東華大學圖書館 |

Chemistry of Nanoscale Solids and Organic Matter in Sustainable Water Management Systems.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Chemistry of Nanoscale Solids and Organic Matter in Sustainable Water Management Systems./
作者:	Wu, Xuanhao.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2020,
面頁冊數:	300 p.
附註:	Source: Dissertations Abstracts International, Volume: 81-10, Section: B.
Contained By:	Dissertations Abstracts International81-10B.
標題:	Environmental engineering. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=27836118
ISBN:	9798607327347

Chemistry of Nanoscale Solids and Organic Matter in Sustainable Water Management Systems.
Wu, Xuanhao.

Chemistry of Nanoscale Solids and Organic Matter in Sustainable Water Management Systems. - Ann Arbor : ProQuest Dissertations & Theses, 2020 - 300 p.

Source: Dissertations Abstracts International, Volume: 81-10, Section: B.

Thesis (Ph.D.)--Washington University in St. Louis, 2020.

This item is not available from ProQuest Dissertations & Theses.

To alleviate global water scarcity and improve public health, engineered water treatment and management systems have been developed for purifying contaminated water and desalinating brackish or ocean water. These engineered systems provide substantial amounts of potable water and lessen environmental concerns about the release of contaminated water. Wastewater treatment plants (WWTPs), water desalination plants (WDPs), and managed aquifer recharge systems (MARs) are three representative sustainable water management (SWM) systems. But the operation of all three poses two fundamental questions: (1) What is the fate of nanoscale solids (e.g., engineered nanomaterials, naturally occurring nanoparticles) in SWM systems and how will their physicochemical properties be changed when they encounter other water constituents, including cations and anions, reactive radical species, and organic matter? (2) How can our current knowledge enable more stable, scalable, and sustainable nanomaterial-based technologies for next-generation water treatment? To seek answers to these two questions, this dissertation focuses on the interface of chemistry and environmental engineering in 3 Systems: advanced oxidation processes (AOPs), managed aquifer recharge (MAR), and membrane distillation (MD), to (i) pursue in-depth and systematic investigations on solid-liquid interfacial interactions between nanoparticles and different water constituents (e.g., organic matter) in both water treatment and subsurface systems, and (ii) to utilize the knowledge obtained from fundamental mechanistic studies to develop nature-inspired nanomaterial-based membranes for sustainable water treatment.First, System 1 focused on investigating the surface chemistry of engineered nanomaterials (ENMs) in advanced oxidation processes (AOPs). The widespread industrial applications of ENMs, such as titanium oxide, cerium oxide, and graphene-based carbon materials, have increased the likelihood of their release into aquatic systems, including engineered water treatment systems, where they can undergo surface chemistry changes induced by water components. Using cerium oxide nanoparticles (CeO2 NPs) as representative ENMs, I examined on the effects of both reactive oxygen species (ROS) generated during UV/H2O2 treatment and dissolved organic matter (DOM) on the NPs' colloidal stability and surface chemistry. During UV/H2O2 treatment, superoxide radicals (O2˙−) dominated in neutralizing the surface charge of CeO2 NPs, leading to decreased electrostatic repulsive forces between nanoparticles and a higher extent of sedimentation. DOM was found to complex with the CeO2 NPs' surface and to act as a protective layer, making direct reactions between ROS and CeO2 and their impacts on colloidal stability insignificant in a short reaction period. These new findings have important implications for understanding the colloidal stability, sedimentation, and surface chemical properties of CeO2 NPs in aqueous systems where DOM and ROS are present.Second, System 2 aimed at investigating sustainable water management by managed aquifer recharge (MAR). To alleviate groundwater over-drafting, MAR has widely applied the engineered injection of secondary water sources into aquifers. However, groundwater chemistry changes induced by recharged water can significantly affect arsenic mobility in subsurface reservoir systems. Elevated arsenic mobility can result from increased oxidative dissolution of arsenic-bearing sulfide minerals, including arsenopyrite (FeAsS). In System 2, the effects of different water components, such as abundant oxyanions (i.e., phosphate, silicate, and bicarbonate) and DOM (natural and effluent organic matter), on the arsenic mobility from FeAsS were studied. Suwannee River DOM (SRDOM) was found to decrease arsenic mobility in the short term (< 6 hours) by inhibiting arsenopyrite oxidative dissolution, but it increased arsenic mobility over a longer experimental time (7 days) by inhibiting secondary iron(III) (hydr)oxide precipitation and decreasing arsenic adsorption onto iron(III) (hydr)oxide. In situ grazing incidence small-angle X-ray scattering (GISAXS) measurements suggested that SRDOM decreased iron(III) (hydr)oxide nucleus sizes and growth rates. A combined analysis of SRDOM and other proteinaceous or labile DOM (alginate, polyaspartate, and glutamate) revealed that DOM with higher molecular weights caused more increased arsenic mobility. In addition to DOM, phosphate showed a time-dependent reversed effect on arsenic mobility. In the short term (6 hours), phosphate promoted the dissolution of FeAsS through monodentate mononuclear surface complexation, while over a longer experimental time (7 days), the enhanced formation of secondary minerals, such as iron(III) (hydr)oxide (maghemite, γ-Fe2O3) and iron(III) phosphate (phosphosiderite, FePO4·2H2O), helped to decrease arsenic mobility through re-adsorption. Over the entire 7-day reaction, silicate increased arsenic mobility, and bicarbonate decreased arsenic mobility in our batch experiments. The phosphate system showed the highest amount and largest sizes of secondary precipitates among the three oxyanions (phosphate, silicate, and bicarbonate). These new observations advance our understanding of the impacts of DOM and oxyanions in injected water on arsenic mobility and on secondary precipitate formation during the geochemical transformation of arsenic-containing sulfide minerals in MAR.In many natural and engineered aquatic systems, including MAR, acid mine drainage, and hydraulic fracturing. (Abstract shortened by ProQuest).

