The introduction of artificial illumination has brought extensive benefits to mankind, and during the last years we have seen a tremendous progress in this field with the introduction of the energy-efficient light-emitting diode (LED) and the high-contrast organic LED display. These high-end technologies are, however, produced using costly and complex processes, and it is anticipated that the next big thing in the field will be the advent of a low-cost and “green” illumination technology, which can be fabricated in a cost- and material-efficient manner using non-toxic and abundant raw materials, and which features attractive form factors such as flexibility, robustness and light-weight. The light-emitting electrochemical cell (LEC) is a newly invented illumination technology, and in this thesis we present results that imply that it can turn the above vision into reality. The thin-film LEC comprises an active material sandwiched between a cathode and an anode as its key constituent parts. With the aid of a handheld air-brush, we show that functional large-area LECs can be fabricated by simply spraying three layers of solution -- forming the anode, active material, and cathode -- on top of a substrate. We also demonstrate that such “spray-sintered” LECs can feature multicolored emission patterns, and be fabricated directly on complex-shaped surfaces, with one notable example being the realization of a light-emission fork! Almost all LECs up-to-date have been fabricated on glass substrates, but for a flexible and light-weight emissive device, it is obviously relevant to identify more appropriate substrate materials. For this end, we show that it is possible to spray-coat the entire LEC directly on conventional copy paper, and that such paper-LECs feature uniform light-emission even under heavy bending and flexing. We have further looked into the fundamental aspects of the LEC operation and demonstrated that the in-situ doping formation, which is a characteristic and heralded feature of LECs, can bring problems in the form of doping-induced self-absorption. By quantitatively analyzing this phenomenon, we provided straightforward guidelines on how future efficiency-optimized LEC devices should be designed. The in-situ doping formation process brings the important advantage that LECs can be fabricated from solely air-stabile materials, but during light emission the device needs to be protected from the ambient air. We have therefore developed a functional glass/epoxy encapsulation procedure for the attainment of LEC devices that feature a record-long ambient-air operational lifetime of 5600 h. For the light-emission device of the future, it is however critical that the encapsulation is flexible, and in our last study, we show that the use of multi-layer barrier can result in high-performance flexible LECs.

京都大学 / 0048 / 新制・課程博士 / 博士(地球環境学) / 甲第18704号 / 地環博第127号 / 新制||地環||26(附属図書館) / 31637 / 京都大学大学院地球環境学舎地球環境学専攻 / (主査)教授 梶井 克純, 教授 杉山 雅人, 准教授 清中 茂樹 / 学位規則第4条第1項該当 / Doctor of Global Environmental Studies / Kyoto University / DFAM

No description available.

Ambient air pollution has been associated with restricted fetal growth, which is linked with adverse respiratory health in childhood. We assessed the effect of maternal exposure to low concentrations of ambient air pollution on birthweight. We pooled data from 14 population-based mother-child cohort studies in 12 European countries. Overall, the study population included 74-178 women who had singleton deliveries between Feb 11, 1994, and June 2, 2011, and for whom information about infant birthweight, gestational age, and sex was available. The primary outcome of interest was low birthweight at term (weight <2500 g at birth after 37 weeks of gestation). Mean concentrations of particulate matter with an aerodynamic diameter of less than 2·5 μm (PM2·5), less than 10 μm (PM10), and between 2·5 μm and 10 μm during pregnancy were estimated at maternal home addresses with temporally adjusted land-use regression models, as was PM2·5 absorbance and concentrations of nitrogen dioxide (NO2) and nitrogen oxides. We also investigated traffic density on the nearest road and total traffic load. We calculated pooled effect estimates with random-effects models. A 5 μg/m3 increase in concentration of PM2·5 during pregnancy was associated with an increased risk of low birthweight at term (adjusted odds ratio [OR] 1·18, 95% CI 1·06-1·33). An increased risk was also recorded for pregnancy concentrations lower than the present European Union annual PM2·5 limit of 25 μg/m3 (OR for 5 μg/m3 increase in participants exposed to concentrations of less than 20 μg/m3 1·41, 95% CI 1·20-1·65). PM10 (OR for 10 μg/m3 increase 1·16, 95% CI 1·00-1·35), NO2 (OR for 10 μg/m3 increase 1·09, 1·00-1·19), and traffic density on nearest street (OR for increase of 5000 vehicles per day 1·06, 1·01-1·11) were also associated with increased risk of low birthweight at term. The population attributable risk estimated for a reduction in PM2·5 concentration to 10 μg/m3 during pregnancy corresponded to a decrease of 22% (95% CI 8-33%) in cases of low birthweight at term. Exposure to ambient air pollutants and traffic during pregnancy is associated with restricted fetal growth. A substantial proportion of cases of low birthweight at term could be prevented in Europe if urban air pollution was reduced. / The European Union

