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Photocathodes for Photochemical Cells, Exploring Charge Separation and Ultrafast Lasers.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Photocathodes for Photochemical Cells, Exploring Charge Separation and Ultrafast Lasers./
Author:	Hargenrader, George Nik.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2021,
Description:	178 p.
Notes:	Source: Dissertations Abstracts International, Volume: 83-06, Section: B.
Contained By:	Dissertations Abstracts International83-06B.
Subject:	Physical chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28927112
ISBN:	9798494427137

Photocathodes for Photochemical Cells, Exploring Charge Separation and Ultrafast Lasers.
Hargenrader, George Nik.

Photocathodes for Photochemical Cells, Exploring Charge Separation and Ultrafast Lasers. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 178 p.

Source: Dissertations Abstracts International, Volume: 83-06, Section: B.

Thesis (Ph.D.)--University of Illinois at Chicago, 2021.

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

Research efforts discussed in this thesis focus on strategies to effect photocatalytic reduction of CO2 to simple hydrocarbons, using solar radiation as the driving force.Chapter 1 consists of a brief introduction on the need to store solar energy as well as the associated challenges. The importance of CO2 reduction is presented and the current methodologies are reviewed.In Chapter 2, the construction of an ultrafast transient absorption pump probe spectrometer is presented. This instrument was used for all the studies presented in this thesis to probe photochemical processes that occur immediately after photon absorption; specifically, charge transfer and the non-productive relaxation pathways. Many of the technical challenges faced during the endeavor are discussed in detail.In Chapter 3, a light harvesting antenna constructed via self-assembly of graphene quantum dots into stacked disc nanowires is investigated. A pair of cobalt based hydrogen evolution catalysts were covalently attached to the monomer unit ("HBCPy") and the ability of the antenna to funnel excited state energy to the reaction site was evaluated. It was found that the HBCPy nanowires allowed excitons to sample 50 monomer units before relaxing, which is significant compared to similar systems. However, energy or electron transfer to the catalyst was not observed, likely due to the formation of non-productive energy pathways. This work gives insight for future improvements for the use of HBCPY as a light harvesting antenna.In Chapter 4, a strategy to photochemically regenerate an NAD+ analog is explored by covalently attaching the catalyst to the wide band gap p-type semiconductor NiO, which serves as an electron donor. The purpose is to address the fact that sequential reduction of CO2 to simple hydrocarbons have been hampered by the high energy intermediate singly reduced state CO2●¯. The strategy of reducing CO2 via a hydride donating catalyst based on NADH may provide a way to avoid this high energy intermediates. However, the strategy is only viable if the NADH analog acts as a true catalyst by being regenerated, as opposed to being consumed in stoichiometric amounts. This work highlights some of the mechanistic challenges associated with photo regeneration of hydride donors.In Chapter 5, a summary is provided of the research presented in this thesis. Future directions are highlighted to address the challenges discussed herein.

ISBN: 9798494427137Subjects--Topical Terms:

1981412
Physical chemistry.
Subjects--Index Terms:

Carbon dioxide reduction

Photocathodes for Photochemical Cells, Exploring Charge Separation and Ultrafast Lasers.
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506 $a This item must not be sold to any third party vendors.
520 $a Research efforts discussed in this thesis focus on strategies to effect photocatalytic reduction of CO2 to simple hydrocarbons, using solar radiation as the driving force.Chapter 1 consists of a brief introduction on the need to store solar energy as well as the associated challenges. The importance of CO2 reduction is presented and the current methodologies are reviewed.In Chapter 2, the construction of an ultrafast transient absorption pump probe spectrometer is presented. This instrument was used for all the studies presented in this thesis to probe photochemical processes that occur immediately after photon absorption; specifically, charge transfer and the non-productive relaxation pathways. Many of the technical challenges faced during the endeavor are discussed in detail.In Chapter 3, a light harvesting antenna constructed via self-assembly of graphene quantum dots into stacked disc nanowires is investigated. A pair of cobalt based hydrogen evolution catalysts were covalently attached to the monomer unit ("HBCPy") and the ability of the antenna to funnel excited state energy to the reaction site was evaluated. It was found that the HBCPy nanowires allowed excitons to sample 50 monomer units before relaxing, which is significant compared to similar systems. However, energy or electron transfer to the catalyst was not observed, likely due to the formation of non-productive energy pathways. This work gives insight for future improvements for the use of HBCPY as a light harvesting antenna.In Chapter 4, a strategy to photochemically regenerate an NAD+ analog is explored by covalently attaching the catalyst to the wide band gap p-type semiconductor NiO, which serves as an electron donor. The purpose is to address the fact that sequential reduction of CO2 to simple hydrocarbons have been hampered by the high energy intermediate singly reduced state CO2●¯. The strategy of reducing CO2 via a hydride donating catalyst based on NADH may provide a way to avoid this high energy intermediates. However, the strategy is only viable if the NADH analog acts as a true catalyst by being regenerated, as opposed to being consumed in stoichiometric amounts. This work highlights some of the mechanistic challenges associated with photo regeneration of hydride donors.In Chapter 5, a summary is provided of the research presented in this thesis. Future directions are highlighted to address the challenges discussed herein.
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