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Characterization of carbon materials by TPD methodLin, Tzu-yi 05 September 2006 (has links)
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Characterization of Carbon Black Surface by TPD MethodTsai, Chi-Ta 06 July 2003 (has links)
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Synthesis and Quantification of Surface Reactivity on CsSnBr3 and Cs2TiBr6Gao, Weiran 13 July 2018 (has links)
We quantified the chemical species present at polycrystalline cesium tin bromide perovskite, CsSnBr3 and cesium titanium bromide antifluorite, Cs2TiBr6. For CsSnBr3, experiments utilized the orthogonal reactivity of the Cs+ cation, the Sn2+ cation, and the Br– halide anion. Ambient- pressure exposure to BF3 solutions probed the reactivity of interfacial bromines. Reactions with p-trifluoromethylanilinium chloride probed the exchange reactivity of the Cs+ cation. A complex-forming ligand, 4,4’-bis(trifluoromethyl)-2,2’-bipyridine, probed for interfacial Sn2+- site cations. For Cs2TiBr6, both BF3 and (C6F5)3B probed the reactivity of interfacial bromines. Fluorine features in x-ray photoelectron spectroscopy (XPS) quantified reaction outcomes for each solution-phase species. XPS indicated adsorption of BF3 on CsSnBr3 and (C6F5)3B on Cs2TiBr6 indicating surface-available halide anions on both surfaces. For CsSnBr3, temperature- programmed desorption (TPD) quantified a ~215 kJ mol–1 desorption energy of BF3 on the surface. Adsorption of the fluorinated anilinium cation included no concomitant adsorption of chlorine as revealed by the absence of Cl 2p features within the limits of XPS detection. The bipyridine ligand demonstrated adsorption to CsSnBr3. We discuss the present results in the context of interfacial stability, passivation, and reactivity for solar-energy conversion devices.
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Synthesis and Quantification of Surface Reactivity on CsSnBr3 and Cs2TiBr6Gao, Weiran 13 July 2018 (has links)
We quantified the chemical species present at polycrystalline cesium tin bromide perovskite, CsSnBr3 and cesium titanium bromide antifluorite, Cs2TiBr6. For CsSnBr3, experiments utilized the orthogonal reactivity of the Cs+ cation, the Sn2+ cation, and the Br– halide anion. Ambient- pressure exposure to BF3 solutions probed the reactivity of interfacial bromines. Reactions with p-trifluoromethylanilinium chloride probed the exchange reactivity of the Cs+ cation. A complex-forming ligand, 4,4’-bis(trifluoromethyl)-2,2’-bipyridine, probed for interfacial Sn2+- site cations. For Cs2TiBr6, both BF3 and (C6F5)3B probed the reactivity of interfacial bromines. Fluorine features in x-ray photoelectron spectroscopy (XPS) quantified reaction outcomes for each solution-phase species. XPS indicated adsorption of BF3 on CsSnBr3 and (C6F5)3B on Cs2TiBr6 indicating surface-available halide anions on both surfaces. For CsSnBr3, temperature- programmed desorption (TPD) quantified a ~215 kJ mol–1 desorption energy of BF3 on the surface. Adsorption of the fluorinated anilinium cation included no concomitant adsorption of chlorine as revealed by the absence of Cl 2p features within the limits of XPS detection. The bipyridine ligand demonstrated adsorption to CsSnBr3. We discuss the present results in the context of interfacial stability, passivation, and reactivity for solar-energy conversion devices.