Solar energy as the most abundant source of energy is clean, non-pollutant, and completely renewable, which provides energy security, independence, and reliability. Organic-inorganic hybrid perovskite solar cells (PSCs) revolutionized the photovoltaics field not only by showing high efficiency of above 22% in just a few years but also by providing cheap and facile fabrication methods. In this dissertation, fabrication of PSCs in both ambient air conditions and environmentally controlled N2-filled glove-box are studied. Several characterization methods such as SEM, XRD, EDS, Profilometry, four-point probe measurement, EQE, and current-voltage measurements were employed to examine the quality of thin films and the performance of the PSCs. A few issues with the use of equipment for the fabrication of thin films are addressed, and the solutions are provided. It is suggested to fabricate PSCs in ambient air conditions entirely, to reduce the production cost. So, in this part, the preparation of the solutions, the fabrication of thin films, and the storage of materials were performed in ambient air conditions regardless of their humidity sensitivity. Thus, for the first part, the fabrication of PSCs in ambient air conditions with relative humidity above ~36% with and without moisture sensitive material, i.e., Li-TFSI are provided. Perovskite materials including MAPbI3 and mixed cation MAyFA(1-y)PbIxBr(1-x) compositions are investigated. Many solution-process parameters such as the spin-coating speed for deposition of the hole transporting layer (HTL), preparation of the HTL solution, impact of air and light on the HTL conductivity, and the effect of repetitive measurement of PSCs are investigated. The results show that the higher spin speed of PbI2 is critical for high-quality PbI2 film formation. The author also found that exposure of samples to air and light are both crucial for fabrication of solar cells with larger current density and better fill factor. The aging characteristics of the PSCs in air and vacuum environments are also investigated. Each performance parameter of air-stored samples shows a drastic change compared with that of the vacuum-stored samples, and both moisture and oxygen in air are found to influence the PSCs performances. These results are essential towards the fabrication of low-cost, high-efficiency PSCs in ambient air conditions. In the second part, the research is focused on the fabrication of high-efficiency PSCs using the glove-box. Both single-step and two-step spin-coating methods with perovskite precursors such as MAyFA(1-y)PbIxBr(1-x) and Cesium-doped mixed cation perovskite with a final formula of Cs0.07MA0.1581FA0.7719Pb1I2.49Br0.51 were considered. The effect of several materials and process parameters on the performance of PSCs are investigated. A new solution which consists of titanium dioxide (TiO2), hydrochloric acid (HCl), and anhydrous ethanol is introduced and optimized for fabrication of quick, pinhole-free, and efficient hole-blocking layer using the spin-coating method. Highly reproducible PSCs with an average power conversion efficiency (PCE) of 15.4% are fabricated using this solution by spin-coating method compared to the conventional solution utilizing both spin-coating with an average PCE of 10.6% and spray pyrolysis with an average PCE of 13.78%. Moreover, a thin layer of silver is introduced as an interlayer between the HTL and the back contact. Interestingly, it improved the current density and, finally the PCEs of devices by improving the adhesion of the back electrode onto the organic HTL and increasing the light reflection in the PSC. Finally, a highly reproducible fabrication procedure for cesium-doped PSCs using the anti-solvent method with an average PCE of 16.5%, and a maximum PCE of ~17.5% is provided.

