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- Genre: Doctoral Dissertation
Description
Nuclear magnetic resonance (NMR) is an important phenomenon involving nuclear magnetic moments in magnetic field, which can provide much information about a wide range of materials, including their chemical composition, chemical environments and nuclear spin interactions. The NMR spectrometer has been extensively developed and used in many areas of research. In this thesis, studies in two different areas using NMR are presented. First, a new kind of nanoparticle, Gd(DTPA) intercalated layered double hydroxide (LDH), has been successfully synthesized in the laboratory of Prof. Dey in SEMTE at ASU. In Chapter II, the NMR relaxation studies of two types of LDH (Mg, Al-LDH and Zn, Al-LDH) are presented and the results show that when they are intercalated with Gd(DTPA) they have a higher relaxivity than current commercial magnetic resonance imaging (MRI) contrast agents, such as DTPA in water solution. So this material may be useful as an MRI contrast agent. Several conditions were examined, such as nanoparticle size, pH and intercalation percentage, to determine the optimal relaxivity of this nanoparticle. Further NMR studies and simulations were conducted to provide an explanation for the high relaxivity. Second, fly ash is a kind of cementitious material, which has been of great interest because, when activated by an alkaline solution, it exhibits the capability for replacing ordinary Portland cement as a concrete binder. However, the reaction of activated fly ash is not fully understood. In chapter III, pore structure and NMR studies of activated fly ash using different activators, including NaOH and KOH (4M and 8M) and Na/K silicate, are presented. The pore structure, degree of order and proportion of different components in the reaction product were obtained, which reveal much about the reaction and makeup of the final product.
ContributorsPeng, Zihui (Author) / Marzke, Robert F (Thesis advisor) / Dey, Sandwip Kumar (Committee member) / Neithalath, Narayanan (Committee member) / Chamberlin, Ralph Vary (Committee member) / Mccartney, Martha Rogers (Committee member) / Arizona State University (Publisher)
Created2013
Description
In this work, a new method, "Nanobonding" [1,2] is conceived and researched to bond Si-based surfaces, via nucleation and growth of a 2 D silicon oxide SiOxHx interphase connecting the surfaces at the nanoscale across macroscopic domains. Nanobonding cross-bridges two smooth surfaces put into mechanical contact in an O2/H2O mixed ambient below T <200 °C via arrays of SiOxHx molecules connecting into a continuous macroscopic bonding interphase. Nano-scale surface planarization via wet chemical processing and new spin technology are compared via Tapping Mode Atomic Force Microscopy (TMAFM) , before and after nano-bonding. Nanobonding uses precursor phases, 2D nano-films of beta-cristobalite (beta-c) SiO2, nucleated on Si(100) via the Herbots-Atluri (H-A) method [1]. beta-c SiO2 on Si(100) is ordered and flat with atomic terraces over 20 nm wide, well above 2 nm found in native oxides. When contacted with SiO2 this ultra-smooth nanophase can nucleate and grow domains with cross-bridging molecular strands of hydroxylated SiOx, instead of point contacts. The high density of molecular bonds across extended terraces forms a strong bond between Si-based substrates, nano- bonding [2] the Si and silica. A new model of beta-cristobalite SiO2 with its <110> axis aligned along Si[100] direction is simulated via ab-initio methods in a nano-bonded stack with beta-c SiO2 in contact with amorphous SiO2 (a-SiO2), modelling cross-bridging molecular bonds between beta-c SiO2 on Si(100) and a-SiO2 as during nanobonding. Computed total energies are compared with those found for Si(100) and a-SiO2 and show that the presence of two lattice cells of !-c SiO2 on Si(100) and a-SiO2 lowers energy when compared to Si(100)/ a-SiO2 Shadow cone calculations on three models of beta-c SiO2 on Si(100) are compared with Ion Beam Analysis of H-A processed Si(100). Total surface energy measurements via 3 liquid contact angle analysis of Si(100) after H-A method processing are also compared. By combining nanobonding experiments, TMAFM results, surface energy data, and ab-initio calculations, an atomistic model is derived and nanobonding is optimized. [1] US Patent 6,613,677 (9/2/03), 7,851,365 (12/14/10), [2] Patent Filed: 4/30/09, 10/1/2011
ContributorsWhaley, Shawn D (Author) / Culbertson, Robert J. (Thesis advisor) / Herbots, Nicole (Committee member) / Rez, Peter (Committee member) / Marzke, Robert F (Committee member) / Lindsay, Stuart (Committee member) / Chamberlin, Ralph V (Committee member) / Arizona State University (Publisher)
Created2011