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Surface Chemistry of CF3I on Cu(111): C-F Activation, Carbene Insertion, £]-Elimination, and Copper Etching ReactionsChiu, Wen-Yi 24 July 2002 (has links)
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Surface Characterization and Reactivity of Methylammionium Lead IodideZielinski, Kenneth M 22 October 2018 (has links)
We quantify the chemical species present at and reactivity of the tetragonal (100) face of single-crystal methylammonium lead iodide, MAPbI3(100). MAPbI3 is an ABX3 perovskite, experiments utilized the orthogonal reactivity of the A+-site cation, the B2+-site cation, and the X–-site halide anion. Ambient-pressure exposure to BF3 solutions probe the reactivity of interfacial halides. Reactions with p-trifluoromethylanilinium chloride probe the exchange reactivity of the A+-site cation. The ligand 4,4’-bis(trifluoromethyl)-2,2’-bipyridine probe for interfacial B2+-site cations. Fluorine features in x-ray photoelectron spectroscopy (XPS) quantify reaction extents with each solution-phase species. XP spectra reveals adsorption of BF3 indicating surface-available halide anions on tetragonal MAPbI3(100) and preliminary examinations on the (112), (110), and thin-film surfaces. Temperature-programmed desorption (TPD) established a ~200 kJ mol–1 desorption activation energy from tetragonal MAPbI3(100). Adsorption of the fluorinated anilinium cation includes no concomitant adsorption of chlorine as revealed by the absence of Cl 2p features within the limits of XPS detection on the tetragonal (100) and (112) faces with no discernable exchange in preliminary experiments on tetragonal (110). Within detection limits, bipyridine ligand demonstrate no adsorption to tetragonal MAPbI3(100) or (112), while it does demonstrate significant adsorption on the (110) in preliminary experiments. We discuss the present results in the context of interfacial stability, passivation, and reactivity for perovskite-based energy conversion materials and some preliminary investigations into bilayer graphene-based dye sensitized photovoltaic materials.
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Oxidation of Co Nanoparticles grown on the linear stripes of oxides of NiAl(100)Chen, Jian-wei 30 July 2007 (has links)
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Characterization of Carbon Black Surface Energy by IGC/TPD Method.Chen, Ke-Cheng 16 July 2002 (has links)
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Surface Chemistry of Difluorovinylidene Species on Cu(111)Lee, Kang-ning 25 July 2008 (has links)
We investigated the reactivity of difluorovinylidene groups (C2F2) on Cu(111) under ultrahigh vacuum conditions. Difluorovinylidene moieties bonded to surface were generated by the dissociative adsorption of 1,1-dibromodifluoroethylene. Temperature Programmed desorption (TPD) and reflection-adsorption infrared spectroscopy (RAIRS) revealed the thermal reaction pathways, and a variety of intermediates were identified or inferred. The major desorption product, hexafluoro-2-butyne (C4F6), was detected at 445 K. It invokes a step of fluoride addition to difluorovinylidene to render the intermediacy of C2F3. However, differences exist when the vibration data from F + C=CF2 were compared with those from C−CF3 and CF=CF2 in previous literature, implying that the form is neither ethylidyne nor vinyl. Based on the concept of fluorine hyperconjugation, density function theory (DFT) calculations were utilized to obtain two transition states, quasi-vinyl and -ethylidyne, which can account for the differences present in the IR spectra. The relative thermal stability follows the trend of vinyl > quasi-ethylidyne > quasi-vinyl > vinylidene > ethylidyne suggested by IR and DFT calculations. Finally, the end product, CF3C¡ÝCCF3, might be formed by coupling of two quasi-ethylidyne species via the partial allenic forms.
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Catalysis research using model catalystsYan, Ting, active 2013 06 November 2013 (has links)
Catalysts are essential for technological advances, because of their indispensable role in chemical and material manufacturing, energy conversion, and pollution control systems. Developing better catalysts is a highly desired goal that is impeded by the complexity of heterogeneous catalysts. This makes it extremely difficult to obtain information regarding active sites and reaction mechanisms, which is critical for improving catalyst design and performance. My research work has led to the understanding of how specific catalytic surface sites affect the performance of catalysts by constructing conceptually simpler planar model catalysts for kinetics and mechanism studies using model surface science tools and batch reaction testing. The work in this dissertation has demonstrated that planar model catalysts are versatile tools to probe reaction mechanisms on industrial catalysts. Supported gold nanoparticles have shown remarkable catalytic activity in a variety of reactions. However, many fundamental aspects of gold catalysts are still unclear, especially about the identity of active sites and oxidizing species. A Au(111) single crystal, the most stable and abundant facet on gold nanoparticles, is utilized to understand the reaction mechanisms of partial oxidation of 2-butanol and allyl alcohol. By controlling oxygen coverage on the surface, 100% selectivity to corresponding ketone and aldehyde, the desirable products, can be achieved. Two model catalysis systems, gold nanoclusters supported on a TiO₂(110) substrate and iron oxide dispersed on a Au(111) surface, were employed to understand the reaction pathways of CO oxidation and probe the role of the oxide/metal interface. The mechanistic and kinetic studies have shown that planar model catalysts are useful tools to probe reactions on industrial catalysts. The mechanistic understanding obtained from model catalyst studies can be used to create better catalysts. / text
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