The research focuses on the environmental problem of volatile organic compounds in ambient air of petrol filling stations. The literature review of the issues, arising from petrol-related VOCs, with actual and proposed VOC emissions trends in Europe, have been performed. Besides petrol filling station’s typical technology layout, petrol nature and composition, applicable petrol vapour recovery solutions and their efficiency were examinated. The volatile organic compounds’ experimental research in two petrol stations of typical technology layout in Vilnius city under similar extreme meteorological conditions (VOC air pollution episodes with low winds, stable stratification and suspended photochemical removal) is done. The emitted from petrol stations VOC experiment is based on air pumped sampling in glass gas pipette and further determination using gas chromatography with flame ionization detector. The experimental results, presented by means of tables and diagrams, are analysed and discussed. The available results of the experiment are loaded into the environmental model “ALOHA” for air pollution evaluation and concentrations prediction in the ambient air under different meteorological conditions and technological emergency situations (petrol spillage) at petrol filling station. The research is summarized in conclusions and recommendations. / Tyrimas skirtas aplinkos oro taršos problemai lakiaisiais organiniais junginiais, išsiskiriančiais nuo benzino degalinių. Atlikta svarstomos aplinkosauginės problemos literatūros apžvalga. Apžvelgti oro taršos pasekmės skatinamos LOJ išsiskyrimų nuo benzino degalinių, aktualios ir numatomos LOJ emisijų tendencijos Europoje, tipinis benzino degalinės technologijos išsidėstymas, benzino sudėtis ir svarbiausios LOJ garų formavimui benzino savybės, taikomi garų grąžinimo sprendiniai ir jų efektyvumas. Detaliai aprašytas LOJ eksperimentinis tyrimas, atliktas dviejose Vilniaus miesto tipinės technologijos degalinėse esant panašioms kraštutinėms (LOJ taršos epizodai prie silpnų vėjų, stabilios stratifikacijos ir suspenduoto fotocheminio šalinimo) meteorologiniams sąlygoms. LOJ mėginių ėmimui panaudotas aktyvus metodas su aspiracija į dujines pipetes, LOJ koncentracijos nustatytos dujinės chromatografijos su liepsnos jonizacijos detektoriumi metodu. Tyrimo rezultatai, pateikti lentelių ir diagramų pavidalu, aptarti ir įvertinti. Eksperimento duomenys įkelti į oro kokybės modelį “ALOHA”, siekiant nustatyti LOJ pernašą ir sudaryti LOJ koncentracijų prognozė benzino degalinių aplinkos ore prie skirtingų meteorologinių parametrų ir avarinių technologinių situacijų (benzino išsiliejimas). Tiriamąjį darbą reziumuoja išvados ir rekomendacijos.

This diploma thesis deals with a plasmochemical treatment of photoanodes with an active layer containing TiO2 deposited on two different substrates by material printing. The plasmochemical treatment was performed by a low-temperature ambient-air plasma using a diffuse coplanar surface barrier discharge (DCSBD). The experimental part is focused on the investigation of DCSBD influence on the fabricated photoanodes photoelectrochemical properties, and the influence of plasma treatment time. Process optimization was achieved by height adjustment of the electrode. The processed coatings were electrochemically investigated by linear sweep voltammetry and chronoamperometry.

Transport, whose intensity year by year increase, has assuredly influence on air quality. This issue solution will be focused especially on localities burden with transport in urban areas. The contribution of transport to increased values of air pollution will be evaluated with regards to meteorological conditions. Background stations from Czech Hydrometeorological Institute categorization will be chosen such as comparative sites. Pollutants emitted from traffic such as particulate matter, nitrogen oxides and carbon monoxide will be observed except meteorological conditions.

