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020 ▼a 9781088322659
035 ▼a (MiAaPQ)AAI13904282
040 ▼a MiAaPQ ▼c MiAaPQ ▼d 247004
0820 ▼a 574
1001 ▼a Hall, Leah Margaret Graham.
24510 ▼a (Ga1-xZnx)(N1-xOx) Nanocrystals: Photochemical H2 Production and Spatial Characterization of Electronic Structure.
260 ▼a [S.l.]: ▼b University of Colorado at Boulder., ▼c 2019.
260 1 ▼a Ann Arbor: ▼b ProQuest Dissertations & Theses, ▼c 2019.
300 ▼a 131 p.
500 ▼a Source: Dissertations Abstracts International, Volume: 81-04, Section: B.
500 ▼a Advisor: Dukovic, Gordana.
5021 ▼a Thesis (Ph.D.)--University of Colorado at Boulder, 2019.
506 ▼a This item must not be sold to any third party vendors.
520 ▼a Solar fuel generation via artificial photosynthesis is a promising pathway to a clean and sustainable source of energy. Nanoscale (Ga1-xZnx)(N1-xOx) has been synthesized in the solid state in order to answer the call for new multinary semiconductors for use in solar fuel generation. Herein, the solid-state mechanism of (Ga1-xZnx)(N1-xOx) nanocrystal formation involving phase transformation of cubic spinel ZnGa2O4 to wurtzite (Ga1-xZnx)(N1-xOx) and diffusion of the elements combined with nitrogen incorporation will be discussed. Understanding how multinary semiconductor compounds function and drive multi-electron photochemical reactions is of the utmost importance for potentially using them in solar applications. One goal is to utilize (Ga1-xZnx)(N1-xOx) nanocrystals for solar photochemistry and understand why their efficiencies have been historically low. The use of (Ga1-xZnx)(N1-xOx) nanocrystals for photochemical H2 generation in an aqueous system with a redox mediator will be discussed. The four-part H2 generation system uses (Ga1-xZnx)(N1-xOx) nanocrystals as a light absorber, methyl viologen as an electron relay, Pt nanoparticles as a cocatalyst, and dithioerythritol as a sacrificial hole scavenger. Each charge-transfer step is studied in isolation in order to evaluate the factors that determine the overall photochemical efficiency. It is concluded that electron transfer from(Ga1-xZnx)(N1-xOx) to MV2+ is likely the most limiting step for the overall system. To date, little analysis has been done on the electronic structure of (Ga1-xZnx)(N1-xOx), particularly for samples with different elemental distributions. How the electronic structure changes when comparing homogeneous and heterogeneous (Ga1-xZnx)(N1-xOx) nanocrystals and how the electronic structure changes spatially throughout a single particle will be investigated. It is found that the heterogeneous (Ga1-xZnx)(N1-xOx) nanocrystals show two energy transitions, one in the UV region and one in the visible region, while the homogeneous particles only show a visible transition. Additionally, the shape of the energy loss spectrum stays constant throughout a particle indicating that the electronic structure is constant in a single particle.
590 ▼a School code: 0051.
650 4 ▼a Chemistry.
650 4 ▼a Nanoscience.
650 4 ▼a Materials science.
650 4 ▼a Biochemistry.
690 ▼a 0485
690 ▼a 0794
690 ▼a 0565
690 ▼a 0487
71020 ▼a University of Colorado at Boulder. ▼b Chemistry.
7730 ▼t Dissertations Abstracts International ▼g 81-04B.
773 ▼t Dissertation Abstract International
790 ▼a 0051
791 ▼a Ph.D.
792 ▼a 2019
793 ▼a English
85640 ▼u http://www.riss.kr/pdu/ddodLink.do?id=T15492530 ▼n KERIS ▼z 이 자료의 원문은 한국교육학술정보원에서 제공합니다.
980 ▼a 202002 ▼f 2020
990 ▼a ***1008102
991 ▼a E-BOOK