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Sökning: WFRF:(Vincent D) > Doktorsavhandling

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1.
  • Persson, Ingemar, 1985- (författare)
  • Surface characterization of 2D transition metal carbides (MXenes)
  • 2019
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Research on two-dimensional (2D) materials is a rapidly growing field owing to the wide range of new interesting properties found in 2D structures that are vastly different from their three-dimensional (3D) analogues. In addition, 2D materials embodies a significant surface area that facilitates a high degree of surface reactions per unit volume or mass, that is imperative in many applications such as catalysis, energy storage, energy conversion, filtration, and single molecule sensing. MXenes constitute a family of 2D materials consisting of transition metal carbides and/or nitrides, which are typically formed after selective etching of their 3D parent MAX phases. The latter, are a family of nanolaminated compounds that typically follow the formula Mn+1AXn (n=1-3), where M is a transition metal, A is a group 13 or 14 element, and X is C and or N. Selective etching by aqueous F- containing acids removes the A layer leaving 2D Mn+1Xn slabs instantly terminated by a mix of O-, OH- and F-groups. The first and most investigated MXene is Ti3C2TX, where TX stands for surface termination, which has shown record properties in a range of applications (eg. electrode in Li-batteries, supercapacitors, sieving membrane, electromagnetic interference shielding, and carbon capture). Adding to that, over 30 different MXenes have been discovered since 2011, exhibiting alternative or superior properties. Most importantly, elegant routes for property design in the MXene family has been demonstrated, by means of either varying the chemistry in the Mn+1Xn compound, by alloying two M elements, or by changing the structure of the MXene by introducing vacancies.The present work has a led to an additional route for post synthesis property tuning in MXenes by manipulation of surface termination elements. This enables a unique toolbox for property tuning which is not available to other 2D materials and is highly beneficial for applications that is dependent on surface reactions. Furthermore, chemical and structural characterization of terminations on single sheets is essential to rule out the influence of intercalants or contamination that is typically present in multilayer MXene samples or thin films. For that purpose, a method for preparing isolated contamination free single sheets of MXene samples for transmission electron microscopy (TEM) characterization was established. In order to determine vacancy and termination sites, atomically resolved scanning (S)TEM imaging and image simulations was carried out. Two main processes were employed to substitute the termination elements.1) An initial thermal treatment in vacuum facilitates F desorption and it was shown that O-terminations rearranges on the evacuated sites. H2 gas exposure in a controlled environment demonstrated a removal of the remaining O-terminations. As a result, termination-free MXene is possible to realize under vacuum conditions.2) CO2 was introduced as a first non-inherent termination on MXene by in situ CO2 gas exposure at low temperatures. That was a first demonstration of Ti3C2TX as promising material for carbon capture. Additionally, O-saturated surfaces were demonstrated after introduction of O2 gas on the F-depleted Ti3C2TX MXene, which is highly relevant for hydrogen evolution reactions where fully O-terminated Ti3C2TX are predicted to improve efficiency.A Lewis acid melt synthesis method was used to realize the first MXene exclusively terminated with Cl. Moreover, this was the first report of a MXene directly synthesised with terminations other than O, OH, and F.Furthermore, we have expanded the space of property tuning by introduction of chemical ordering, by selective etching of Y in an alloyed (Mo2/3Y1/3)2CTX MXene. This either produced chemical ordering with one M (Mo) element and vacancies, or ordering between two M (Mo and Y) elements. This was further reported to significantly increase volumetric capacitance because of the increased number of active sites around vacancies, leading to an increasing charge density. As a final note, the stability of Nb2CTX MXene under ambient conditions was investigated. It was found that the surface Nb adatoms, present after etching, got oxidized over time which resulted in local clustering and effectively degraded the MXene.This work has demonstrated reproducible surface characterization methods for determining termination elements and sites in 2D MXenes, that is ultimately governing MXene properties. Most importantly, we report on a new approach for MXene property tuning as well as contributing to several existing property tuning approaches. 
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2.
  • Wilhelms, Susanne, 1985- (författare)
  • The epidemiology of severe sepsis in Sweden : Methodological aspects on the use of ICD coding in national registries
  • 2018
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Severe sepsis is characterized by acute organ dysfunction caused by an infection. Despite advanced treatment with antibiotics and organ support the mortality remains high. The epidemiological research on severe sepsis has expanded over the years but has led to conflicting results. In this thesis, we present evidence that some of these conflicting results may be explained by inappropriate methods used in epidemiological studies on severe sepsis. The definition of severe sepsis relies on consensus criteria including a number of clinical signs, parameters and laboratory findings. To facilitate large nation-wide studies on the incidence of severe sepsis in already existing administrative datasets, several investigators have attempted to mirror the clinical criteria by using combinations of the International Classification of Diseases (ICD) codes for infection and organ dysfunction. In paper I of this thesis, however, we found that three different ICD code abstraction strategies applied on the same dataset (the Swedish National Patient Register) generated three almost separate cohorts of patients. Furthermore, in paper II, where we followed intensive care unit (ICU)-treated patients with severe sepsis according to clinical consensus criteria to discharge, we observed that most patients did not meet any ICD code abstraction strategies for severe sepsis when reviewing their ICD codes registered at discharge from the hospital. In conclusion, the ICD code abstraction strategies previously used in the epidemiological research on sepsis seem to be inaccurate in the Swedish setting.  Sepsis may also result in poor long-term outcomes, and contribute to an increased risk of late mortality. However, the actual causes of late mortality in sepsis remain unclear. In paper III, we investigated causes of death over 1 year after treatment of sepsis in the ICU. In this study, a matched control group consisting of ICU-treated patients without sepsis was included. The most common causes of late mortality in both the sepsis group and the control group were heart diseases and cancer. The sepsis group, however, had a significantly increased incidence of infectious-related deaths compared with the control group, even over 1 year after the initial ICU event.   
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