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Transition Metal Catalysts for the Reduction and Utilization of Carbon Dioxide.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Transition Metal Catalysts for the Reduction and Utilization of Carbon Dioxide./
Author:	Rondeau, Jarec.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2019,
Description:	142 p.
Notes:	Source: Dissertations Abstracts International, Volume: 81-04, Section: B.
Contained By:	Dissertations Abstracts International81-04B.
Subject:	Inorganic chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=22622056
ISBN:	9781687965103

Transition Metal Catalysts for the Reduction and Utilization of Carbon Dioxide.
Rondeau, Jarec.

Transition Metal Catalysts for the Reduction and Utilization of Carbon Dioxide. - Ann Arbor : ProQuest Dissertations & Theses, 2019 - 142 p.

Source: Dissertations Abstracts International, Volume: 81-04, Section: B.

Thesis (Ph.D.)--University of New Hampshire, 2019.

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

The rising concentration of atmospheric carbon dioxide (CO2) has been viewed as the source of a growing list of environmental problems. This greenhouse gas is a waste product from the burning of fossil fuels and one of the largest producers of CO2 emissions is electricity generation. As the need for energy generation grows worldwide, emissions have shown little indication of decreasing without large scale changes to electricity generation methods. Currently, carbon capture and storage technologies are one of the more widely utilized methods of preventing emissions at the source of generation. Broad adoption of carbon capture methods is expensive, however, and requires retrofitting of aging infrastructure. In order to offset that cost, utilization of CO2 as a feedstock for chemical transformations and solar fuels has been investigated. CO2 is a highly stable molecule, which makes these transformations an energy intensive procedure.In this work, several approaches were investigated for the transformation and utilization of CO2. In our investigation of hybrid catalysts, progress was made toward the synthesis of surface immobilized Ni(0) complexes for the use of CO2 in carboxylation of unsaturated hydrocarbons. The dicarbonyl Ni(0) complexes provided valuable insight into the effects of surface immobilization on this method of converting CO2 to industrially relevant products. Immobilization of Fe(III)-bipyridine catalysts was investigated for the oxidation of terminal olefins. Covalent attachment of these complexes to inert silica surfaces was investigated as a method to produce a robust and recyclable catalyst. Variation in the linker functional group was investigated as a method to tune product selectivity and improve conversion. The electronic effect of imine functionalization of Re(I)-bipyridine complexes on CO2 reduction was investigated. The stability of the complexes covalently attached to silica surfaces was investigated and the imine functionalization was observed to have interesting effects on the formation of deactivating species.A series of homogeneous Re(I) complexes were investigated for the photocatalytic reduction of CO2. An aliphatic imine derivatized bipyridine complex displayed interesting electrochemical properties. Expanding upon this structure, a series of thiocarbazide derivatives were investigated to promote hydrogen bonding interactions towards a dimeric reduction of CO2. Carbon nitride (C3N4) was investigated as a photosensitizer for these catalytic systems. Preliminary work towards the use of hydrogen bonding interactions and covalent attachment of complexes to C3N4 was performed to promote efficient electron transfer from photoexcited C3N4 surfaces to Re(I) catalysts.

ISBN: 9781687965103Subjects--Topical Terms:

3173556
Inorganic chemistry.
Subjects--Index Terms:

Transition metal catalysts

Transition Metal Catalysts for the Reduction and Utilization of Carbon Dioxide.
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500 $a Source: Dissertations Abstracts International, Volume: 81-04, Section: B.
500 $a Advisor: Li, Gonghu.
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520 $a The rising concentration of atmospheric carbon dioxide (CO2) has been viewed as the source of a growing list of environmental problems. This greenhouse gas is a waste product from the burning of fossil fuels and one of the largest producers of CO2 emissions is electricity generation. As the need for energy generation grows worldwide, emissions have shown little indication of decreasing without large scale changes to electricity generation methods. Currently, carbon capture and storage technologies are one of the more widely utilized methods of preventing emissions at the source of generation. Broad adoption of carbon capture methods is expensive, however, and requires retrofitting of aging infrastructure. In order to offset that cost, utilization of CO2 as a feedstock for chemical transformations and solar fuels has been investigated. CO2 is a highly stable molecule, which makes these transformations an energy intensive procedure.In this work, several approaches were investigated for the transformation and utilization of CO2. In our investigation of hybrid catalysts, progress was made toward the synthesis of surface immobilized Ni(0) complexes for the use of CO2 in carboxylation of unsaturated hydrocarbons. The dicarbonyl Ni(0) complexes provided valuable insight into the effects of surface immobilization on this method of converting CO2 to industrially relevant products. Immobilization of Fe(III)-bipyridine catalysts was investigated for the oxidation of terminal olefins. Covalent attachment of these complexes to inert silica surfaces was investigated as a method to produce a robust and recyclable catalyst. Variation in the linker functional group was investigated as a method to tune product selectivity and improve conversion. The electronic effect of imine functionalization of Re(I)-bipyridine complexes on CO2 reduction was investigated. The stability of the complexes covalently attached to silica surfaces was investigated and the imine functionalization was observed to have interesting effects on the formation of deactivating species.A series of homogeneous Re(I) complexes were investigated for the photocatalytic reduction of CO2. An aliphatic imine derivatized bipyridine complex displayed interesting electrochemical properties. Expanding upon this structure, a series of thiocarbazide derivatives were investigated to promote hydrogen bonding interactions towards a dimeric reduction of CO2. Carbon nitride (C3N4) was investigated as a photosensitizer for these catalytic systems. Preliminary work towards the use of hydrogen bonding interactions and covalent attachment of complexes to C3N4 was performed to promote efficient electron transfer from photoexcited C3N4 surfaces to Re(I) catalysts.
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653 $a Carbon dioxide
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