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Cobalt and nickel macrocycles anchor...

Achey, Darren Craig.

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Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association.

Record Type:	Language materials, printed : Monograph/item
Title/Author:	Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association./
Author:	Achey, Darren Craig.
Description:	213 p.
Notes:	Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.
Contained By:	Dissertation Abstracts International75-02B(E).
Subject:	Chemistry, Inorganic. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3574983
ISBN:	9781303523823

Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association.
Achey, Darren Craig.

Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association. - 213 p.

Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.

Thesis (Ph.D.)--The Johns Hopkins University, 2013.

The global demand for renewable, clean electricity and fuel has compelled efforts to utilize the immense power incident upon the Earth from the Sun. Photovoltaic systems could power the planet's electrical demands with only moderate efficiencies. However, mitigation of fossil fuels used for transportation and night-time electricity requires the storage of photon energy, for example, in the form of chemical bonds. Mesoporous, nanocrystalline TiO2 thin films provide a manifold for anchoring molecular species that absorb and utilize photons to catalyze fuel-generating reactions. The overarching theme of this thesis is to improve understanding of the semiconductor/molecule interface utilizing earth abundant first-row transition metal coordination compounds.

ISBN: 9781303523823Subjects--Topical Terms:

517253
Chemistry, Inorganic.

Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association.
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020 $a 9781303523823
035 $a (MiAaPQ)AAI3574983
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100 1 $a Achey, Darren Craig. $3 2094201
245 1 0 $a Cobalt and nickel macrocycles anchored to nanocrystalline titanium dioxide thin films: Sensitization, catalysis, and ligand association.
300 $a 213 p.
500 $a Source: Dissertation Abstracts International, Volume: 75-02(E), Section: B.
500 $a Adviser: Gerald J. Meyer.
502 $a Thesis (Ph.D.)--The Johns Hopkins University, 2013.
520 $a The global demand for renewable, clean electricity and fuel has compelled efforts to utilize the immense power incident upon the Earth from the Sun. Photovoltaic systems could power the planet's electrical demands with only moderate efficiencies. However, mitigation of fossil fuels used for transportation and night-time electricity requires the storage of photon energy, for example, in the form of chemical bonds. Mesoporous, nanocrystalline TiO2 thin films provide a manifold for anchoring molecular species that absorb and utilize photons to catalyze fuel-generating reactions. The overarching theme of this thesis is to improve understanding of the semiconductor/molecule interface utilizing earth abundant first-row transition metal coordination compounds.
520 $a Chapter 2 presents the non-ideal redox behavior of cobalt porphyrins anchored to semiconductor surfaces. Additionally, CoI porphyrins were utilized as photocatalysts for the 2e- reduction of organobromides to yield a CoIII-R intermediate. The cobalt-carbon bond of CoIII-R was photodissociated with visible light to yield Co II and R·. The organic radical dimerized to form R-R.
520 $a Light excitation of CoI compounds was found to result in electron transfer to TiO2, Chapter 3. Cobalt porphyrins, phthalocyanines, glyoximes, and corrins were all observed to exhibit this behavior. Electron transfer was demonstrated to primarily occur via excitation into the large extinction coefficient metal-to-ligand charge transfer absorption bands of CoI complexes.
520 $a Chapter 4 focuses on the unique coordination chemistry of cobalt porphyrins anchored to a TiO2 thin film. Notably, pyridine axially ligated a CoII porphyrin following excited-state electron transfer of the CoI porphyrin to the TiO2. The rate constant for recombination of an electron in the TiO2 with CoII was observed to decrease with increasing pyridine concentration, behavior attributed primarily to a negative shift of the CoII/I potential in the presence of pyridine.
520 $a Finally, Chapter 5 reports a comparative study of the kinetic and thermodynamic properties of the equilibrium between a 4-coordinate, low spin and a 6-coordinate, high spin nickel porphyrin, both in solution and anchored to TiO2. The mesoporous TiO2 thin film was found to influence the enthalpy and entropy of axial ligation while also altering the dissociative activation energy of axial ligation.
590 $a School code: 0098.
650 4 $a Chemistry, Inorganic. $3 517253
650 4 $a Chemistry, Physical. $3 560527
650 4 $a Engineering, Materials Science. $3 1017759
690 $a 0488
690 $a 0494
690 $a 0794
710 2 $a The Johns Hopkins University. $b Chemistry. $3 2094202
773 0 $t Dissertation Abstracts International $g 75-02B(E).
790 $a 0098
791 $a Ph.D.
792 $a 2013
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3574983