This dissertation is devoted to the attractive and rapidly developing field of
heterogeneous catalysts with isolated metal sites. The following research
questions served as the source of inspiration for it: • How to design a catalyst with isolated metal sites? • How to synthesize and develop a catalyst with isolated metal sites? • How to characterize a catalyst with isolated metal sites?
In the first part of this dissertation (Chapters 2-3) the route for design,
synthesis, characterization and further modification of heterogeneous
catalysts with isolated sites is described, using the development of a
catalyst for direct conversion of methane to methanol as an example. The
second part (Chapters 4-5) investigates the applicability of X-ray based
analysis techniques (primarily X-ray photoelectron spectroscopy (XPS) and
X-ray absorption spectroscopy (XAS)) for the characterization of such
catalysts ... Read more

In this thesis we presented comprehensive studies on methane activation by binuclear Fe-oxo sites located in porous MOF and zeolite frameworks. Many of such studies have been previously performed, however the main focus was usually on the C-H bond activation of methane. Here we focused on the whole reaction mechanism including the activation of the Fe site and the overoxidation of methanol, as well as the effects of the porous framework. ... Read more

Membrane separation is an energy efficient technology with a small physical footprint in which the membrane is the core of process. Membranes need to be further developed to be specifically applied in the field of gas separation. The most challenging target in designing membranes is to improve the permeation and selectivity, simultaneously. This goal cannot be achieved without acquiring the knowledge of material science to tune the membrane material properties. This PhD thesis focusses on designing mixed matrix membranes (MMMs) by using a new class of crystalline materials known as metal organic frameworks (MOFs) as filler. In combination with polymers as continuous phase it was expected to improve both the processability and separation performance of this composite material in comparison with the polymer only. This work has been performed in the framework of the FP7-EU project M4CO2 ('MOF-based Mixed Matrix Membranes for energy efficient CO2 capture', grant agreement n° 608490). Therefore the focus in this thesis was on, but not limited to, membranes for the separation of CO2 from N2, as a model for stack gases in coal combustion ('post-combustion separation'). To this aim, the overall concept of this thesis is divided into three parts in which the most relevant aspects of design in mixed matrix membranes are carefully studied. Part I (Chapter 2) elucidated the influence of MOF pore structure and topology on the MMMs separation performance. In part II (Chapter 3 and 4) the effect of MOF morphology and polymer free volume is studied. Finally, part III (Chapter 5) reports a study on free-standing and thin supported MOF nanosheet based membranes by using industrially viable methods. The summary of each Chapter in this thesis is presented as follows... ... Read more

This thesis, Gas Adsorptive Separation through Microporous Materials, presents the research done on gas separation processes in the Catalysis Engineering team. This thesis intends to collect the knowledge and results of five years’ experimental research dealing with gas mixtures and microporous materials, but also with tubing, and setup maintenance and designing. This thesis contains a first introduction chapter, four research chapters (based on journal publications) and this last summarizing chapter with an outlook about the field of adsorption regarding the thesis' results. ... Read more