La grossesse est une période sensible et déterminante pour le développement de l’enfant et l’état de santé à l’âge adulte. L'adaptation biologique et physiologique de l'organisme face à des « stresseurs » physiques et psychosociaux au cours de cette période peut ainsi exercer ses effets à l'âge adulte (et possiblement sur plusieurs générations). Cette toxicité différée suppose intrinsèquement la nécessité d’étudier les conséquences des expositions environnementales au cours de la vie foetale et ce suivant une approche holistique intégrant autant les facteurs de risque à des niveaux micro (caractéristiques individuelles) et macro (expositions physiques externes et contexte psycho-social). Etant donné l’hétérogénéité du territoire breton dans lequel s’inscrit ce travail de thèse, nous avons cherché à explorer l’impact des inégalités sociales et de l’environnement physique (pollution atmosphérique) sur l’issue de la grossesse (croissance foetale et risque de prématurité) indépendamment chez des femmes enceintes résidant dans des zones urbaines et rurales. Ce travail s’est appuyé sur les données issues de la cohorte bretonne mère-enfant PELAGIE, qui a inclus 3421 femmes enceintes entre 2002- 2006. Les paramètres anthropométriques et l’âge gestationnel à la naissance ont été renseignés à l’accouchement par le personnel médical. Le contexte urbain et rural breton a été caractérisé à partir de la définition des unités urbaines de l’INSEE. Les concentrations annuelles de pollution atmosphérique (dioxyde d’azote (NO2)) ont été modélisées à une échelle de 100 m à partir d’un modèle de "land-use regression" développé à l’échelle européenne. Enfin, le niveau socio-économique des IRIS a été estimé à l’aide d’un indice de désavantage social - construit à partir des données du recensement de l’INSEE et dont la validité et l’adaptabilité à des territoires à la fois urbains et ruraux a été examinée au préalable. Nos résultats suggèrent une influence délétère d’un contexte de vie socioéconomique défavorable sur la croissance intra-utérine, spécifiquement chez les femmes résidant en milieu rural. Nous avons également observé une augmentation du risque de prématurité associée à des niveaux > 16.4 μg.m-3 de NO2 dans l’air, à l’inverse, uniquement chez les femmes résidant dans des zones urbaines. Les associations entre l’exposition à la pollution atmosphérique et les marqueurs de la croissance intra-utérine, bien que sexe-spécifiques, ne semblent en revanche pas varier sensiblement suivant le gradient urbain-rural. Ce travail confirme la nécessité d’évaluer l’influence des inégalités sociales et environnementales sur le développement intra-utérin et de considérer l’importance et le rôle du contexte de vie, notamment urbain-rural, dans la formation de ces inégalités. / Pregnancy is a sensitive and critical period for the development of the child and the health of adults-to-be. The biological and physiological adaptation of the body dealing physical and psychosocial stressors during this period may exert its effects in adulthood (and possibly over several generations). This delayed toxicity presupposes intrinsically the need to study the effects of exposure to environmental risk factors during fetal life using a holistic approach involving risk factors at both the micro (individual characteristics) and the macro level (physical and psycho-social context). Given the heterogeneity of the Breton territory in which this work was conducted, we explored whether the impact of social inequalities and the physical environment (air pollution) on birth outcomes (fetal growth and the risk of prematurity) could be modified according to an urban or rural place of residence. This work was based on data collected as part of the Breton mother-child cohort PELAGIE, which had included 3421 pregnant women between 2002- 2006. The anthropometric parameters and gestational age at birth were measured by medical personnel at delivery. We defined urban and rural areas according to the definition of “urban units” from the National Census Bureau (INSEE). The annual concentrations of air pollution (nitrogen dioxide (NO2)) were estimated using a land-use regression modeled at a 100 m scale and developed as part of an European project. Finally, neighbourhood deprivation was estimated using a composite index developed at census blocks level and whose use was legitimated over both urban and rural areas. Neighbourhood deprivation was associated with an increased risk of infants with fetal growth restriction, only for women living in rural areas. We also observed an increased risk of preterm birth associated with NO2 concentrations > 16.4 μg.m-3, only among women residing in urban areas. The associations between air pollution and fetal growth, although sex-specific, did not seem on the other hand, to vary significantly according to the urban-rural spectrum. This work confirms the need to explore the influence of both social and environmental inequalities on intrauterine development, and to assess the role of place-based factors, such as the urban-rural context, in shaping these inequalities.

Particulate matter in the ambient air of down-town New Orleans, LA, is not currently recorded by any government, state, or private organization. This research quantified particulate matter (PM) and its metal concentration in ambient air of the New Orleans Historic District. Both, PM10 (PM less than 10 micron in size) and PM2.5 (PM less than 2.5 micron in size) were quantified by gravimetric analysis using an Andersen Dichotomous Sampler (Series 240). Posterior to gravimetric analysis, the filters were analyzed with a fluorescent test method using an Innov-X Portable XRF Analyzer (Model A-6500). This study demonstrated that the ambient air of the New Orleans Historic District is in compliance with the National Ambient Ai Quality Standards regarding contamination of particulate matter and Lead.