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Reactivity of Tetraborylmethanes and Electronic Structure Calculations of Dimensionally Reduced Materials
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| 자료유형 | 학위논문 |
|---|---|
| 서명/저자사항 | Reactivity of Tetraborylmethanes and Electronic Structure Calculations of Dimensionally Reduced Materials. |
| 개인저자 | Baum, Zachary John. |
| 단체저자명 | The Ohio State University. Chemistry. |
| 발행사항 | [S.l.]: The Ohio State University., 2018. |
| 발행사항 | Ann Arbor: ProQuest Dissertations & Theses, 2018. |
| 형태사항 | 241 p. |
| 기본자료 저록 | Dissertations Abstracts International 81-05B. Dissertation Abstract International |
| ISBN | 9781687936509 |
| 학위논문주기 | Thesis (Ph.D.)--The Ohio State University, 2018. |
| 일반주기 |
Source: Dissertations Abstracts International, Volume: 81-05, Section: B.
Advisor: Goldberger, Joshua. |
| 이용제한사항 | This item must not be sold to any third party vendors. |
| 요약 | The combined use of organic and inorganic precursors enables the discovery of new hybrid organic-inorganic materials as well as the development of improved synthetic routes to conventional solids. Herein, we present three major directions: the application of tetraborylmethanes as organometallic single-C synthons for carbon-metal bond formation in carbides, the synthesis and theoretical study of low-dimensional early transition metal dichalcogenide derivatives, and a separate study on the development of a new layered exfoliatable Zintl phase. In Chapter 2, we present the stepwise deborylation-homologation of C(Bpg)4 (pg = 1,3-propanediolate) with trimethylsilyl and trimethylgermyl groups as organometallic models for the initial carbon-metal bond formation in SiC and GeC. We demonstrate that 2 substitutions with these tertiary substituents proceed readily, and that the disubstituted derivatives are recalcitrant towards further homologation. In Chapter 3, we explore various strategies to utilize tetraborylmethanes as a carbido source with the intent to form solid state metal carbide materials at low temperatures. We present the thermal co-decomposition of C(Bpg)4 with Si(IV) and Nb(V) sources, which ultimately formed intimate SiO2:B2O3/C and Nb2O5/C mixtures. We also discuss the synthesis of a single-source Si-C precursor molecule, SiCl3C(Bpg)3, and its chemistry with activating bases and hydride sources. In Chapter 4, we present the rational synthesis, characterization, and electronic structure of 1D- TiS2 derivatives TiS2(en) (en = ethylenediamine) and TiS2(pn) (pn = 1,3-propylenediamine), which feature direct band gaps attractive for near-IR optoelectronics. Additionally, we discuss the synthesis of [V7S8Cl2(en)8]Cl4 (en = ethylenediamine), the first early transition metal chalcogenide dicubane, and DFT calculations explaining its observed magnetic behavior. In Chapter 5, we present the synthesis, electronic structure calculations, and exfoliation studies of the layered Zintl phase EuSn2As2. This anisotropic pseudo-2D material features anti-ferromagnetic coupling out-of-plane and ferromagnetic coupling in-plane. Overall, the work presented herein builds on our understanding of polyborylmethane chemistry as well as the rational synthesis and properties of low- dimensional metal-organic solids, and motivates further exploration of 2D Sn-containing lattices for the discovery of novel magnetic phenomena. |
| 일반주제명 | Chemistry. Physical chemistry. |
| 언어 | 영어 |
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