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De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal.

Record Type:	Electronic resources : Monograph/item
Title/Author:	De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal./
Author:	Cui, Yanbin.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2019,
Description:	207 p.
Notes:	Source: Dissertations Abstracts International, Volume: 81-03, Section: B.
Contained By:	Dissertations Abstracts International81-03B.
Subject:	Environmental engineering. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=13881383
ISBN:	9781085635516

De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal.
Cui, Yanbin.

De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal. - Ann Arbor : ProQuest Dissertations & Theses, 2019 - 207 p.

Source: Dissertations Abstracts International, Volume: 81-03, Section: B.

Thesis (Ph.D.)--State University of New York at Buffalo, 2019.

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

Cr(VI) is an important raw material that is used and released from various industrial sectors, such as electroplating, leather tanning, and paint production. This heavy metal is highly toxic to humans and ecosystems due to its oxidizing and mutagenic properties. Among various Cr(VI) remediation materials, iron/carbon (Fe/C) nanocomposites can efficiently remove Cr(VI) due to synergistic adsorption and reduction, and its magnetic property facilitates material recovery for regeneration. While various Fe/C preparation methods are available, concerns exist related to cost-effectiveness and scalability associated with the precursor, process, and energy demand. Conventionally, Fe/C composites for Cr(VI) removal are prepared by impregnating an iron precursor solution onto porous carbon, followed by calcination and pyrolysis. However, this method is slow, non-continuous, and labor intensive, requiring a series of discrete steps that each requires energy input. Therefore, an overarching goal for this study is to develop procedures that allow for efficient and scalable production of Fe/C nanocomposites for Cr(VI) removal.This study applies de novo synthesis strategies for material production. For Fe/C synthesis, de novo indicates that processing begins with the raw precursors, combining carbonization, activation, functionalization, and metal impregnation into a single-step process. Reported single-step processes include one-pot thermal treatment (batch) and spray pyrolysis (continuous). For the batch one-pot method, a solution/slurry containing carbon and iron precursors is heated in an inert gas to form carbon products with well-dispersed iron nanoparticles. For the continuous ultrasonic spray pyrolysis (USP) method, a precursor solution is aerosolized and pyrolyzed to decompose metal and carbon precursors, generating carbon spheres with well-dispersed iron nanoparticles. Two types of waste-based precursors are considered in this research due to their unique properties that facilitate de novo synthesis of Fe/C. Glycerol, a by-product of the biodiesel industry, and harmful algal bloom (HABs) biomass were considered. Both of these wastes can be viewed favorably as precursors for producing carbon-based, pollution prevention materials. This study begins by describing the relationship between glycerol-to-AC conversion and the physical, chemical, and adsorption properties of glycerol-derived AC. Formation mechanisms of unique physically and chemically tailored ACs were identified using sulfuric or phosphoric acid-mediated dehydration, polymerization, and carbonization of glycerol, followed by steam or CO2 activation. With this understanding, a one-pot batch pyrolysis was established to synthesize magnetic mesoporous Fe/C adsorbents from glycerol while tailoring their porous structure and oxygen groups by varying precursors and processing conditions. The practical application value of the materials for Cr(VI) treatment in wastewater was demonstrated. Alternatively, a continuous production process for generating Fe/C microspheres from a glycerol-containing precursor via USP was established. In this part, iron and template salts are shown to impact Fe/C composite chemistry, with the goal of producing materials with tailored surface functional groups and iron oxidation states.To address the pressing and local environmental concern of HABs in Lake Erie, HAB biomass was considered as a sustainable precursor for Fe/C production. To comprehensively compare aqueous pollutant removal by HAB-derived materials, three pollution prevention products, a biosorbent, an AC, and Fe/C, were prepared from HAB biomass for Cr(VI) and phenol removal. This component of the dissertation also identified how physiochemical property variability for each material class is related to its preparation methodology and subsequent performance in water treatment applications. Finally, two Fe/C preparation methods applying the HAB biomass precursor, iron bioaccumulation or iron biosorption, were investigated. This part reveals how the iron precursor and loading method impact resulting Fe/C properties, Cr(VI) removal performance, and material stability and reusability. This is the first study to develop de novo synthesis processes to prepare Fe/C composites from two well-publicized wastes, glycerol and HAB biomass. This work streamlined multi-step production methods into two different one-step processes via de novo synthesis approaches, enhancing production efficiency and scalability. Prepared Fe/C materials are applied for Cr(VI) removal, considering equilibrium, kinetics, environmental conditions (e.g., pH, ion strength, water matrix), material reuse, and a real wastewater matrix. This interdisciplinary research highlights an opportunity to convert waste-based precursors into materials that prevent aqueous pollution, and has implications for sustainable waste management, environmental engineering, and materials science/engineering.

