase chemistry has been recognized as the main source of isoprene-derived SOA. However, unknowns/uncertainties in the formation/sink pathways, formation/sink rates, and resulting chemical composition of isoprene-derived SOA have led to underestimations of PM2.5 mass in isoprene-rich regions by current air quality and climate models.This dissertation research combines laboratory experiments, field measurements, and modeling to fundamentally improve our detailed chemical understanding of the effects of aerosol sulfate, phase state, and aging on the atmospheric transformation of IEPOX into PM2.5. Laboratory experiments revealed rapid conversion of acidic Sulfinorg aerosol into particulate OSs by IEPOX, resulting in measurable and predicted changes in aerosol physicochemical properties, which impeded additional IEPOX multiphase reactivity. These effects were tentatively investigated by a chamber box model, with the outcome anticipated to change the predicted IEPOX-derived SOA mass by large-scale chemical transport models. Heterogeneous hydroxyl radical (•OH) oxidation (or aging) of IEPOX-derived OSs was found to yield highly oxygenated multifunctional OSs, and these laboratory findings were further confirmed by the chemical characterization of ambient PM2.5 samples collected from field measurements. This dissertation provides new mechanistic insights into the formation/sink mechanisms, kinetics, chemical composition, and changes in aerosol physicochemical properties of IEPOX-derived SOA. As these aspects are highly interdependent, it is critical for existing air quality and climate models to consider these new findings to improve the prediction of IEPOX-derived SOA, and ultimately their public health and climatic impacts.

ISBN: 9798516059315Subjects--Topical Terms:

677245
Environmental science.
Subjects--Index Terms:

Aerosol sulfate

Characterizing the Effects of Aerosol Sulfate, Phase State and Aging on Atmospheric Secondary Organic Aerosol Formation from Isoprene Epoxydiols.
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500 $a Source: Dissertations Abstracts International, Volume: 82-12, Section: B.
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506 $a This item must not be sold to any third party vendors.
520 $a Atmospheric fine particulate matter (PM2.5, aerosols with aerodynamic diameters <= 2.5 μm) has a key role in Earth's climate system as well as adversely affects air quality and human health. Organic matter is a substantial PM2.5 component and is mostly generated from atmospheric oxidations of volatile organic compounds (VOCs). Atmospheric oxidation of isoprene, the most abundant VOC emitted from trees, is currently estimated to contribute ~ 30% of the global organic mass fraction of PM2.5. Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), key isoprene oxidation products under low-nitric oxide (NO) conditions, with acidic inorganic sulfate (Sulfinorg) aerosol yields substantial amounts of secondary organic aerosol (SOA) through rapid formation of polyols, low-volatility organosulfates (OSs) and oligomers. Over the last decade, IEPOX multiphase chemistry has been recognized as the main source of isoprene-derived SOA. However, unknowns/uncertainties in the formation/sink pathways, formation/sink rates, and resulting chemical composition of isoprene-derived SOA have led to underestimations of PM2.5 mass in isoprene-rich regions by current air quality and climate models.This dissertation research combines laboratory experiments, field measurements, and modeling to fundamentally improve our detailed chemical understanding of the effects of aerosol sulfate, phase state, and aging on the atmospheric transformation of IEPOX into PM2.5. Laboratory experiments revealed rapid conversion of acidic Sulfinorg aerosol into particulate OSs by IEPOX, resulting in measurable and predicted changes in aerosol physicochemical properties, which impeded additional IEPOX multiphase reactivity. These effects were tentatively investigated by a chamber box model, with the outcome anticipated to change the predicted IEPOX-derived SOA mass by large-scale chemical transport models. Heterogeneous hydroxyl radical (•OH) oxidation (or aging) of IEPOX-derived OSs was found to yield highly oxygenated multifunctional OSs, and these laboratory findings were further confirmed by the chemical characterization of ambient PM2.5 samples collected from field measurements. This dissertation provides new mechanistic insights into the formation/sink mechanisms, kinetics, chemical composition, and changes in aerosol physicochemical properties of IEPOX-derived SOA. As these aspects are highly interdependent, it is critical for existing air quality and climate models to consider these new findings to improve the prediction of IEPOX-derived SOA, and ultimately their public health and climatic impacts.
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