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Quantum-Mechanical Investigations of...

Suleiman, Olabisi M.

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Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites./
作者:	Suleiman, Olabisi M.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2023,
面頁冊數:	179 p.
附註:	Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
Contained By:	Dissertations Abstracts International85-01B.
標題:	Chemistry. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30490410
ISBN:	9798379769130

Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites.
Suleiman, Olabisi M.

Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites. - Ann Arbor : ProQuest Dissertations & Theses, 2023 - 179 p.

Source: Dissertations Abstracts International, Volume: 85-01, Section: B.

Thesis (Ph.D.)--University of Nevada, Reno, 2023.

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

Over the years, there has been significant interest in the conversion of methane to methanol. This has been due to the abundant nature of natural gas which is composed mainly of methane. In order to prevent over-oxidation of CO2, CO, and HCOOH, it has been demonstrated that copper-exchanged zeolites can kinetically trap activated methane as strongly bound methoxy groups. We describe the process by which over oxidation products are produced in great detail. We have investigated the impact of heterometallic extra-framework motifs on the temperature gradients of each step. We also discuss quantum-mechanical computations of activated copper-exchanged zeolites; realizing how these systems have evolved at the molecular level will open up possibilities for enhancing reactivity.Here, we used quantum-mechanical methods to study dipyrrinones. These are nonfluorescent yellow-pigmented components of bilirubin, when excited with UV/blue light experiences Z to E isomerization and produce highly fluorescent compounds like N,N-methylene-bridged dipyrrinones and xanthoglows. The first instances of dipyrrinone analogues with fluorescence without covalently bonding the nitrogen atoms of the pyrole and pyrrolidine are described in this thesis.{A0}We also considered the possibility of using quantum-mechanical calculations to develop the brightest series of pyronin fluorophores. Typically, pyronin Y and B (PY and PB, respectively) are used in staining applications. However, these dyes have low fluorophore brightness, we developed the brightest series of pyronin fluorophores ever reported, these systems outperform both pyronin Y and B through a combination of experimental and theoretical work (PY and PB). The pyronins have a low fluorophore brightness, though, and there is not a clear process in the literature for creating enhanced variants. The best agreement for this group of systems is obtained using DFT functionals with an exact Hartree-Fock exchange of 0-10%. The intensities of the pyronin fluorophores are determined by TD-DFT calculations of interconversion barriers and energies between{A0}structures on the lowest excited singlet (S1) surface and twisted intermolecular charge transfer (TICT) states.Lastly, as a capstone to this thesis, we developed a new double hybrid density functional approximation (DH-DFA), {CF}{89}B88PTPSS, which incorporates the equipartition of density functional theory (DFT) and non-local correlation but with a meta-GGA correlation functional as well as the range-separated exchange of {CF}{89}B2PLYP. The new density functional provides accurate excitation energies for conventional systems as well as correct prescription of negative singlet-triplet gaps for non-conventional systems with inverted gaps (INVEST). {CF}{89}B88PTPSS performs quite well than recent DH-DFAs for open-shell systems, it correctly and accurately predicts negative gaps for 50 systems with inverted singlet-triplet gaps, for intramolecular charge-transfer excitations, in which its performance was achieved near-CC2 and ADC(2) quality for the QUESTDB set and also relative to EOM-CCSD reference.

ISBN: 9798379769130Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Methanol

Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites.
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245 1 0 $a Quantum-Mechanical Investigations of Excited State and Catalytic Properties of Organic Luminophores and Zeolites.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2023
300 $a 179 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
500 $a Advisor: Odoh, Samuel O.
502 $a Thesis (Ph.D.)--University of Nevada, Reno, 2023.
506 $a This item must not be sold to any third party vendors.
520 $a Over the years, there has been significant interest in the conversion of methane to methanol. This has been due to the abundant nature of natural gas which is composed mainly of methane. In order to prevent over-oxidation of CO2, CO, and HCOOH, it has been demonstrated that copper-exchanged zeolites can kinetically trap activated methane as strongly bound methoxy groups. We describe the process by which over oxidation products are produced in great detail. We have investigated the impact of heterometallic extra-framework motifs on the temperature gradients of each step. We also discuss quantum-mechanical computations of activated copper-exchanged zeolites; realizing how these systems have evolved at the molecular level will open up possibilities for enhancing reactivity.Here, we used quantum-mechanical methods to study dipyrrinones. These are nonfluorescent yellow-pigmented components of bilirubin, when excited with UV/blue light experiences Z to E isomerization and produce highly fluorescent compounds like N,N-methylene-bridged dipyrrinones and xanthoglows. The first instances of dipyrrinone analogues with fluorescence without covalently bonding the nitrogen atoms of the pyrole and pyrrolidine are described in this thesis.{A0}We also considered the possibility of using quantum-mechanical calculations to develop the brightest series of pyronin fluorophores. Typically, pyronin Y and B (PY and PB, respectively) are used in staining applications. However, these dyes have low fluorophore brightness, we developed the brightest series of pyronin fluorophores ever reported, these systems outperform both pyronin Y and B through a combination of experimental and theoretical work (PY and PB). The pyronins have a low fluorophore brightness, though, and there is not a clear process in the literature for creating enhanced variants. The best agreement for this group of systems is obtained using DFT functionals with an exact Hartree-Fock exchange of 0-10%. The intensities of the pyronin fluorophores are determined by TD-DFT calculations of interconversion barriers and energies between{A0}structures on the lowest excited singlet (S1) surface and twisted intermolecular charge transfer (TICT) states.Lastly, as a capstone to this thesis, we developed a new double hybrid density functional approximation (DH-DFA), {CF}{89}B88PTPSS, which incorporates the equipartition of density functional theory (DFT) and non-local correlation but with a meta-GGA correlation functional as well as the range-separated exchange of {CF}{89}B2PLYP. The new density functional provides accurate excitation energies for conventional systems as well as correct prescription of negative singlet-triplet gaps for non-conventional systems with inverted gaps (INVEST). {CF}{89}B88PTPSS performs quite well than recent DH-DFAs for open-shell systems, it correctly and accurately predicts negative gaps for 50 systems with inverted singlet-triplet gaps, for intramolecular charge-transfer excitations, in which its performance was achieved near-CC2 and ADC(2) quality for the QUESTDB set and also relative to EOM-CCSD reference.
590 $a School code: 0139.
650 4 $a Chemistry. $3 516420
650 4 $a Physical chemistry. $3 1981412
650 4 $a Organic chemistry. $3 523952
653 $a Methanol
653 $a Density functional theory
653 $a Xanthoglows
653 $a Dipyrrinone
653 $a Zeolites
690 $a 0485
690 $a 0490
690 $a 0494
710 2 $a University of Nevada, Reno. $b Chemistry. $3 1030667
773 0 $t Dissertations Abstracts International $g 85-01B.
790 $a 0139
791 $a Ph.D.
792 $a 2023
793 $a English
856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30490410