ISBN: 9781085635516Subjects--Topical Terms:

548583
Environmental engineering.
Subjects--Index Terms:

Cr(VI) treatment

De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal.
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245 1 0 $a De novo Synthesis of Iron/Carbon Composites from Waste Precursors for Hexavalent Chromium Removal.
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500 $a Source: Dissertations Abstracts International, Volume: 81-03, Section: B.
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506 $a This item must not be sold to any third party vendors.
520 $a Cr(VI) is an important raw material that is used and released from various industrial sectors, such as electroplating, leather tanning, and paint production. This heavy metal is highly toxic to humans and ecosystems due to its oxidizing and mutagenic properties. Among various Cr(VI) remediation materials, iron/carbon (Fe/C) nanocomposites can efficiently remove Cr(VI) due to synergistic adsorption and reduction, and its magnetic property facilitates material recovery for regeneration. While various Fe/C preparation methods are available, concerns exist related to cost-effectiveness and scalability associated with the precursor, process, and energy demand. Conventionally, Fe/C composites for Cr(VI) removal are prepared by impregnating an iron precursor solution onto porous carbon, followed by calcination and pyrolysis. However, this method is slow, non-continuous, and labor intensive, requiring a series of discrete steps that each requires energy input. Therefore, an overarching goal for this study is to develop procedures that allow for efficient and scalable production of Fe/C nanocomposites for Cr(VI) removal.This study applies de novo synthesis strategies for material production. For Fe/C synthesis, de novo indicates that processing begins with the raw precursors, combining carbonization, activation, functionalization, and metal impregnation into a single-step process. Reported single-step processes include one-pot thermal treatment (batch) and spray pyrolysis (continuous). For the batch one-pot method, a solution/slurry containing carbon and iron precursors is heated in an inert gas to form carbon products with well-dispersed iron nanoparticles. For the continuous ultrasonic spray pyrolysis (USP) method, a precursor solution is aerosolized and pyrolyzed to decompose metal and carbon precursors, generating carbon spheres with well-dispersed iron nanoparticles. Two types of waste-based precursors are considered in this research due to their unique properties that facilitate de novo synthesis of Fe/C. Glycerol, a by-product of the biodiesel industry, and harmful algal bloom (HABs) biomass were considered. Both of these wastes can be viewed favorably as precursors for producing carbon-based, pollution prevention materials. This study begins by describing the relationship between glycerol-to-AC conversion and the physical, chemical, and adsorption properties of glycerol-derived AC. Formation mechanisms of unique physically and chemically tailored ACs were identified using sulfuric or phosphoric acid-mediated dehydration, polymerization, and carbonization of glycerol, followed by steam or CO2 activation. With this understanding, a one-pot batch pyrolysis was established to synthesize magnetic mesoporous Fe/C adsorbents from glycerol while tailoring their porous structure and oxygen groups by varying precursors and processing conditions. The practical application value of the materials for Cr(VI) treatment in wastewater was demonstrated. Alternatively, a continuous production process for generating Fe/C microspheres from a glycerol-containing precursor via USP was established. In this part, iron and template salts are shown to impact Fe/C composite chemistry, with the goal of producing materials with tailored surface functional groups and iron oxidation states.To address the pressing and local environmental concern of HABs in Lake Erie, HAB biomass was considered as a sustainable precursor for Fe/C production. To comprehensively compare aqueous pollutant removal by HAB-derived materials, three pollution prevention products, a biosorbent, an AC, and Fe/C, were prepared from HAB biomass for Cr(VI) and phenol removal. This component of the dissertation also identified how physiochemical property variability for each material class is related to its preparation methodology and subsequent performance in water treatment applications. Finally, two Fe/C preparation methods applying the HAB biomass precursor, iron bioaccumulation or iron biosorption, were investigated. This part reveals how the iron precursor and loading method impact resulting Fe/C properties, Cr(VI) removal performance, and material stability and reusability. This is the first study to develop de novo synthesis processes to prepare Fe/C composites from two well-publicized wastes, glycerol and HAB biomass. This work streamlined multi-step production methods into two different one-step processes via de novo synthesis approaches, enhancing production efficiency and scalability. Prepared Fe/C materials are applied for Cr(VI) removal, considering equilibrium, kinetics, environmental conditions (e.g., pH, ion strength, water matrix), material reuse, and a real wastewater matrix. This interdisciplinary research highlights an opportunity to convert waste-based precursors into materials that prevent aqueous pollution, and has implications for sustainable waste management, environmental engineering, and materials science/engineering.
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