ISBN: 9798607327347Subjects--Topical Terms:

548583
Environmental engineering.
Subjects--Index Terms:

Advanced oxidation processes

Chemistry of Nanoscale Solids and Organic Matter in Sustainable Water Management Systems.
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500 $a Source: Dissertations Abstracts International, Volume: 81-10, Section: B.
500 $a Advisor: Jun, Young-Shin.
502 $a Thesis (Ph.D.)--Washington University in St. Louis, 2020.
506 $a This item is not available from ProQuest Dissertations & Theses.
506 $a This item must not be sold to any third party vendors.
520 $a To alleviate global water scarcity and improve public health, engineered water treatment and management systems have been developed for purifying contaminated water and desalinating brackish or ocean water. These engineered systems provide substantial amounts of potable water and lessen environmental concerns about the release of contaminated water. Wastewater treatment plants (WWTPs), water desalination plants (WDPs), and managed aquifer recharge systems (MARs) are three representative sustainable water management (SWM) systems. But the operation of all three poses two fundamental questions: (1) What is the fate of nanoscale solids (e.g., engineered nanomaterials, naturally occurring nanoparticles) in SWM systems and how will their physicochemical properties be changed when they encounter other water constituents, including cations and anions, reactive radical species, and organic matter? (2) How can our current knowledge enable more stable, scalable, and sustainable nanomaterial-based technologies for next-generation water treatment? To seek answers to these two questions, this dissertation focuses on the interface of chemistry and environmental engineering in 3 Systems: advanced oxidation processes (AOPs), managed aquifer recharge (MAR), and membrane distillation (MD), to (i) pursue in-depth and systematic investigations on solid-liquid interfacial interactions between nanoparticles and different water constituents (e.g., organic matter) in both water treatment and subsurface systems, and (ii) to utilize the knowledge obtained from fundamental mechanistic studies to develop nature-inspired nanomaterial-based membranes for sustainable water treatment.First, System 1 focused on investigating the surface chemistry of engineered nanomaterials (ENMs) in advanced oxidation processes (AOPs). The widespread industrial applications of ENMs, such as titanium oxide, cerium oxide, and graphene-based carbon materials, have increased the likelihood of their release into aquatic systems, including engineered water treatment systems, where they can undergo surface chemistry changes induced by water components. Using cerium oxide nanoparticles (CeO2 NPs) as representative ENMs, I examined on the effects of both reactive oxygen species (ROS) generated during UV/H2O2 treatment and dissolved organic matter (DOM) on the NPs' colloidal stability and surface chemistry. During UV/H2O2 treatment, superoxide radicals (O2˙−) dominated in neutralizing the surface charge of CeO2 NPs, leading to decreased electrostatic repulsive forces between nanoparticles and a higher extent of sedimentation. DOM was found to complex with the CeO2 NPs' surface and to act as a protective layer, making direct reactions between ROS and CeO2 and their impacts on colloidal stability insignificant in a short reaction period. These new findings have important implications for understanding the colloidal stability, sedimentation, and surface chemical properties of CeO2 NPs in aqueous systems where DOM and ROS are present.Second, System 2 aimed at investigating sustainable water management by managed aquifer recharge (MAR). To alleviate groundwater over-drafting, MAR has widely applied the engineered injection of secondary water sources into aquifers. However, groundwater chemistry changes induced by recharged water can significantly affect arsenic mobility in subsurface reservoir systems. Elevated arsenic mobility can result from increased oxidative dissolution of arsenic-bearing sulfide minerals, including arsenopyrite (FeAsS). In System 2, the effects of different water components, such as abundant oxyanions (i.e., phosphate, silicate, and bicarbonate) and DOM (natural and effluent organic matter), on the arsenic mobility from FeAsS were studied. Suwannee River DOM (SRDOM) was found to decrease arsenic mobility in the short term (< 6 hours) by inhibiting arsenopyrite oxidative dissolution, but it increased arsenic mobility over a longer experimental time (7 days) by inhibiting secondary iron(III) (hydr)oxide precipitation and decreasing arsenic adsorption onto iron(III) (hydr)oxide. In situ grazing incidence small-angle X-ray scattering (GISAXS) measurements suggested that SRDOM decreased iron(III) (hydr)oxide nucleus sizes and growth rates. A combined analysis of SRDOM and other proteinaceous or labile DOM (alginate, polyaspartate, and glutamate) revealed that DOM with higher molecular weights caused more increased arsenic mobility. In addition to DOM, phosphate showed a time-dependent reversed effect on arsenic mobility. In the short term (6 hours), phosphate promoted the dissolution of FeAsS through monodentate mononuclear surface complexation, while over a longer experimental time (7 days), the enhanced formation of secondary minerals, such as iron(III) (hydr)oxide (maghemite, γ-Fe2O3) and iron(III) phosphate (phosphosiderite, FePO4·2H2O), helped to decrease arsenic mobility through re-adsorption. Over the entire 7-day reaction, silicate increased arsenic mobility, and bicarbonate decreased arsenic mobility in our batch experiments. The phosphate system showed the highest amount and largest sizes of secondary precipitates among the three oxyanions (phosphate, silicate, and bicarbonate). These new observations advance our understanding of the impacts of DOM and oxyanions in injected water on arsenic mobility and on secondary precipitate formation during the geochemical transformation of arsenic-containing sulfide minerals in MAR.In many natural and engineered aquatic systems, including MAR, acid mine drainage, and hydraulic fracturing. (Abstract shortened by ProQuest).
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653 $a Nanoscale solids
653 $a Organic matter
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