京都大学 / 0048 / 新制・課程博士 / 博士(エネルギー科学) / 甲第21887号 / エネ博第388号 / 新制||エネ||75(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー基礎科学専攻 / (主査)教授 齊藤 泰司, 教授 横峯 健彦, 准教授 伊藤 啓 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

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The pursuit of sustainable and high-performance materials is of utmost significance in driving the progress of battery technologies. Solid-state technology represents a promising avenue for the development of batteries with improved sustainability and performance. In this context, the present study delves into the examination of composition and the substitution of oxygen with nitrogen within the 50Li2O-xSiO2-(50-x)P2O5 glass system, specifically as applied to Solid-State electrolytes. The objective is to evaluate the influence of these factors on the electrical properties of the glass and their potential implications for Solid-State battery technology. The glass matrix was obtained through the melt-quenching technique, followed by comprehensive characterization using electrochemical impedance spectroscopy. The influence of varying silica content on the conductivity of the glass was investigated. This led to the selection of the glass system with the highest conductivity for further experiments involving nitridation. Subsequent experiments on nitridation aimed to explore the impact of nitrogen incorporation on the conductivity of the glass. By systematically varying the nitrogen content at different temperatures, the study sought to elucidate the relationship between nitrogen content and the resulting increase in glass conductivity.    The study reveals a noteworthy finding regarding the impact of nitrogen content on the conductivity of the glass. Specifically, when the nitrogen content was increased, the conductivity increased. In the case of a similar glass composition in pellet form, the conductivity at room temperature increased from Log σ = -8,009 (for glass without nitrogen) to Log σ = -6,951 (for nitrided glass). Additionally, the introduction of nitrogen into the glass resulted in a decrease in activation energy, being reduced from 0,66 eV (for oxide glass) to 0,60 eV (for oxynitride glass). These results indicate a clear correlation between increased nitrogen content and enhanced electrical properties of the investigated glasses; although obtaining a homogeneous bulk glass after nitridation was not feasible. Therefore, the nitrided samples were pelletized and sintered under different thermal conditions to obtain characterizable samples. The findings suggest that nitrogen substitution could be a promising approach for enhancing the electrical properties of the glasses of the title system of composition. Further investigation is required to optimize the process and achieve homogeneous bulk oxynitride glass.

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The objectives of this research were to 1) monitor in-situ moisture and diffusivity for both conventional concrete and concrete containing pre-wetted lightweight fine aggregate (LWFA), 2) compare deck performance in terms of early-age cracking, compressive strength, and chloride ingress, and 3) compare concrete properties in terms of compressive strength, chloride permeability, elastic modulus, and water content in the laboratory using cylinders cast in the field at the time of deck construction. The research involved field and laboratory evaluations of four newly constructed bridge decks located in northern Utah, two constructed using conventional concrete and two constructed using pre-wetted LWFA to promote internal curing. Data from sensors embedded in the concrete decks indicate that the moisture content of the internally cured concrete was consistently 1.5 to 4 percentage points higher than the moisture content of the conventional concrete for the first 6 months following deck construction. By 1 year, however, the internally cured concrete showed little difference in moisture content compared to the conventional concrete. While the internally cured concrete decks had a higher average moisture content, the electrical conductivity values were not consistently higher than those measured on the conventional concrete decks during the first approximately 8 to 10 months. However, after 8 to 10 months, both internally cured concrete decks exhibited higher electrical conductivity values than those measured on the conventional concrete decks. Laboratory compressive strength data indicate that, for the first 6 months following deck construction, the two concrete mixtures exhibited very similar strength gain characteristics. However, at 1 year, the conventional concrete was stronger by an average of 12.9 percent, or nearly 900 psi, than the internally cured concrete. In rapid chloride permeability testing, the internally cured concrete consistently passed between 13.1 and 17.5 percent less current than that passed by the conventional concrete. Laboratory free-free resonant testing at 1 year showed that the modulus of the internally cured concrete was 3.9 percent lower, on average, than that of the conventional concrete. For the tested specimens, the moisture content of the internally cured concrete was 0.5 percentage points higher, on average, than that of the conventional concrete. In the field, Schmidt rebound hammer testing showed that the internally cured concrete was neither consistently stronger nor weaker than the conventional concrete. On average, the internally cured concrete exhibited higher chloride concentrations than the conventional concrete. On average, the conventional concrete bridge decks had 4.6, 21.5, and 2.8 times more cracking than the internally cured concrete decks at 5 months, 8 months, and 1 year, respectively. At 1 year, very distinctive reflection cracks from the joints between the underlying pre-cast half-deck panels were observed on all of the decks.

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Two-dimensional conjugated metal−organic frameworks (2D c-MOFs) have emerged as a new class of crystalline layered conducting materials that hold significant promise for applications in electronics and spintronics. However, current 2D c- MOFs are mainly made from organic planar ligands, whereas layered 2D c-MOFs constructed by curved or twisted ligands featuring novel orbital structures and electronic states remain less developed. Herein, we report a Cu-catecholate wavy 2D c-MOF (Cu3(HFcHBC)2) based on a fluorinated core-twisted contorted hexahydroxy-hexa-cata-hexabenzocoronene (HFcHBC) ligand. We show that the resulting film is composed of rod-like single crystals with lengths up to ∼4 μm. The crystal structure is resolved by high-resolution transmission electron microscopy (HRTEM) and continuous rotation electron diffraction (cRED), indicating a wavy honeycomb lattice with AA-eclipsed stacking. Cu3(HFcHBC)2 is predicted to be metallic based on theoretical calculation, while the crystalline film sample with numerous grain boundaries apparently exhibits semiconducting behavior at the macroscopic scale, characterized by obvious thermally activated conductivity. Temperature-dependent electrical conductivity measurements on the isolated single-crystal devices indeed demonstrate the metallic nature of Cu3(HFcHBC)2, with a very weak thermally activated transport behavior and a room-temperature conductivity of 5.2 S cm−1. Furthermore, the 2D c-MOFs can be utilized as potential electrode materials for energy storage, which display decent capacity (163.3 F g−1) and excellent cyclability in an aqueous 5 M LiCl electrolyte. Our work demonstrates that wavy 2D c-MOF using contorted ligands are capable of intrinsic metallic transport, marking the emergence of new conductive MOFs for electronic and energy applications.

