Heterogeneous catalysis is essential to many industrial applications. These catalysts are often comprised of supported nanoparticles, which contain various different surface sites. For some... Show moreHeterogeneous catalysis is essential to many industrial applications. These catalysts are often comprised of supported nanoparticles, which contain various different surface sites. For some reactions, the presence of specific surface sights dominates the overall reactivity. Fundamental insight into the influence of different surface sites on the surface reaction dynamics may lead to better catalyst design in the future. In this thesis, we combine ultra-high vacuum techniques and (curved) single crystal surfaces to study surface structure effects relevant to heterogeneous catalysis. We study how step edges on a platinum surface affect (elementary) reactions that occur in oxygen reduction: hydrogen dissociation, hydrogen recombination, and oxygen reduction. Show less
Dijkman, T.F. van; Siegler, M.A.; Bouwman, E. 2016
This thesis uses the surface science approach to address questions regarding the interaction of oxygen with platinum and its subsequent reaction with carbon monoxide. A Pt(111) single crystal... Show moreThis thesis uses the surface science approach to address questions regarding the interaction of oxygen with platinum and its subsequent reaction with carbon monoxide. A Pt(111) single crystal surface is used as a model for the catalyst. Chapter 1 provides an overview of the literature on the subject. The description of employed experimental techniques and their backgrounds are presented in Chapter 2. Chapter 3 discusses the adsorption of oxygen on Pt(111) at various temperatures and its role in the oxidation of carbon monoxide. Chapter 4 gives an atomic scale insight into the reaction between adsorbed oxygen and carbon monoxide for different ratios of oxygen and carbon monoxide pressures. In Chapter 5, the reaction between CO and oxygen on Pt(111) was used to register noise in tunneling current due to diffusion and recombination of molecules on the catalytically active surface, to draw conclusions on the most likely rate-limiting step in the process Show less
The primary focus of this thesis is the formation of low-mass protostars, specifically the earliest deeply embedded phase, when material from the collapsing envelope is still accreted onto the... Show moreThe primary focus of this thesis is the formation of low-mass protostars, specifically the earliest deeply embedded phase, when material from the collapsing envelope is still accreted onto the growing young star. Rotational transitions of CO and O2 data are obtained by the Herschel Space Observatory key projects, WISH and HOP, together with ground-based observations from APEX and the JCMT. We have found that CO and its isotopologs have different line profiles tracing different materials in the protostellar regions. Our new high-J rotational transitons of CO is key to characterize the warmer parts of the protostellar envelope and quantify feedback of the protostars on their surroundings in terms of shocks, ultraviolet (UV) heating, photodissociation, and outflow dispersal. Radiative transfer modeling was performed to determine the CO abundance structure in the envelope, showing evidence for significant freeze-out in the coldest regions in the parts of the envelope where the temperature exceeds 25 K. A tentative detection of O2 is reported toward the source position of a protostar, which originates from the surrounding cloud. These kind of detailed studies of the physical and chemical structure of low-mass protostars are important for a complete understanding of the evolution of young stellar objects (YSOs). Show less
The study of gas-surface interaction dynamics is important both for the fundamental knowledge it provides and also to aid the development of applications involving processes such as sputtering,... Show moreThe study of gas-surface interaction dynamics is important both for the fundamental knowledge it provides and also to aid the development of applications involving processes such as sputtering, plasma etching and heterogeneous catalysis. Elementary steps in the interactions, such as chemical reactions, adsorption and scattering are prototypical of more complex processes and better understanding of them deepens our knowledge of such processes. In addition, experimental measurements of specific interactions can be used to validate advanced computer models. Hence the experiments in this thesis have been carried out under well-defined condition, namely in ultrahigh vacuum and using high-purity single-crystal samples. The thesis is primarily focussed on understanding the interaction of hyperthermal Ar and N (~4-6 eV) with Ru(0001) and Ag(111) via scattering studies. Ar is very inert and its interaction with surfaces is primarily repulsive in nature, while N atoms probe the surface chemisorption well. From the study of Ar scattering dynamics, surface properties have been probed. From N scattering studies, chemisorption dynamics have been investigated. It is found that the electronic state of the incident particle may play an important role in the gas-surface interaction. Separately, the influence of pre-adsorbed CO on Ru(0001) on D2 dissociation have been unravelled. Show less