Yes / Archaeological research at Stonehenge (UK) is increasingly aimed at understanding the dynamic of the wider archaeological landscape. Through the application of state-of-the-art geophysical techniques, unprecedented insight is being gathered into the buried archaeological features of the area. However, applied survey techniques have rarely targeted natural soil variation, and the detailed knowledge of the palaeotopography is consequently less complete. In addition, metallic topsoil debris, scattered over different parts of the Stonehenge landscape, often impacts the interpretation of geophysical datasets. The research presented here demonstrates how a single multi-receiver electromagnetic induction (EMI) survey, conducted over a 22 ha area within the Stonehenge landscape, offers detailed insight into natural and anthropogenic soil variation at Stonehenge. The soil variations that were detected through recording the electrical and magnetic soil variability, shed light on the genesis of the landscape, and allow for a better definition of potential palaeoenvironmental and archaeological sampling locations. Based on the multi-layered dataset, a procedure was developed to remove the influence of topsoil metal from the survey data, which enabled a more straightforward identification of the detected archaeology. The results provide a robust basis for further geoarchaeological research, while potential to differentiate between modern soil disturbances and the underlying sub-surface variations can help in solving conservation and management issues. Through expanding this approach over the wider area, we aim at a fuller understanding of the human–landscape interactions that have shaped the Stonehenge landscape.

Halbleitermaterialien sind in den elektrischen Anwendungen der heutigen Zeit unerlässlich geworden. In dieser Arbeit wird der Fokus auf die Untersuchung der elektrischen und thermischen Eigenschaften von zwei Halbleiterklassen gelegt. Zum einen wird mit -Ga2O3 ein Mitglied der Klasse der transparenten leitfähigen Oxide untersucht.Hier wurden die elektrischen Eigenschaften von dünnen Schichten (Dicke von 28nm-225nm) und Volumenkristallen temperaturabhängig untersucht.Dabei zeigt sich bei Volumenkristallen und mindestens 150nm dicken Schichten eine Steigerung der elektrischen Leitfähigkeit bis 100K durch die Streuung von Elektronen an Störstellen und bei Temperaturen über 100K wieder ein Abfall der elektrischen Leitfähigkeit durch Elektron-Phonon-Wechselwirkung. Die Untersuchung der thermische Leitfähigkeit von beta-Ga2O3 zeigt ein anisotropes Verhalten mit minimalen Werten in [100]-Richtung und maximalen Werten in [010]-Richtung. Die Temperaturabhängigkeit der thermischen Eigenschaften zeigt eine Verringerung der thermischen Leitfähigkeit und der thermischen Diffusivität mit steigender Temperatur. Eine zweite untersuchte Materialklasse ist die der Kesterite. Zu dieser Kristallstruktur wurden zwei Elementkonfigurationen untersucht, Kupfer-Zink-Zinn-Sulfid und Kupfer- Zink-Zinn-Selenid. Der Transport bei Raumtemperatur und darunter findet über verschiedene Tunnelprozesse lokalisierter Ladungsträger statt. Zusätzlich wird auf die Veränderung der elektrischen Eigenschaften durch die Kristallinität und Komposition eingegangen. Die thermischen Eigenschaften zeigen analog zum beta-Ga2O3 eine Dominanz der Phonon-Phonon-Umklapp-Streuung bei hohen Temperaturen, während bei niedrigen Temperaturen Streuung an Störstellen und Grenzflächen vorherrscht. Methodisch zeigt diese Arbeit unterschiedlichste Messmethoden zur Charakterisierung der elektrischen und thermischen Eigenschaften, welche die Standardmethoden sowohl nutzen, als auch sinnvoll erweitern. / Semiconductors are essential for electronic applications nowadays. Here, the electrical and thermal properties of two semiconductor classes with huge application potential are investigated. As a transparent conducting oxide beta-Ga2O3 is investigated. In this work, the temperature dependent electrical properties were investigated for bulk materials and thin films. An increase in the electrical conductivity until 100K is found through electron-impurity-scattering and a decrease at higher temperatures through electron-phonon-scattering for for films with a thickness of at least 150nm. The investigation of the thermal properties of -Ga2O3 show an anisotropy for the different crystal orientations with minimal primary axis values for the [100]-direction and maximal values for the [010]-direction. The temperature-dependence of the thermal properties shows a decease in conductivity and diffusivity for increasing temperature. For temperatures over 150K phonon-phonon-Umklapp-scattering can explain the measured values. For low temperatures phonon-impurity scattering is most likely the dominant scattering mechanism. A second investigated material class are kesterites. For this crystal structure two configurations were investigated, copper-zinc-tin-sulfide and copper-zinc-tin-selenide. The electrical properties show semiconducting characteristics with p-type conduction. The transport processes are defined through localised thermal activated tunneling within the band gap. Other reductions of the mobility are found by the crystalinity and the composition of the materials. The thermal properties show dominant phonon-phonon- Umklapp-scattering at higher temperatures and phonon-impurity-scattering for lower temperatures in a similar way as in beta-Ga2O3. This work shows new implemented measurement methods for investigating electrical and thermal properties as extentions to common methods.